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635 results on '"Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086))"'

1. Co–Ru Nanoalloy Catalysts for the Acceptorless Dehydrogenation of Alcohols

Author: Brandon Azeredo, Tayssir Ben Ghzaiel, Ning Huang, Kamila Kaźmierczak, Wenjie Shen, Guillaume Wang, Delphine Schaming, Patricia Beaunier, Philippe Decorse, Noémie Perret, Jennifer Peron, Marion Giraud, Carine Michel, Lorette Sicard, Jean-Yves Piquemal, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Unité de Recherche de Chimie Minérale Appliquée, Université de Tunis El Manar (UTM), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Matériaux et Phénomènes Quantiques (MPQ (UMR_7162)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Laboratoire de Réactivité de Surface (LRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), IRCELYON-C'Durable (CDURABLE), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL)
Subjects: General Materials Science, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract: International audience
Published: 2022
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2. Thermally Switchable Nanogate Based on Polymer Phase Transition

Author: Pauline J. Kolbeck, Dihia Benaoudia, Léa Chazot-Franguiadakis, Gwendoline Delecourt, Jérôme Mathé, Sha Li, Romeo Bonnet, Pascal Martin, Jan Lipfert, Anna Salvetti, Mordjane Boukhet, Véronique Bennevault, Jean-Christophe Lacroix, Philippe Guégan, Fabien Montel, Laboratoire de Physique de l'ENS Lyon (Phys-ENS), École normale supérieure de Lyon (ENS de Lyon)-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Analyse, Modélisation et Matériaux pour la Biologie et l'Environnement (LAMBE - UMR 8587), Université d'Évry-Val-d'Essonne (UEVE)-Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-CY Cergy Paris Université (CY), Utrecht University [Utrecht], Centre International de Recherche en Infectiologie (CIRI), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Université Jean Monnet - Saint-Étienne (UJM)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Technische Universität Dresden = Dresden University of Technology (TU Dresden), and CNRS 80 Prime NanoViro
Subjects: biomolecule filtration, [CHIM.POLY]Chemical Sciences/Polymers, [PHYS.PHYS.PHYS-BIO-PH]Physics [physics]/Physics [physics]/Biological Physics [physics.bio-ph], Mechanical Engineering, thermoresponsive polymer, coil−globule transition, General Materials Science, Bioengineering, General Chemistry, nanopore, zero-mode waveguide, Condensed Matter Physics
Abstract: International audience; Mimicking and extending the gating properties of biological pores is of paramount interest for the fabrication of membranes that could be used in filtration or drug processing. Here, we build a selective and switchable nanopore for macromolecular cargo transport. Our approach exploits polymer graftings within artificial nanopores to control the translocation of biomolecules. To measure transport at the scale of individual biomolecules, we use fluorescence microscopy with a zero-mode waveguide set up. We show that grafting polymers that exhibit a lower critical solution temperature creates a toggle switch between an open and closed state of the nanopore depending on the temperature. We demonstrate tight control over the transport of DNA and viral capsids with a sharp transition (∼1 °C) and present a simple physical model that predicts key features of this transition. Our approach provides the potential for controllable and responsive nanopores in a range of applications.
Published: 2023
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3. Tuning the competition between photoisomerization and photothermy in biomimetic cyclocurcumin analogues

Author: Pecourneau, Jérémy, Losantos, Raúl, Gansmuller, Axel, Parant, Stéphane, Bernhard, Yann, Mourer, Maxime, Monari, Antonio, Pasc, Andreea, 0000-0002-9792-9144, Laboratoire Lorrain de Chimie Moléculaire (L2CM), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Universidad de La Rioja (UR), Cristallographie, Résonance Magnétique et Modélisations (CRM2), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), PhotoNS, and European Project: Synergie LO0024898,FEDER,FIRELIGHT(2018)
Subjects: Cyclocurcumine, General Chemical Engineering, General Physics and Astronomy, [CHIM]Chemical Sciences, Photoswitch, General Chemistry, Photothermal conversion, Fluorescence, Pyrone
Abstract: International audience; We report the synthesis and photophysical characterization of biomimetic D-A-D’ cyclocurcumin derivatives, which can potentially be used in light activated chemotherapy. Particularly we highlight that both the donor (D) and acceptor (A) groups significantly influence the photophysical response of the chromophore inducing strong bathochromic shift with D/A strength increase and notable fluorescence quantum yield enhancement with donor strength increase. More important, the nature of the acceptor group (oxo or malonitrile) dramatically modifies the outcome in non-radiative deactivation channels. Indeed, while compounds functionalized with an oxo-moiety undergo ethylenic E→Z photoisomerization, the one bearing a malonitrile group leads exclusively to other non-adiabatic internal conversion channels which much favor photothermal conversion as no isomerization of the ethylenic double bond was observed. The tuning of the photophysical properties and the alteration of isomerization vs. photothermal conversion is rationalized through the analysis of the potential energy surfaces along the most relevant degrees of freedom and shows a competitive pathway over malonitrile rotation. Our results offer novel perspective in oxygen-independent light activated chemotherapy and in the control of photochemical processes in biomimetic chromophores.
Published: 2023
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4. Phosphonium Ylides vs Iminophosphoranes: The Role of the Coordinating Ylidic Atom in cis -[Phosphine-Ylide Rh(CO) 2 ] Complexes

Author: Ingrid Popovici, Cécile Barthes, Thibault Tannoux, Carine Duhayon, Nicolas Casaretto, Antonio Monari, Audrey Auffrant, Yves Canac, Laboratoire de chimie moléculaire (LCM), École polytechnique (X)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de chimie de coordination (LCC), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Centre National de la Recherche Scientifique (CNRS), Ecole polytechnique, ANR-21-CE07-0026,LYMACATO,Ligands ylure et Métaux abondants pour la Catalyse et l'Optique(2021), ANR-10-LABX-0096,SEAM,Science and Engineering for Advanced Materials and devices(2010), ANR-18-IDEX-0001,Université de Paris,Université de Paris(2018), and ANR-11-IDEX-0002,UNITI,Université Fédérale de Toulouse(2011)
Subjects: Infrared (IR) CO stretching frequency, Iminophosphorane, Phosphonium ylide, Electron-donation, Rhodium complex, Ligands, Substituents, Inorganic Chemistry, Metals, Cations, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Chelating ligand, Physical and Theoretical Chemistry, Diffraction
Abstract: International audience; The coordinating properties of two families of ylides, namely, phosphonium ylides and iminophosphoranes, differently substituted at the ylidic center (CH2– vs NiPr–), have been investigated in structurally related cationic phosphine-ylide Rh(CO)2 complexes obtained from readily available phosphine-phosphonium salt precursors derived from an ortho-phenylene bridge. However, while the Rh(CO)2 complex bearing the P+–CH2– donor moiety proved to be stable, the P═NiPr donor end appeared to induce lability to one of the CO groups. All of the RhI carbonyl complexes in both ylide series were fully characterized, including through X-ray diffraction analysis. Based on the experimental and calculated infrared (IR) CO stretching frequencies in Rh(CO)2 complexes, we evidenced that the phosphonium ylide ligand is a stronger donor than the iminophosphorane ligand. However, we also found that the difference in the intrinsic electronic properties can be largely compensated by the introduction of an iPr substituent on the N atom of the iminophosphorane, hence pointing to the noninnocent role of the peripheral substituent and opening novel possibilities to tune the properties of metal complexes containing ylide ligands.
Published: 2023
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5. UV-Visible photo-reactivity of permanently polarized inorganic nanotubes coupled to gold nanoparticles

Author: Sabyasachi Patra, Fabienne Testard, Frédéric Gobeaux, Lorette Sicard, Delphine Shaming, Sophie Le Caër, Antoine Thill, Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Radiochemistry division, Bhabha Atomic Research Centre, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: plasmon, imogolite, nanotube, [CHIM]Chemical Sciences, General Materials Science, photocatalysis, gold nanoparticle
Abstract: International audience; Hybrid aluminosilicate nanotubes (Imo-CH3) have the ability to trap small organic molecules inside their hydrophobic internal cavity while being dispersed in water owing to their hydrophilic external surface. They also display a curvature-induced polarization of their wall, which favors reduction outside the nanotubes and oxidation inside. Here, we coupled bare plasmonic gold nanoparticles (GNPs) with Imo-CH3 and analyzed for the first time the redox reactivity of these hybrid nano-reactors upon UV illumination. We show that the coupling between GNPs and Imo-CH3 significantly enhances the nanotube photocatalytic activity, with a large part of water reduction occurring directly on the gold surface. The coupling mechanism strongly influences the initial H2 production rate, which can go from ×10 to more than ×90 as compared to bare Imo-CH3 depending on the synthesis route of the GNPs. The present results show that this hybrid photocatalytic nano-reactor benefits from a synergy of polarization and confinement effects that facilitate efficient H2 production.
Published: 2023
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6. Spectroscopy of individual Brownian nanoparticles in real-time using holographic localization

Author: Minh-Chau Nguyen, Pascal Berto, Fabrice Valentino, Frederic Kanoufi, Gilles Tessier, Kanoufi, Frederic, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Institut de la Vision, Institut National de la Santé et de la Recherche Médicale (INSERM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Neurophotonique (UMR 8250), and Université Paris Descartes - Paris 5 (UPD5)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS.PHYS.PHYS-OPTICS] Physics [physics]/Physics [physics]/Optics [physics.optics], [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], [PHYS.PHYS.PHYS-INS-DET] Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], [PHYS.PHYS.PHYS-INS-DET]Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], Atomic and Molecular Physics, and Optics, [PHYS.PHYS.PHYS-CHEM-PH] Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph]
Abstract: International audience; Individual nanoparticle spectroscopic characterization is fundamental, but challenging in liquids. While confocal selectivity is necessary to isolate a particle in a crowd, Brownian motion constantly offsets the particle from the light collection volume. Here, we present a system able to acquire holograms and reconstruct them to precisely determine the 3D position of a particle in real time. These coordinates drive an adaptive system comprising two galvanometric mirrors (x,y, transverse directions) and a tunable lens (z, longitudinal) which redirect light scattered from the corresponding region of space towards the confocal entrance of a spectrometer, thus allowing long spectral investigations on individual, freelymoving particles. A study of the movements and spectra of individual 100 nm Au nanoparticles undergoing two types of aggregations illustrates the possibilities of the method.
Published: 2022
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7. Theobroma cacao improves bone growth by modulating defective ciliogenesis in a mouse model of achondroplasia

Author: Ludovic Martin, Nabil Kaci, Catherine Benoist-Lasselin, Marine Mondoloni, Suzanne Decaudaveine, Valentin Estibals, Maxence Cornille, Léa Loisay, Justine Flipo, Benoît Demuynck, Maria de la Luz Cádiz-Gurrea, Florent Barbault, Salvador Fernández-Arroyo, Laurent Schibler, Antonio Segura-Carretero, Emilie Dambroise, Laurence Legeai-Mallet, Molecular and Physiopathological bases of osteochondrodysplasia - Bases moléculaires et physiopathologiques des ostéochondrodysplasies (Equipe Inserm U1163), Imagine - Institut des maladies génétiques (IHU) (Imagine - U1163), Institut National de la Santé et de la Recherche Médicale (INSERM)-Université Paris Cité (UPCité)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université Paris Cité (UPCité), Inovarion, Universidad de Granada = University of Granada (UGR), Centro de Investigação do Desporto e da Atividade Física (CIDAF), Universidade de Coimbra [Coimbra], Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), University Rovirai Virgili de Tarragona (URV), Maison Nationale des Eleveurs (MNE), and Université Paris Cité, Equipe HAL
Subjects: musculoskeletal diseases, 0303 health sciences, congenital, hereditary, and neonatal diseases and abnormalities, Histology, QH301-705.5, Physiology, Endocrinology, Diabetes and Metabolism, [SDV]Life Sciences [q-bio], Diseases, Article, 3. Good health, [SDV] Life Sciences [q-bio], 03 medical and health sciences, 0302 clinical medicine, 030220 oncology & carcinogenesis, QP1-981, Biology (General), Bone, 030304 developmental biology
Abstract: We thank the Imagine Institute's imaging facility and the SFR's histology facility for their help with this work. This program received a state subsidy managed by the National Research Agency under the "Investments for the Future" Program bearing the reference ANR-10-IAHU-01. Some of the work presented here was funded by the European Community's Seventh Framework Program under grant agreement 602300 (the SYBIL program (https://www.sybil-fp7.eu/) is funded by the MRC (MC_UU_000007/9))., A gain-of-function mutation in the fibroblast growth factor receptor 3 gene (FGFR3) results in achondroplasia (ACH), the most frequent form of dwarfism. Constitutive activation of FGFR3 impairs bone formation and elongation and many signal transduction pathways. Identification of new and relevant compounds targeting the FGFR3 signaling pathway is of broad importance for the treatment of ACH, and natural plant compounds are prime drug candidate sources. Here, we found that the phenolic compound (-)-epicatechin, isolated from Theobroma cacao, effectively inhibited FGFR3’s downstream signaling pathways. Transcriptomic analysis in an Fgfr3 mouse model showed that ciliary mRNA expression was modified and influenced significantly by the Indian hedgehog and PKA pathways. (-)-Epicatechin is able to rescue mRNA expression impairments that control both the structural organization of the primary cilium and ciliogenesis-related genes. In femurs isolated from a mouse model (Fgfr3Y367C/+) of ACH, we showed that (-)-epicatechin eliminated bone growth impairment during 6 days of ex vivo culture. In vivo, we confirmed that daily subcutaneous injections of (-)-epicatechin to Fgfr3Y367C/+ mice increased bone elongation and rescued the primary cilium defects observed in chondrocytes. This modification to the primary cilia promoted the typical columnar arrangement of flat proliferative chondrocytes and thus enhanced bone elongation. The results of the present proof-of-principle study support (-)-epicatechin as a potential drug for the treatment of ACH., French National Research Agency (ANR) ANR-10-IAHU-01, European Community - MRC 602300 MC_UU_000007/9
Published: 2022
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8. Electrochemistry and Optical Microscopy

Author: Frederic Kanoufi, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), and Kanoufi, Frederic
Subjects: [PHYS.PHYS.PHYS-OPTICS] Physics [physics]/Physics [physics]/Optics [physics.optics], [CHIM.ANAL] Chemical Sciences/Analytical chemistry, Materials science, Microscope, FOS: Physical sciences, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, law.invention, Micrometre, symbols.namesake, electrochemical conversion], Optical microscope, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, law, Surface plasmon resonance, Raman, Condensed Matter - Materials Science, [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], refractive index, Scattering, scattering, Resolution (electron density), Materials Science (cond-mat.mtrl-sci), imaging, electrode, 021001 nanoscience & nanotechnology, [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Optical microscopies, 3. Good health, 0104 chemical sciences, Condensed Matter - Other Condensed Matter, single entity, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], symbols, fluorescence, 0210 nano-technology, Raman spectroscopy, Refractive index, surface plasmon resonance, Physics - Optics, Optics (physics.optics), Other Condensed Matter (cond-mat.other)
Abstract: Electrochemistry exploits local current heterogeneities at various scales ranging from the micrometer to the nanometer. The last decade has witnessed unprecedented progress in the development of a wide range of electroanalytical techniques allowing to reveal and quantify such heterogeneity through multiscale and multifonctionnal operando probing of electrochemical processes. However most of these advanced electrochemical imaging techniques, employing scanning probes, suffer from either low imaging throughput or limited imaging size. In parallel, optical microscopies, which can image a wide field of view in a single snapshot, have made considerable progress in terms of sensitivity, resolution and implementation of detection modes. Optical microscopies are then mature enough to propose, with basic bench equipment, to probe in a non destructive way a wide range of optical (and therefore structural) properties of a material in situ, in real time: under operating conditions. They offer promising alternative strategies for quantitative high-resolution imaging of electrochemistry. The first sections recall the optical properties of materials and how they can be probed optically. They discuss fluorescence, Raman, surface plasmon resonance, scattering or refractive index. Then the different optical microscopes used to image electrochemical processes are examined along with some strategies to extract quantitative electrochemical information from optical images. Finally the last section reviews some examples of in situ imaging, at micro- to nanometer resolution, and quantification of electrochemical processes ranging from solution diffusion to the conversion of molecular interfaces or solids., Comment: 66 pages, 23 figures. To be published in Encyclopedia of Electrochemistry
Published: 2021
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9. Estimation of activity coefficients for aqueous organic redox flow batteries: Theoretical basis and equations

Author: Gaël Mourouga, Déborah Chery, Emmanuel Baudrin, Hyacinthe Randriamahazaka, Thomas J. Schmidt, Juergen O. Schumacher, ZHAW School of Engineering, Zürich University of Applied Sciences (ZHAW), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire réactivité et chimie des solides - UMR CNRS 7314 (LRCS), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Picardie - FR 3085 (ICP), Réseau sur le stockage électrochimique de l'énergie (RS2E), Aix Marseille Université (AMU)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Nantes Université (Nantes Univ)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: 621.3: Elektro-, Kommunikations-, Steuerungs- und Regelungstechnik, Chemistry, Computational chemistry, Multidisciplinary, Erneuerbare Batterie, Concentrated solution theory, Estimation of activity coefficients, Electrochemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, Redox flow battery, Virial matrix, Electrochemical energy storage
Abstract: The field of aqueous organic redox flow batteries (AORFBs) has been developing fast in recent years, and many chemistries are starting to emerge as serious contenders for grid-scale storage. The industrial development of these systems would greatly benefit from accurate physics-based models, allowing to optimize battery operation and design. Many authors in the field of flow battery modeling have brought evidence that the dilute solution hypothesis (the assumption that aqueous electrolytes behave ideally) does not hold for these systems and that calculating cell voltage or chemical potentials through concentrations rather than activities, while serviceable, may become insufficient when greater accuracy is required. This article aims to provide the theoretical basis for calculating activity coefficients of aqueous organic electrolytes used in AORFBs to provide tools to predict the concentrated behavior of aqueous electrolytes, thereby improving the accuracy of physics-based models for flow batteries., iScience, 25 (9), ISSN:2589-0042
Published: 2022
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10. Periodic nanoporous inorganic patterns directly made by self-ordering of cracks

Author: Mateusz Odziomek, Fanny Thorimbert, Cedric Boissiere, Glenna L. Drisko, Stephane Parola, Clement Sanchez, Marco Faustini, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de la Matière Condensée de Bordeaux (ICMCB), Université de Bordeaux (UB)-Institut Polytechnique de Bordeaux-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and The European Research Council (ERC) under European Union’s Horizon 2020 Programme (Grant Agreement no. 803220, TEMPORE). The College de France for financial support and the Foundation for Polish Science (FNP) for a START scholarship.
Subjects: patterning, Mechanics of Materials, Mechanical Engineering, porous films, inorganic, crack, photonics, General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; Solution-processed inorganic nanoporous films are key components for the vast spectrum of applications ranging from dew harvesting to solar cells. Shaping them into complex architectures required for advanced functionality, often need time-consuming or expensive fabrication. In this work, we show how crack formation is harnessed to pattern porous inorganic films in a single step and without using lithography. We developed aqueous ink formulations that, in the presence of polymeric latexes, enable evaporation-induced, defect-free periodic arrays of cracks with tunable dimensions over several centimeters. The ink formulation strategy was generalized to more than ten inorganic materials including simple and binary porous oxide and metallic films covering a whole spectrum of properties including insulator, photocatalytic, electrocatalytic, conductive or electrochromic materials. Notably, this approach enables three-dimensional self-assembly of cracks by stacking several layers of different compositions, yielding periodic assemblies of polygonal shapes and Janus-type patterns. The crack patterned periodic arrays of nanoporous TiO2 diffract light, and are used as temperature-responsive diffraction grating sensors. More broadly, this method represents a unique example of self-assembly process leading to long-range order (over several cm) in a robust and controlled way.
Published: 2022
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11. Electrochemical Active Surface Area Determination of Iridium‐Based Mixed Oxides by Mercury Underpotential Deposition

Author: Duran, Silvia, Elmaalouf, Marine, Odziomek, Mateusz, Piquemal, Jean‐Yves, Faustini, Marco, Giraud, Marion, Peron, Jennifer, Tard, Cédric, Piquemal, Jean-Yves, Piquemal, J.-Y, Laboratoire de chimie moléculaire (LCM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Oxygen evolution, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Underpotential deposition, Electrochemistry, 01 natural sciences, Catalysis, 0104 chemical sciences, Mercury (element), Chemical engineering, Physisorption, chemistry, Degradation (geology), Iridium, [CHIM.OTHE]Chemical Sciences/Other, 0210 nano-technology
Abstract: International audience; The electrochemical surface area (ECSA) is a critical property to describe, analyze and compare electrocatalysts. The determination of the mass activity of a given catalyst is associated with this parameter which can thus lead to materials benchmarking. Reliable and robust methods to measure ECSA are needed, and those have to accommodate different structures, morphologies and compositions. In this study, we investigate mercury underpotential deposition (HgUPD) as a way to estimate ECSA for ultraporous electrocatalysts based on iridium and iridium-molybdenum electrocatalysts for the oxygen evolution reaction. Results reveal a clear agreement between physisorption measurements and HgUPD with excellent reproducibility. The method shows also that pre- and post-catalysis surface area measurements are not affected by the catalytic process on short timescale, opening the possibility of electrocalyst stability and degradation monitoring.
Published: 2021
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12. Electrochemical and Plasmon‐induced Grafting of n‐Dopable π‐Conjugated Oligomers

Author: Denis Frath, Sarra Gam-Derouich, Jean-Christophe Lacroix, Mathieu Bastide, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: Materials science, 02 engineering and technology, Conjugated system, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, Grafting, Photochemistry, 01 natural sciences, Catalysis, 0104 chemical sciences, [CHIM]Chemical Sciences, Surface modification, Thin film, 0210 nano-technology, Plasmon
Abstract: International audience; Electrodes are functionalized by electrochemical reduction of the diazonium cation from 4-(2,3-diethylthieno[3,4-b]pyrazine-5-yl)aniline with ultrathin organic layers incorporating thienopyrazine units. This layer can be n-doped while being covalently grafted to the surface. Moreover, it can be deposited onto gold nanoparticles (NPs) by plasmon-induced diazonium reduction, thanks to the transfer of hot electrons from the excited plasmonic NPs to the diazonium salt. This confirms that localized surface plasmon resonance can induce nanolocalized electrochemical reactions.
Published: 2021
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13. Beyond Chemical Accuracy for Alkane Thermochemistry: The DHthermo Approach

Author: Bernardino Tirri, Éric Brémond, Carlo Adamo, Hanwei Li, Juan Carlos Sancho-García, Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Universidad de Alicante, Universidad de Alicante. Departamento de Química Física, and Química Cuántica
Subjects: Isodesmic reaction, Basis (linear algebra), 010405 organic chemistry, Chemistry, Chemical accuracy, Alkane thermochemistry, Organic Chemistry, 010402 general chemistry, DHthermo, 01 natural sciences, Stability (probability), London dispersion force, 0104 chemical sciences, Intramolecular force, Thermochemistry, [SDV.BBM]Life Sciences [q-bio]/Biochemistry, Molecular Biology, Density functional theory, Química Física, Statistical physics, Basis set
Abstract: The so-called protobranching phenomenon, that is the greater stability of branched alkanes with respect to their linear isomers, represents an interesting challenge for approaches based on density functional theory (DFT), since it requires a balanced description of several electronic effects, including (intramolecular) dispersion forces. Here, we investigate this problem using a protocol recently developed based on double-hybrid functionals and a small basis set, DH-SVPD, suited for noncovalent interactions. The energies of bond separation reactions (BSR), defined on the basis of an isodesmic principle, are taken as reference properties for the evaluation of 15 DFT approaches. The obtained results show that error lower than the so-called “chemical accuracy” (
Published: 2021
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14. Data on nitridation effect of AlTiTaZrHf(-N) high entropy films by X-ray photoelectron spectroscopy

Author: El Garah, Mohamed, Touaibia, Djallel Eddine, Achache, Sofiane, Michau, Alexandre, Sviridova, Elizaveta, Postnikov, Pavel, Chehimi, Mohamed, Schuster, Frederic, Sanchette, Frederic, Laboratoire des Systèmes Mécaniques et d'Ingénierie Simultanée (LASMIS), Université de Technologie de Troyes (UTT), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Tomsk Polytechnic University [Russie] (UPT), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: [SPI]Engineering Sciences [physics], ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2022
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15. Environmental Control of Single‐Molecule Junction Evolution and Conductance: A Case Study of Expanded Pyridinium Wiring

Author: Gábor Mészáros, Philippe P. Lainé, Jakub Šebera, Viliam Kolivoška, Štěpánka Nováková Lachmanová, Magdaléna Hromadová, Jindřich Gasior, Grégory Dupeyre, J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Division of Livestock Sciences, Universität für Bodenkultur Wien [Vienne, Autriche] (BOKU), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: expanded pyridiniums, Materials science, 02 engineering and technology, Substrate (electronics), 010402 general chemistry, 01 natural sciences, Catalysis, law.invention, chemistry.chemical_compound, law, Water environment, [CHIM]Chemical Sciences, Molecule, ComputingMilieux_MISCELLANEOUS, Research Articles, 010405 organic chemistry, Conductance, Molecular electronics, General Medicine, General Chemistry, 021001 nanoscience & nanotechnology, solvent gating, 0104 chemical sciences, chemistry, Chemical physics, single-molecule conductance, scanning tunneling microscopy, Pyridinium, Molecular Electronics, Scanning tunneling microscope, 0210 nano-technology, Break junction, Research Article
Abstract: Environmental control of single‐molecule junction evolution and conductance was demonstrated for expanded pyridinium molecules by scanning tunneling microscopy break junction method and interpreted by quantum transport calculations including solvent molecules explicitly. Fully extended and highly conducting molecular junctions prevail in water environment as opposed to short and less conducting junctions formed in non‐solvating mesitylene. A theoretical approach correctly models single‐molecule conductance values considering the experimental junction length. Most pronounced difference in the molecular junction formation and conductance was identified for a molecule with the highest stabilization energy on the gold substrate confirming the importance of molecule–electrode interactions. Presented concept of tuning conductance through molecule–electrode interactions in the solvent‐driven junctions can be used in the development of new molecular electronic devices., Single‐molecule junction conductance can be efficiently tuned by solvent environment. A series of expanded pyridinium molecular wires gave higher conductance with fully extended junction geometries in solvating water environment as opposed to mesitylene solvent. Environmental control efficiently operates the molecule–electrode interactions.
Published: 2021
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16. Versatile one-pot synthesis of gold nanoclusters and nanoparticles using 3,6-(dipyridin-2-yl)-(1,2,4,5)-tetrazine

Author: Vincent Guérineau, Alexa Courty, Stéphane Maisonneuve, Yahdi Bin Rus, Fabien Miomandre, Vincent Noël, Margarita Bosmi, Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Institut de Chimie des Substances Naturelles (ICSN), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), De la Molécule aux Nanos-objets : Réactivité, Interactions et Spectroscopies (MONARIS), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: chemistry.chemical_classification, Reaction mechanism, General Chemical Engineering, One-pot synthesis, Nanoparticle, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Photochemistry, 01 natural sciences, 0104 chemical sciences, Nanoclusters, Tetrazine, chemistry.chemical_compound, chemistry, X-ray photoelectron spectroscopy, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Thiol, [CHIM]Chemical Sciences, Absorption (chemistry), 0210 nano-technology
Abstract: A one-pot synthesis of gold nano-objects is described by simply mixing a gold salt (HAuCl4), dodecanethiol and 3,6-di-2-pyridyl-1,2,4,5-tetrazine. When a large excess of thiol is used, gold nanoclusters of 2 nm are obtained in a large amount and with a narrow size distribution. The reaction mechanism was investigated by absorption and emission spectroscopies and shows the in situ formation of dihydrotetrazine acting as the reductant of Au(III) to make Au(0). Au nanoclusters were isolated from the molecular precursors by HPLC. The nature of the ligands stabilizing Au nanoclusters was investigated by various techniques such as mass spectrometry, SEM-EDS, XPS and NMR. Thiol and tetrazine are shown to play both the role of ligand stabilizing the clusters. Finally, when a much smaller amount of thiol is used, a mixture of Au nanoclusters and Au nanoparticles of 10–15 nm, sometimes aggregated into clusters of 50 nm is obtained. The formation of larger nanoobjects is explained by the lower amount of thiol available to block the growth at the early stage as shown by UV-vis absorption monitoring.
Published: 2021
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17. Inorganic nanotubes with permanent wall polarization as dual photo-reactors for wastewater treatment with simultaneous fuel production

Author: Jean-Blaise Brubach, Lorette Sicard, Marie-Claire Pignié, Pierre Picot, Antoine Thill, Sabyasachi Patra, Delphine Schaming, Sophie Lecaer, Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), ligne AILES, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), DIM RESPORE 2019-20: Project GRANITE, CEA Bottom Up 2020-21 grant PHOTOTUBE, European Project: 844909, Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: energy conversion, Materials Science (miscellaneous), Kinetics, Polycyclic aromatic hydrocarbon, charge separation, 02 engineering and technology, Nanoreactor, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Redox, chemistry.chemical_compound, wastewater management, General Environmental Science, chemistry.chemical_classification, Anthracene, [CHIM.MATE]Chemical Sciences/Material chemistry, Mineralization (soil science), 021001 nanoscience & nanotechnology, 6. Clean water, 0104 chemical sciences, imogolite, chemistry, Chemical engineering, 13. Climate action, confinement, photo-catalysis, Photocatalysis, Degradation (geology), 0210 nano-technology
Abstract: International audience; Photocatalytic production of fuels, even in small quantities, from the mineralization of hazardous pollutants, is a promising and renewable way of recycling wastewater. In the present work, the potential of methyl functionalized inorganic aluminosilicate nanotubes (methyl imogolite/Imo-CH3) as photocatalytic nanoreactors for this application is demonstrated. Using the phototoxic polycyclic aromatic hydrocarbon dibenzo(a,h)anthracene (DBAN) as a model pollutant, we show that DBAN molecules can be efficiently trapped inside Imo-CH3 nanotubes from an aqueous medium to undergo subsequent oxidative photo-degradation under UV light. The kinetics of this photo-degradation were shown to depend strongly on both the initial DBAN concentration in the nanotubes and the presence/absence of dissolved dioxygen. The photo-degradation process followed a complex mechanistic pathway, consisting of combined photo-oxidation and photo-cycloaddition reactions, where detection of carbon dioxide (CO2) as a photo-oxidation product confirmed the mineralization of encapsulated DBAN. CO and CH4 molecules were also formed, however these could arise from the further photo-reduction of CO2 on the external surface of the nanotubes. Moreover, dihydrogen (H2) was produced upon UV illumination under anaerobic conditions due to water reduction reactions on the external surfaces of Imo-CH3 nanotubes. The possible mechanistic pathways of these processes are proposed, and the dual capability of Imo-CH3 nanotubes for simultaneous pollutant degradation and H2 production is then demonstrated – a rare feat for a single photocatalyst material.
Published: 2021
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18. Synthesis and Properties of Nanostructured Tungsten Oxide on Au(111)

Author: Jérôme Lagoute, Vincent Repain, Mahamadou Seydou, Sylvie Rousset, Yann Girard, Philippe Decorse, Cyril Chacon, Mariem Ben Youssef, Rishav Harsh, Philippe Lang, Amandine Bellec, Jean-Yves Piquemal, Laboratoire Matériaux et Phénomènes Quantiques (MPQ (UMR_7162)), Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), and Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Nanostructure, Materials science, Tungsten oxide, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, General Energy, Chemical engineering, 0103 physical sciences, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], Physical and Theoretical Chemistry, 010306 general physics, 0210 nano-technology
Abstract: International audience; WO 3 nanostructures have been synthesized on Au(111) through solution processing. Three types of structures have been obtained, reticulated polymeric structures, two dimensional WO 3 (111) and three-dimensional islands. Their electronic properties have been probed by scanning tunneling spectroscopy. The reticulated structure has a featureless spectrum. WO 3 (111) shows n-type semiconducting properties with resonances corresponding to surface states arising from W 5d states. Those oxyde nanostructures are efficiently decoupling the electronic states of molecular adsorbates from the metal substrate.
Published: 2020
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19. Enhanced Photochromism of Diarylethene Induced by Excitation of Localized Surface Plasmon Resonance on Regular Arrays of Gold Nanoparticles

Author: Leïla Boubekeur-Lecaque, Ryohei Yasukuni, Jean Aubard, Nordin Félidj, Stéphanie Lau-Truong, Nara Institute of Science and Technology, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: Materials science, Photoisomerization, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Photochemistry, 01 natural sciences, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Photochromism, symbols.namesake, chemistry.chemical_compound, Diarylethene, chemistry, symbols, Nanorod, Physical and Theoretical Chemistry, Surface plasmon resonance, 0210 nano-technology, Raman scattering, Visible spectrum, Localized surface plasmon
Abstract: International audience; Localized surface plasmon resonance (LSPR) excitation on the photochromic reaction of a diarylethene derivative (DE) was studied by surface enhanced Raman scattering (SERS). UV and visible light irradiations transform reversibly DE between open-form (OF) and closed-form (CF) isomers, respectively. A mixture of PMMA and DE (either OF or CF isomer) was spin-coated onto gold nanorods (GNRs) arrays, designed by electron beam lithography, with two localized surface plasmon resonances (LSPR) at distinct wavelengths, due to their anisotropy. The photochromic reaction rates from CF to OF isomers, under LSPR excitation, were monitored from SERS spectral changes under different polarizations, on the same GNR substrate to compare the effect of LSPR field strength. It appears that the photoisomerization rate was faster when LSPR was excited with the polarization parallel to the GNR long axis. The present results highlight a potential genuine mechanism, from near field LSPR excitation, involved in the photochromic enhancement of diarylethene photochromes.
Published: 2020
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20. Electrocatalytic O2 Activation by Fe Tetrakis(pentafluorophenyl)porphyrin in Acidic Organic Media. Evidence of High-Valent Fe Oxo Species

Author: Célia Achaibou, Marc Robert, Elodie Anxolabéhère-Mallart, Claire Fave, Frédéric Kanoufi, Nikolaos Kostopoulos, Jean-Marc Noël, Laboratoire d'Electrochimie Moléculaire (LEM (UMR_7591)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), and Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086))
Subjects: 010405 organic chemistry, Chemistry, reductive O2 activation, [CHIM.CATA]Chemical Sciences/Catalysis, molecular electrochemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, Electrochemistry, 01 natural sciences, Medicinal chemistry, Organic media, Porphyrin, 0104 chemical sciences, Catalysis, Inorganic Chemistry, chemistry.chemical_compound, Physical and Theoretical Chemistry, iron porphyrin, [CHIM.OTHE]Chemical Sciences/Other
Abstract: International audience; O2 activation under mild conditions remains a weighty challenge for chemists. Herein we report a study of electrochemical O2 reductive activation catalyzed by Fe III (F20 TPP)Cl, by means of cyclic voltammetry and UV−vis spectroelectrochemistry in acidic solutions of N,N-dimethylformamide. Two parallel catalytic pathways have been evidenced occurring at different overpotentials. At high overpotential a classical electron−proton (EPT) pathway where protonation of Fe peroxo ultimately leads to the formation of high-valent Fe oxo species dominates. At low overpotential a proton−electron (PET) pathway involving a hydrosuperoxo species has been identified.
Published: 2020
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21. New Insights into the Redox Properties of Pyridinium Appended 1,2-Dithienylcyclopentenes

Author: Lambert Sicard, Frederic Lafolet, Martial Boggio‐Pasqua, Christophe Bucher, Guy Royal, Saioa Cobo, Département de Chimie Moléculaire (DCM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Photochimie théorique et computationnelle (LCPQ) (PTC), Laboratoire de Chimie et Physique Quantiques Laboratoire (LCPQ), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Fédération de recherche « Matière et interactions » (FeRMI), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, photochemistry, Isomerism, electrochemistry, dithienylethene, density functional calculations, Cyclopentanes, Physical and Theoretical Chemistry, photochromism, Oxidation-Reduction, Atomic and Molecular Physics, and Optics, ComputingMilieux_MISCELLANEOUS
Abstract: International audience; Complex mechanism: We investigate optical and redox properties of a methyl pyridinium appended 1,2-dithienylethene photochromic derivative employing (spectro-) electrochemical measurements complemented by theoretical calculations. Based on our findings, we propose a complex multi-step photo/redox mechanism for the closed isomer.AbstractThe optical and redox properties of a methyl pyridinium appended 1,2-dithienylethene photochromic derivative have been thoroughly investigated. A complex multi-step photo/redox mechanism is proposed for the closed isomer on the ground of spectro-electrochemical and theoretical data. The generated compounds are not stable over the time because of chemical reactions associated to the redox processes and a new dithienylethene derivative incorporating a seven-membered ring has been isolated and characterized.
Published: 2022
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22. Nanotubes d'imogolite associés à des nanoparticules d'or. Impact du mode de préparation sur la réactivité sous éclairement UV et visible

Author: Patra, Sabyasachi, Testard, Fabienne, Le Caër, Sophie, Gobeaux, Frédéric, Sicard, Lorette, Thill, Antoine, Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Radiochemistry division, Bhabha Atomic Research Centre, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), GdR CNRS n°2002, and Palacin, Serge
Subjects: [CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2022

23. Asymmetric Effect on the Length Dependence of Oligo(Phenylene ethynylene)-Based Molecular Junctions

Author: Yinqi Fan, Sylvain Pitie, Chenguang Liu, Cezhou Zhao, Chun Zhao, Mahamadou Seydou, Yannick J. Dappe, Richard J. Nichols, Li Yang, University of Liverpool, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Shenzhen University [Shenzhen], Xi'an Jiaotong-Liverpool University [Suzhou], Service de physique de l'état condensé (SPEC - UMR3680), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics], General Energy, Single molecular electronics, [CHIM]Chemical Sciences, oligo (phenylene ethynylene)s, Physical and Theoretical Chemistry, graphene contacts, density functional theory, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials
Abstract: International audience; It is well known that the electrical conductance of molecular junctions in the tunneling regime varies exponentially with the length of the molecular backbone. This behavior is strongly influenced by anchoring groups, which connect the molecular backbone to the electrodes and locate the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) resonances with respect to the Fermi level. Nevertheless, most of the studies have been performed on symmetric junctions, namely, using the same electrodes and anchoring groups at both sides of the junctions. Only recently, there have been some reports detailing the influence of introducing asymmetry into single-molecule junctions, using different contacts or different anchoring groups at either end of the molecular bridge. These studies have revealed that such junction asymmetry strongly impacts electrical characteristics. In this study, Au and graphene electrodes were used to provide asymmetry to a single-molecule junction. The conductance and length dependence of amine and methyl sulfide-terminated oligo(phenylene ethynylene) have been determined experimentally and theoretically. The impact of introducing this asymmetry has been quantified by comparing the conductance and β values of oligo(phenylene ethynylene) (OPE)based molecules within Au/Au electrodes and Au/graphene junctions, respectively. Our results show that the introduction of a graphene electrode leads to lower conductance values and attenuation factors, similar to what has been previously observed in alkane chains. This is attributed to a shift of the electronic molecular levels toward the Fermi level, mainly driven by acetylene groups linking adjacent phenyl groups.
Published: 2022
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24. SERS tags derived from silver nanoparticles and aryl diazonium salts for cell Raman imaging

Author: Da Li, Philippe Nizard, Delphine Onidas, Aazdine Lamouri, Jean Pinson, Samia Mahouche-Chergui, Kelly Aubertin, Florence Gazeau, Yun Luo, Claire Mangeney, Université Paris Cité (UPCité), Laboratoire de Chimie et de Biochimie Pharmacologiques et Toxicologiques (LCBPT - UMR 8601), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie et des Matériaux Paris-Est (ICMPE), Institut de Chimie du CNRS (INC)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Est (UPE), Matière et Systèmes Complexes (MSC (UMR_7057)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), and Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)
Subjects: inorganic chemicals, Silver, Microscopy, Electron, Transmission, technology, industry, and agriculture, [CHIM]Chemical Sciences, Metal Nanoparticles, General Materials Science, Salts, macromolecular substances, Spectrum Analysis, Raman
Abstract: International audience; The surface functionalization of silver nanoparticles (NPs) by Raman reporters has stimulated a wide interest in recent years for the design of Surface-Enhanced Raman Spectroscopy (SERS) labels. However, silver NPs are prone to oxidation and aggregation, which strongly limits their applications. The design of stable SERS tags based on Ag NPs still represents a major challenge for Raman bioimaging. We address this issue herein by taking advantage of aryl diazonium salt chemistry to obtain stable Ag NPs functionalized by multifunctional polyaryl layers bearing different Raman reporters (-NO2,-CN,-CCH). The resulting SERS-encoded Ag NPs were characterized by UV-vis absorption, transmission electron microscopy (TEM) and SERS. The formation of multilayers at the surface of Ag NPs gives access to new spectrally distinguishable SERS codes thus broadening the library of available Raman tags. Proof-of-concept Raman imaging experiments were performed on cancer cells (HeLa) after NP uptake, highlighting the large potentials of diazonium salt chemistry to design Ag NPsbased SERS labels for Raman bioimaging.
Published: 2022
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25. Ruthenium icosahedra and ultrathin platelets: the role of surface chemistry on the nanoparticle structure

Author: Raj Kumar Ramamoorthy, Katerina Soulantica, Iker Del Rosal, Raul Arenal, Philippe Decorse, Jean-Yves Piquemal, Bruno Chaudret, Romuald Poteau, Guillaume Viau, Laboratoire de physique et chimie des nano-objets (LPCNO), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Fédération de recherche « Matière et interactions » (FeRMI), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Instituto de Nanociencia de Aragón [Saragoza, España] (INA), University of Zaragoza - Universidad de Zaragoza [Zaragoza], Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Agence Nationale de la Recherche (France), Universidad de Zaragoza, Ministerio de Economía y Competitividad (España), European Commission, and Calcul en Midi-Pyrénées
Subjects: General Chemical Engineering, Materials Chemistry, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: The control of the crystalline structure and shape (crystal habit) of nanoparticles (NPs) is the key to controlling their physical and chemical properties. Among the different metals, the crystallogenesis of ruthenium NPs has been less studied, and until recently, the Ru NP crystal structure and morphology have been considered as presenting less versatility than the face-centered cubic (fcc) metals of the platinum group. Here, we show that while the hydrogenation of [Ru(COD)(COT)] in solutions containing a long-chain amine (hexadecylamine, HDA) in large excess leads to isotropic NPs adopting the expected hexagonal close-packed (hcp) structure of bulk Ru, a long-chain carboxylic acid (lauric acid, LA) in large excess induces the formation of Ru nano-objects of two original structures: ultrathin platelets and icosahedra. The latter have never been produced so systematically by other methods. We show that carbon monoxide, produced in situ by the decarbonylation of lauric acid, plays a pivotal role in the stabilization of the Ru icosahedra. This result is supported by density functional theory (DFT) calculations, which show that above a critical surface coverage of CO, small Ru icosahedra are more stable than the Ru bipyramid polyhedra crystallizing in the hcp structure. Thus, in situ production of CO results in a competition between icosahedral and hcp seeds, which explains the mixture of icosahedra and ultrathin platelets. Another effect of the large excess of lauric acid is the stabilization of the ruthenium precursors in solution, limiting the nucleation extent and slowing down the NP growth. While the growth of the icosahedral seeds is limited because of the structural strains, the growth of the hcp seeds preferentially develops the (0001) facets, leading to ultrathin platelets and threefold stars., This work was funded by the French National Research Agency, ANR, in the framework of the TANOPOL project (ANR-15-CE07-0011-01). Teresa Hungria (Plateforme Castaing, Toulouse) is warmly thanked for HAADF-STEM images. The authors gratefully acknowledge the International Associated Laboratory (LIA)-M2OZART for financial support. High-resolution HAADF-STEM images were performed at the Laboratorio de Microscopias Avanzadas, Instituto de Nanociencia de Aragon, Universidad de Zaragoza, Spain. R.A. gratefully acknowledges the support from the Spanish Ministry of Economy and Competitiveness (MINECO) through project MAT2016-79776-P (AEF/FEDER. UE). I.D.R. and R.P. thank the HPC CALcul en Midi-Pyrénées (CALMIP, OLYMPE machine, grant P0611) for a very generous allocation of computer time on this project.
Published: 2022
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26. Lipophilic quinolone derivatives: Synthesis and in vitro antibacterial evaluation

Author: Sadowski, Elodie, Bercot, Beatrice, Chauffour, Aurélie, Gomez, Catherine, Varon, Emmanuelle, Mainardis, Mary, Sougakoff, Wladimir, Mayer, Claudine, Sachon, Emmanuelle, Anquetin, Guillaume, Aubry, Alexandra, Centre d'Immunologie et des Maladies Infectieuses (CIMI), Institut National de la Santé et de la Recherche Médicale (INSERM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), CHU Pitié-Salpêtrière [AP-HP], Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Sorbonne Université (SU), Laboratoire des biomolécules (LBM UMR 7203), Chimie Moléculaire de Paris Centre (FR 2769), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Département de Chimie - ENS Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Infection, Anti-microbiens, Modélisation, Evolution (IAME (UMR_S_1137 / U1137)), Institut National de la Santé et de la Recherche Médicale (INSERM)-Université Paris Cité (UPCité)-Université Sorbonne Paris Nord, Hopital Saint-Louis [AP-HP] (AP-HP), Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP), Laboratoire Génomique, bioinformatique et chimie moléculaire (GBCM), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), Centre Hospitalier Intercommunal de Créteil (CHIC), Laboratoire des sciences de l'ingénieur, de l'informatique et de l'imagerie (ICube), École Nationale du Génie de l'Eau et de l'Environnement de Strasbourg (ENGEES)-Université de Strasbourg (UNISTRA)-Institut National des Sciences Appliquées - Strasbourg (INSA Strasbourg), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut National de Recherche en Informatique et en Automatique (Inria)-Les Hôpitaux Universitaires de Strasbourg (HUS)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Microbiologie structurale - Structural Microbiology (Microb. Struc. (UMR_3528 / U-Pasteur_5)), Institut Pasteur [Paris] (IP)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Spectrométrie de masse de Sorbonne Université [IBPS] (MS3U), Institut de Biologie Paris Seine (IBPS), Institut National de la Santé et de la Recherche Médicale (INSERM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Université Paris Cité (UPCité), The work was supported by grants from the order of Malta Grants for Leprosy Research, QUIET Lutech MA077/SL00091 – ref UPMCX13042 from the SATT LUTECH and ANR DETONATOR., ANR-20-CE18-0030,DETONATOR,Décryptage du mode d'action de nouveaux antituberculeux prometteurs(2020), Centre d'Immunologie et de Maladies Infectieuses (CIMI), Centre National de Référence des Mycobactéries et de la Résistance aux Antituberculeux [CHU Pitié-Salpêtrière], Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Sorbonne Université (SU)-Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Sorbonne Université (SU), Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Chimie Moléculaire de Paris Centre (FR 2769), Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut National de la Santé et de la Recherche Médicale (INSERM), Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Paris (UP)-Université Sorbonne Paris Nord, Service de Bactériologie et d'Hygiène Hospitalière [CHU Pitié-Salpêtrière], Institut National des Sciences Appliquées - Strasbourg (INSA Strasbourg), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-École Nationale du Génie de l'Eau et de l'Environnement de Strasbourg (ENGEES)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Institut Pasteur [Paris]-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Université de Paris (UP), Noel, Anne-Laure, Décryptage du mode d'action de nouveaux antituberculeux prometteurs - - DETONATOR2020 - ANR-20-CE18-0030 - AAPG2020 - VALID, and Centre National de Référence des Mycobactéries et de la Résistance aux Antituberculeux [CHU Pitié-Salpêtrière] (CNR-MyRMA)
Subjects: Dose-Response Relationship, Drug, Molecular Structure, [CHIM.THER] Chemical Sciences/Medicinal Chemistry, ESKAPE, Microbial Sensitivity Tests, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, Quinolones, [SDV.MP.BAC]Life Sciences [q-bio]/Microbiology and Parasitology/Bacteriology, Neisseria gonorrhoeae, Anti-Bacterial Agents, Antibacterial, Structure-Activity Relationship, Synthesis, [SDV.MP.BAC] Life Sciences [q-bio]/Microbiology and Parasitology/Bacteriology, Hydrophobic and Hydrophilic Interactions, Fluoroquinolones
Abstract: International audience; This paper reports on the design of a series of 10 novel lipophilic piperazinyl derivatives of the 1-cyclopropyl-6-fluoro-8-methoxy-4-oxo-1,4-dihydroquinoline-3-carboxylic acid, their synthesis, their characterisation by 1H, 13C and 19F NMR, IR spectroscopy and HRMS, as well as their biological activity against bacteria of medical interest. Among these derivatives, 2 were as potent as the parent quinolone against Neisseriagonorrhoeae whereas all the compounds displayed lower activity than the parent quinolone against other bacteria of medical interest. Our results showing that the increased lipophilicity was deleterious for antibacterial activity may help to design new quinolone derivatives in the future, especially lipophilic quinolones which have been poorly investigated previously.
Published: 2022
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27. 3D Spectroscopic Tracking of Individual Brownian Nanoparticles during Galvanic Exchange

Author: Minh-Chau Nguyen, Pascal Berto, Fabrice Valentino, Jean-François Lemineur, Jean-Marc Noel, Frédéric Kanoufi, Gilles Tessier, Tessier, Gilles, Université Paris Cité (UPCité), Sorbonne Université (SU), Institut de la Vision, Institut National de la Santé et de la Recherche Médicale (INSERM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: [PHYS.PHYS.PHYS-OPTICS] Physics [physics]/Physics [physics]/Optics [physics.optics], Chemical Physics (physics.chem-ph), [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], Physics - Chemical Physics, General Engineering, General Physics and Astronomy, Soft Condensed Matter (cond-mat.soft), FOS: Physical sciences, General Materials Science, Condensed Matter - Soft Condensed Matter, Physics - Optics, Optics (physics.optics)
Abstract: Monitoring chemical reactions in solutions at the scale of individual entities is challenging: single particle detection requires small confocal volumes which are hardly compatible with Brownian motion, particularly when long integration times are necessary. Here, we propose a real-time (10 Hz) holography-based nm-precision 3D tracking of single moving nanoparticles. Using this localization, the confocal collection volume is dynamically adjusted to follow the moving nanoparticle and allow continuous spectroscopic monitoring. This concept is applied to the study galvanic exchange in freely-moving collo{\"i}dal silver nanoparticles with gold ions generated in-situ. While the Brownian trajectory reveals particle size, spectral shifts dynamically reveal composition changes and transformation kinetics at the single object level, pointing at different transformation kinetics for free and tethered particles., Comment: ACS Nano, American Chemical Society, 2022
Published: 2022
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28. Role of protective stoma after primary anastomosis for generalized peritonitis due to perforated diverticulitis—DIVERTI 2 (a prospective multicenter randomized trial): rationale and design (nct04604730)

Author: Jean Pinson, Jean-Jacques Tuech, Mehdi Ouaissi, Murielle Mathonnet, François Mauvais, Estelle Houivet, Elie Lacroix, Julie Rondeaux, Charles Sabbagh, Valérie Bridoux, DESSAIVRE, Louise, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Génomique et Médecine Personnalisée du Cancer et des Maladies Neuropsychiatriques (GPMCND), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut National de la Santé et de la Recherche Médicale (INSERM), EA4245 - Transplantation, Immunologie, Inflammation [Tours] (T2i), Université de Tours (UT), Université de Limoges (UNILIM), Chirurgie digestive [CHU Amiens], CHU Amiens-Picardie, Simplification des soins chez les patients complexes - UR UPJV 7518 (SSPC), Université de Picardie Jules Verne (UPJV), Unité de biostatistiques [CHU Rouen], CHU Rouen, Normandie Université (NU)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Centre de recherche en épidémiologie et santé des populations (CESP), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Hôpital Paul Brousse-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université Paris-Saclay, Endothélium, valvulopathies et insuffisance cardiaque (EnVI), Nouvelles Cibles Pharmacologiques de la Protection Endothéliale et de l'Insuffisance Cardiaque (EnVI), Normandie Université (NU)-Institut National de la Santé et de la Recherche Médicale (INSERM), Nutrition, Inflammation et axe Microbiote-Intestin-Cerveau (ADEN), Normandie Université (NU)-Normandie Université (NU)-Institute for Research and Innovation in Biomedicine (IRIB), Normandie Université (NU)-Normandie Université (NU)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM), Institute for Research and Innovation in Biomedicine (IRIB), Normandie Université (NU)-Normandie Université (NU)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), UNIROUEN - UFR Santé (UNIROUEN UFR Santé), Normandie Université (NU)-Normandie Université (NU), and Service de chirurgie digestive [CHU Rouen]
Subjects: [SDV.MHEP.CHI] Life Sciences [q-bio]/Human health and pathology/Surgery, Anastomosis, Surgical, General Medicine, [SDV.MHEP.CHI]Life Sciences [q-bio]/Human health and pathology/Surgery, Peritonitis, Diverticulitis, Colonic, Treatment Outcome, Intestinal Perforation, Colostomy, Quality of Life, Humans, Surgery, Prospective Studies, Diverticulitis
Abstract: Background Traditionally, patients with peritonitis Hinchey III and IV due to perforated diverticulitis were treated with Hartmann’s procedure. In the past decade, resection and primary anastomosis have gained popularity over Hartmann’s procedure and recent guidelines recommend Hartmann’s procedure in two situations only: critically ill patients and in selected patients with multiple comorbidity (at high risk of complications). The protective stoma (PS) is recommended after resection with primary anastomosis, however its interest has never been studied. The aim of this trial is to define the role of systematic PS after resection and primary anastomosis for peritonitis Hinchey III and IV due to perforated diverticulitis. Methods/design This DIVERTI 2 trial is a multicenter, randomized, controlled, superiority trial comparing resection and primary anastomosis with (control group) or without (experimental group) PS in patients with peritonitis Hinchey III and IV due to perforated diverticulitis. Primary endpoint is the overall 1 year morbidity according to the Clavien–Dindo classification of surgical complications. All complications occurring during hospitalization will be collected. Late complications occurring after hospitalization will be collected during follow-up. In order to obtain 80% power for a difference given by respective main probabilities of 67% and 47% in the protective stoma and no protective stoma groups respectively, with a two-sided type I error of 5%, 96 patients will have to be included in each group, hence 192 patients overall. Expecting a 5% rate of patients not assessable for the primary end point (lost to follow-up), 204 patients will be enrolled. Secondary endpoints are postoperative mortality, unplanned reinterventions, incisional surgical site infection (SSI), organ/space SSI, wound disruption, anastomotic leak, operating time, length of hospital stay, stoma at 1 year after initial surgery, quality of life, costs and quality-adjusted life years (QALYs). Discussion The DIVERTI 2 trial is a prospective, multicenter, randomized, study to define the best strategy between PS and no PS in resection and primary anastomosis for patients presenting with peritonitis due to perforated diverticulitis. Trial registration ClinicalTrial.gov: NCT04604730 date of registration October 27, 2020. https://clinicaltrials.gov/ct2/show/NCT04604730?recrs=a&cond=Diverticulitis&draw=2&rank=12.
Published: 2022
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29. Etching suppression as a means to Pt dendritic ultrathin nanosheets by seeded growth

Author: Deliang Yi, Cécile Marcelot, Idaline Romana, Marine Tassé, Pier-Francesco Fazzini, Laurent Peres, Nicolas Ratel-Ramond, Philippe Decorse, Bénédicte Warot-Fonrose, Guillaume Viau, Philippe Serp, Katerina Soulantica, Laboratoire de physique et chimie des nano-objets (LPCNO), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Fédération de recherche « Matière et interactions » (FeRMI), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de chimie de coordination (LCC), Institut de Chimie de Toulouse (ICT), Institut Laue-Langevin (ILL), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), University of Toulouse, and ANR-17-EURE-0009,NanoX,Science et Ingénierie à l'Echelle Nano(2017)
Subjects: General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract: International audience; 2D ultrathin metal nanostructures are emerging materials displaying distinct physical and chemical properties compared to their analogues of different dimensionalities. Nanosheets of fcc metals are intriguing, as their crystal structure does not favour a 2D configuration. Thanks to their increased surface-to-volume ratios and the optimal exposure of low-coordinated sites, 2D metal nanostructures can be advantageously exploited in catalysis. Synthesis approaches to ultrathin nanosheets of pure platinum are scarce compared to other noble metals and to Pt-based alloys. Here, we present the selective synthesis of Pt ultrathin nansosheets by a simple seeded-growth method. The most crucial point in our approach is the selective synthesis of Pt seeds comprising planar defects, a main driving force for the 2D growth of metals with fcc structure. Defect engineering is employed here, not in order to disintegrate, but for conserving the defect comprising seeds. This is achieved by in situ elimination of the principal etching agent, chloride, which is present in the PtCl2 precursor. As a result of etching suppression, twinned nuclei, that are selectively formed during the early stage of nucleation, survive and grow to multipods comprising planar defects. Using the twinned multipods as seeds for the subsequent 2D overgrowth of Pt from Pt(acac)2 yields ultrathin dendritic nanosheets, in which the planar defects are conserved. Using phenylacetylene hydrogenation as a model reaction of selective hydrogenation, we compared the performance of Pt nanosheets to that of a commercial Pt/C catalyst. The Pt nanosheets show better stability and much higher selectivity to styrene than the commercial Pt/C catalyst for comparable activity
Published: 2021
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30. Insights on asymmetric BTB-based molecular junctions: Effect of electrode coupling

Author: Sylvain Pitié, Mahamadou Seydou, Yannick J. Dappe, Pascal Martin, François Maurel, Jean Christophe Lacroix, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Service de physique de l'état condensé (SPEC - UMR3680), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Groupe Modélisation et Théorie (GMT), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, ANR-10-LABX-0096,SEAM,Science and Engineering for Advanced Materials and devices(2010), and ANR-18-IDEX-0001,Université de Paris,Université de Paris(2018)
Subjects: [PHYS]Physics [physics], General Physics and Astronomy, [CHIM]Chemical Sciences, Physical and Theoretical Chemistry
Abstract: International audience; NEGF and DFT calculations within Fisher Lee formalism are used to explore the effect of the asymmetry and the strength of coupling with the electrode on transport properties of (1-(2-bisthienyl)benzene) oligomers. Electronic analysis of metal-molecule interactions reveals the ionic nature of Ti-C bonds inducing an interfacial dipole. The Ti d-orbitals are found to be strongly coupled to the lowest unoccupied orbital of BTB, thus facilitating charge transfer from Ti to the molecule. The hole transport mechanism is found in the cases of Au-(BTB)$_n$-Au and Au-(BTB)$_n$-Ti while possible combined hole and electron transport is predicted in the case of Ti-(BTB)$_n$-Ti.
Published: 2021
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31. Bidentate pyridyl‐NHC ligands: synthesis, ground and excited state properties of their iron(II) complexes and role of the fac/mer isomerism

Author: Stefan Haacke, Antonio Francés-Monerris, Philippe C. Gros, Antonio Monari, Kévin Magra, Cristina Cebrian, Institut de Chimie Moléculaire et des Matériaux d'Orsay (ICMMO), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Facultat de Fisica [València] (UV), Universitat de València (UV), Laboratoire Lorrain de Chimie Moléculaire (L2CM), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Laboratoire de Physique et Chimie Théoriques (LPCT), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), A.F.-M.is grateful to Generalitat Valenciana and the European Social Fund (project GV/2020/226) and the Ministerio de Ciencia e Innovación (projectCTQ2017-87054-C2-2-P and Juande la Cierva contract IJC2019-039297-I) for financial support., ANR-16-CE07-0013,PhotIron,Design de complexes de fer à propriétés photophysiques applicables(2016), ANR-10-IDEX-0002,UNISTRA,Par-delà les frontières, l'Université de Strasbourg(2010), ANR-20-SFRI-0012,STRAT'US,Façonner les talents en formation et en recherche à l'Université de Strasbourg(2020), ANR-17-EURE-0024,QMAT,Quantum Science and Nanomaterials(2017), European Project: Synergie LO0024898,FEDER,FIRELIGHT(2018), GROS, PHILIPPE C., Design de complexes de fer à propriétés photophysiques applicables - - PhotIron2016 - ANR-16-CE07-0013 - AAPG2016 - VALID, Initiative d'excellence - Par-delà les frontières, l'Université de Strasbourg - - UNISTRA2010 - ANR-10-IDEX-0002 - IDEX - VALID, Façonner les talents en formation et en recherche à l'Université de Strasbourg - - STRAT'US2020 - ANR-20-SFRI-0012 - SFRI - VALID, Quantum Science and Nanomaterials - - QMAT2017 - ANR-17-EURE-0024 - EURE - VALID, and FireLight : Photo-bio-active molecules and nanoparticles - FIRELIGHT - - FEDER2018-01-01 - 2022-12-31 - Synergie LO0024898 - VALID
Subjects: Computational chemistry, Denticity, 010405 organic chemistry, Chemistry, Iron, Bidentate ligands, [CHIM.COOR] Chemical Sciences/Coordination chemistry, 010402 general chemistry, 01 natural sciences, Medicinal chemistry, 0104 chemical sciences, Inorganic Chemistry, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, Excited state, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Carbene ligands, Ultrafast spectroscopy
Abstract: International audience; Iron complexes are promising candidates for the development of sustainable molecular photoactive materials as an alternative to those based on precious metals such as Ir, Pt or Ru. These compounds possess metal-ligand charge transfer (MLCT) transitions potentially of high interest for energy conversion or photocatalysis applications if the ultrafast deactivation via lower-lying metal-centred (MC) states can be impeded. Following an introduction describing the main design strategies used so far to increase the MLCT lifetimes, we review some of our latest contributions to the field regarding bidentate Fe(II) complexes comprising N-heterocyclic carbene ligands. The discussion covers all aspects from their synthesis to their characterization via photophysical, electrochemical and computational techniques. The impact of bidentate coordination together with the configuration (facial and meridional isomers) is analysed, finally highlighting the current challenges in this promising area.
Published: 2021
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32. Multimodal Plasmonic Hybrids: Efficient and Selective Photocatalysts

Author: Miguel A. Correa-Duarte, Lucas V. Besteiro, Alexander O. Govorov, Zhiming Wang, Yoel Negrín-Montecelo, Miguel Comesaña-Hermo, Xiang-Tian Kong, Moisés Pérez-Lorenzo, Enrique Carbó-Argibay, Department of Physical Chemistry, Biomedical Research Center (CINBIO), Ohio University, International Iberian Nanotechnology Laboratory (INL), University of Electronic Science and Technology of China (UESTC), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: Materials science, Tandem, Energy transfer, Photocatalysis, Surface modification, [CHIM]Chemical Sciences, Charge carrier, Nanotechnology, 7. Clean energy, Plasmon, Hot-carrier injection, Spectral separation
Abstract: Important efforts are currently under way in order to implement plasmonic phenomena in the growing field of photocatalysis, striving for improved efficiency and reaction selectivity. A significant fraction of such efforts has been focused on distinguishing, understanding and enhancing specific energy transfer mechanisms from plasmonic nanostructures to their environment. Herein we report a synthetic strategy that brings together two of the main physical mechanisms driving plasmonic photocatalysis into an engineered system by rationally combining the photochemical features of energetic charge carriers and the electromagnetic field enhancement inherent to the plasmonic excitation. We do so by creating hybrid photocatalysts that integrate multiple plasmonic resonators in a single entity, controlling their joint contribution through spectral separation and differential surface functionalization. This strategy allows us to study the combination of different photosensitization mechanisms when activated simultaneously. Our results show that hot electron injection can be combined with an energy transfer process mediated by near-field interaction, leading to a significant increase of the final photocatalytic response of the material. In this manner, we overcome the limitations that hinder photocatalysis driven only by a single energy transfer mechanism, and move the field of plasmonic photocatalysis closer to energy-efficient applications. Furthermore, our multimodal hybrids offer a test system to probe the properties of the two targeted mechanisms in energy-related applications such as the photocatalytic generation of hydrogen and open the door to wavelength-selective photocatalysis and novel tandem reactions.
Published: 2021

33. Don’t help them to bury the light. The interplay between intersystem crossing and hydrogen transfer in photoexcited curcumin revealed by surface-hopping dynamics

Author: Antonio Monari, Raúl Losantos, Andreea Pasc, Laboratoire Lorrain de Chimie Moléculaire (L2CM), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), European Project: Synergie LO0024898,FEDER,FIRELIGHT(2018), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: Curcumin, Surface Properties, Population, General Physics and Astronomy, Surface hopping, 02 engineering and technology, Molecular Dynamics Simulation, 010402 general chemistry, Photochemistry, 01 natural sciences, chemistry.chemical_compound, [CHIM]Chemical Sciences, Physical and Theoretical Chemistry, Triplet state, education, education.field_of_study, Molecular Structure, Chemistry, Photochemical Processes, 021001 nanoscience & nanotechnology, Enol, Tautomer, 3. Good health, 0104 chemical sciences, Intersystem crossing, Photochemotherapy, Absorption (chemistry), 0210 nano-technology, Hydrogen
Abstract: Curcumin is a natural compound extracted from turmeric (Curcuma longa), which has shown remarkable anti-inflammatory, antibacterial, and possibly anticancer properties. The intense absorption in the visible domain and the possibility of intersystem crossing make curcumin attractive also for photodynamic therapy purposes. In the present contribution, we unravel, thanks to non-adiabatic surface hopping dynamics, the interplay between intersystem crossing and hydrogen transfer in the enol form, i.e. the most stable tautomer of curcumin. Most notably, we show that while hydrogen transfer is ultrafast and happens in the sub-ps regime, intersystem crossing is still present, as shown by the non-negligible population of the triplet state manifold after 2 ps. Hence, while the hydrogen transfer channel can act as a deactivating channel, curcumin, also in the red-shifted absorption enol form, can still be regarded as potentially favorable for photodynamic therapy applications.
Published: 2021
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34. Supramolecular organization and biological interaction of squalenoyl siRNA nanoparticles

Author: Caillaud, Marie, Gobeaux, Frédéric, Hémadi, Miryana, Boutary, Suzan, Guenoun, Patrick, Desmaële, Didier, Couvreur, Patrick, Wien, Frank, Testard, Fabienne, Massaad-Massade, Liliane, Massaad- Massade, Liliane, Massade, Liliane, Maladies et hormones du système nerveux (DHNS), Institut National de la Santé et de la Recherche Médicale (INSERM)-Université Paris-Saclay, Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Institut Galien Paris-Saclay (IGPS), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Petites Molécules de neuroprotection, neurorégénération et remyélinisation, and Université Paris-Sud - Paris 11 (UP11)-Institut National de la Santé et de la Recherche Médicale (INSERM)
Subjects: Squalene, [SDV.BIO]Life Sciences [q-bio]/Biotechnology, medicine.medical_treatment, Supramolecular chemistry, Pharmaceutical Science, Nanoparticle, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, Targeted therapy, 03 medical and health sciences, chemistry.chemical_compound, 0302 clinical medicine, X-Ray Diffraction, Scattering, Small Angle, Gene expression, structural studies, medicine, Biological media, [CHIM]Chemical Sciences, RNA, Small Interfering, ComputingMilieux_MISCELLANEOUS, 030304 developmental biology, 0303 health sciences, Bioconjugation, Chemistry, [SDV.BA]Life Sciences [q-bio]/Animal biology, Albumin, 3. Good health, biological interaction, 030220 oncology & carcinogenesis, siRNA, Biophysics, Nanoparticles, nanotechnologies
Abstract: International audience; Small interfering RNAs (siRNA) are attractive and powerful tools to inhibit the expression of a targeted gene. However, their extreme hydrophilicities combined with a negative charge and short plasma half-life counteract their use as therapeutics. Previously, we chemically linked siRNA to squalene (SQ) which self-assembled as nanoparticles (NPs) with pharmacological efficiency in cancers and recently in a hereditary neuropathy. In order to understand the siRNA-SQ NP assembly and fate once intravenously injected, the present study detailed characterization of siRNA-SQ NP structure and its interaction with serum components.From SAXS and SANS analysis, we propose that the siRNA-SQ bioconjugate self-assembled as 11-nm diameter supramolecular assemblies, which are connected one to another to form spherical nanoparticles of around 130-nm diameter. The siRNA-SQ NPs were stable in biological media and interacted with serum components, notably with albumin and LDL. The high specificity of siRNA to decrease or normalize gene expression and the high colloidal stability when encapsulated into squalene nanoparticles offer promising targeted therapy with wide applications for pathologies with gene expression dysregulation.
Published: 2021
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35. Structural and functional characterization of DdrC, a novel DNA damage-induced nucleoid associated protein involved in DNA compaction

Author: Anne-Sophie Banneville, Claire Bouthier de la Tour, Cécilia Hognon, Joanna Timmins, Pascale Servant, Antonio Monari, Jean-Marie Teulon, François Dehez, Aline Le Roy, Jacques-Philippe Colletier, Jean-Luc Pellequer, Fabrice Confalonieri, Institut de biologie structurale (IBS - UMR 5075), Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Institut de Biologie Intégrative de la Cellule (I2BC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie Théoriques (LPCT), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), The ANR (Agence Nationale de la Recherche) and CGI (Commissariat à l’Investissement d’Avenir) are gratefully acknowledged for their financial support of this work through Labex SEAM (Science and Engineering for Advanced Materials and devices): ANR-11-LABX-086 and ANR-11-IDEX-05-02, ANR-10-INBS-0005,FRISBI,Infrastructure Française pour la Biologie Structurale Intégrée(2010), ANR-10-LABX-0049,GRAL,Grenoble Alliance for Integrated Structural Cell Biology(2010), ANR-17-EURE-0003,CBH-EUR-GS,CBH-EUR-GS(2017), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: 0303 health sciences, DNA Repair, [SDV.BBM.BS]Life Sciences [q-bio]/Biochemistry, Molecular Biology/Structural Biology [q-bio.BM], biology, 030306 microbiology, Chemistry, DNA damage, DNA repair, Deinococcus radiodurans, biology.organism_classification, Cell biology, DNA binding site, 03 medical and health sciences, chemistry.chemical_compound, Bacterial Proteins, Genetics, Nucleoid, A-DNA, Deinococcus, DNA, Circular, Gene, DNA, DNA Damage, 030304 developmental biology
Abstract: Deinococcus radiodurans is a spherical bacterium well-known for its outstanding resistance to DNA-damaging agents. Exposure to such agents leads to drastic changes in the transcriptome of D. radiodurans. In particular, four Deinococcus-specific genes, known as DNA Damage Response genes, are strongly up-regulated and have been shown to contribute to the resistance phenotype of D. radiodurans. One of these, DdrC, is expressed shortly after exposure to γ-radiation and is rapidly recruited to the nucleoid. In vitro, DdrC has been shown to compact circular DNA, circularize linear DNA, anneal complementary DNA strands and protect DNA from nucleases. To shed light on the possible functions of DdrC in D. radiodurans, we determined the crystal structure of the domain-swapped DdrC dimer at a resolution of 2.2 Å and further characterized its DNA binding and compaction properties. Notably, we show that DdrC bears two asymmetric DNA binding sites located on either side of the dimer and can modulate the topology and level of compaction of circular DNA. These findings suggest that DdrC may be a DNA damage-induced nucleoid-associated protein that enhances nucleoid compaction to limit the dispersion of the fragmented genome and facilitate DNA repair after exposure to severe DNA damaging conditions.
Published: 2021
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36. Molecular Mechanisms Associated with Clustered Lesion-Induced Impairment of 8-oxoG Recognition by the Human Glycosylase OGG1

Author: Tao Jiang, Antonio Monari, Elise Dumont, Emmanuelle Bignon, Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie Théoriques (LPCT), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Institut Universitaire de France (IUF), and Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.)
Subjects: Guanine, DNA repair, DNA damage, [PHYS.PHYS.PHYS-BIO-PH]Physics [physics]/Physics [physics]/Biological Physics [physics.bio-ph], Pharmaceutical Science, Computational biology, Molecular Dynamics Simulation, Genome, Article, Analytical Chemistry, Lesion, chemistry.chemical_compound, QD241-441, clustered DNA lesions, Base Excision Repair Pathway, Drug Discovery, medicine, [CHIM]Chemical Sciences, Humans, heterocyclic compounds, Physical and Theoretical Chemistry, Chemistry, Organic Chemistry, DNA, molecular dynamics, Chemistry (miscellaneous), DNA glycosylase, DNA glycosylases, Molecular Medicine, medicine.symptom, DNA Damage
Abstract: The 8-oxo-7,8-dihydroguanine, referred to as 8-oxoG, is a highly mutagenic DNA lesion that can provoke the appearance of mismatches if it escapes the DNA Damage Response. The specific recognition of its structural signature by the hOGG1 glycosylase is the first step along the Base Excision Repair pathway, which ensures the integrity of the genome by preventing the emergence of mutations. 8-oxoG formation, structural features, and repair have been matters of extensive research, more recently, this active field of research expended to the more complicated case of 8-oxoG within clustered lesions. Indeed, the presence of a second lesion within 1 or 2 helix turns can dramatically impact the repair yields of 8-oxoG by glycosylases. In this work, we use μs-range molecular dynamics simulations and machine-learning-based postanalysis to explore the molecular mechanisms associated with the recognition of 8-oxoG by hOGG1 when embedded in a multiple-lesion site with a mismatch in 5′ or 3′. We delineate the stiffening of the DNA–protein interactions upon the presence of the mismatches, and rationalize the much lower repair yields reported with a 5′ mismatch by describing the perturbation of 8-oxoG structural features upon addition of an adjacent lesion.
Published: 2021
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37. Electrografting and Langmuir-Blodgett: Covalently Bound Nanometer-Thick Ordered Films on Graphite

Author: Xiaonan Sun, Jean-Philippe Michel, Da Li, Jean Pinson, Claire Mangeney, Jérôme Médard, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Laboratoire de Chimie et de Biochimie Pharmacologiques et Toxicologiques (LCBPT - UMR 8601), Institut Galien Paris-Saclay (IGPS), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), ANR-10-LABX-0096,SEAM,Science and Engineering for Advanced Materials and devices(2010), and ANR-18-IDEX-0001,Université de Paris,Université de Paris(2018)
Subjects: Langmuir, Materials science, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Langmuir–Blodgett film, law.invention, symbols.namesake, Highly oriented pyrolytic graphite, law, Monolayer, Electrochemistry, General Materials Science, Spectroscopy, Organic electronics, [CHIM.MATE]Chemical Sciences/Material chemistry, Surfaces and Interfaces, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Chemical engineering, symbols, Surface modification, Scanning tunneling microscope, [CHIM.OTHE]Chemical Sciences/Other, 0210 nano-technology, Raman spectroscopy
Abstract: International audience; We present two different molecular organizations obtained from octadecylamine (ODA) molecules on Highly Oriented Pyrolytic Graphite (HOPG) surface: i) self-organized physisorbed ODA molecules lying flat on the surface and ii) strongly electrografted compact crystalline monolayer of ODA molecules standing up on the surface. This new structure is obtained by combining the Langmuir-Blodgett transfer of an ODA Langmuir film onto HOPG with oxidative electrografting. The presence of organic film on HOPG is characterized by ATR-IR (Attenuated Total Reflectance-Infrared Spectroscopy) and Raman spectroscopies, while Atomic Force Microscopy (AFM) and Scanning Tunneling Microscopy (STM) allow the observation of the two molecular organizations, with adsorbed molecules lying flat on HOPG or strongly grafted in an upright position on the HOPG surface. Interestingly, the second molecular organization preserves a hexagonal symmetry and its lattice parameters are intermediate between those of ODA Langmuir films and that of HOPG underlying surface. The functionalization of surfaces with organic films is a major issue in the design of sensors with biomedical applications, or organic electronics and energy storage devices and these structures may find applications in these fields.
Published: 2021
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38. Polyol-Made Spinel Ferrite Nanoparticles—Local Structure and Operating Conditions: NiFe2O4 as a Case Study

Author: GAUDISSON, T., Nowak, S., Nehme, Z., Menguy, N., Yaacoub, N., Grenèche, J.-M., Ammar, S., Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: inorganic chemicals, 57Fe Mossbauer spectrometry, Technology, polyol-mediated annealing, [CHIM]Chemical Sciences, local structure analysis, 57 Fe Mossbauer spectrometry, ferrite nanoparticles, polyol process
Abstract: International audience; We report the effect of a polyol-mediated annealing on nickel ferrite nanoparticles. By combining X-ray fluorescence spectroscopy, X-ray diffraction, and 57 Fe Mössbauer spectrometry, we showed that whereas the as-prepared nanoparticles (NFO) are stoichiometric, the annealed ones (a-NFO) are not, since Ni 0-based crystals precipitate. Nickel depletion from the spinel lattice and reduction in the polyol solvent are accompanied with an important cation migration. Indeed, thanks to Mössbauer hyperfine structure analysis, we evidenced that the cation distribution in NFO departs from the thermodynamically stable inverse spinel structure with a concentration of tetrahedrally coordinated Ni 2+ of 20 wt-% (A sites). After annealing, and nickel demixing, originated very probably from the A sites of NFO lattice, the spinel phase accommodates with cation and anion vacancies, leading to the (Fe 3+ 0.84□0.16) A [Ni 2+ 0.80 Fe 3+ 1.16□0.04 ] B O 4-0.20 formula, meaning that the applied polyol-mediated treatment is not so trivial.
Published: 2021
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39. Direct vs Indirect Grafting of Alkyl and Aryl Halides

Author: Catherine Combellas, Dardan Hetemi, Frédéric Kanoufi, Fetah I. Podvorica, University of Prishtina, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: Steric effects, Radical, Halide, 02 engineering and technology, aryl iodides, 010402 general chemistry, 01 natural sciences, chemistry.chemical_compound, direct reduction, Polymer chemistry, [CHIM]Chemical Sciences, Reactivity (chemistry), Physical and Theoretical Chemistry, Alkyl, alkyl halides, Carbanion, chemistry.chemical_classification, indirect reduction, Aryl, Chemical modification, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, steric hindrance, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other
Abstract: International audience; The direct and indirect electrochemical grafting of alkyl and aryl halides (RX, ArX) on carbon, metal and polymer surfaces is examined. Their electrochemical reduction occurs at highly negative potential in organic solvents and very often produces carbanions because the reduction potentials of RX and ArX are more negative than those of their corresponding radicals. Therefore, direct electrografting of alkyl and aryl radicals generated from RX and ArX is not easy to perform. This obstacle is overcome using aryl radicals derived from the 2,6dimethylbenzenediazonium salt (2,6-DMBD), which do not react on the electrode surface due to their steric hindrance but react in solution by abstracting an iodine or bromine atom from RX (X= I, Br) or ArI to give alkyl or aryl radicals. As a consequence, alkyl and aryl radicals are generated at very low driving force by diverting the reactivity of aryl radicals derived from an aryl diazonium salt; they attack the electrode surface and form strongly attached organic layers. This strategy applies to the chemical modification of polymers (polyethylene, polymethylmethacrylate) by alkyl halides under heating.
Published: 2021
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40. Unprecedented ON/OFF Ratios in Photoactive Diarylethene-Bisthienylbenzene Molecular Junctions

Author: Sebastien Bellynck, Frédéric Lafolet, Imen Hnid, Denis Frath, Jean-Christophe Lacroix, Xiaonan Sun, Mingyang Liu, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: Materials science, Molecular junction, Bioengineering, 02 engineering and technology, 010402 general chemistry, Electrochemistry, electroswitch, 01 natural sciences, chemistry.chemical_compound, Diarylethene, modified surfaces, General Materials Science, Quantum tunnelling, Deposition (law), molecular junctions, photoswitch, Photoswitch, business.industry, Mechanical Engineering, Bilayer, Conductance, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, diarylethenes, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry, Optoelectronics, Electronics, 0210 nano-technology, business
Abstract: International audience; Photoactive molecular junctions, based on 4 nm thick diarylethene (DAE) and 5 nm thick bisthienylbenzene (BTB) layers, were fabricated by electrochemical deposition. Total thickness was around 9 nm, that is, above the direct tunneling limit and in the hopping regime. The DAE units were switched between their open and closed forms. The DAE/BTB bilayer structure exhibits new electronic functions combining photoswitching and photorectification. The open form of DAE/BTB shows low conductance and asymmetric I–V curves while the closed form shows symmetric I–V curves and high conductance. More importantly, unprecedented ON/OFF current ratios of over 10 000 at 1 V were reproducibly measured.
Published: 2021
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41. Electron Storage System Based on a Two-Way Inversion of Redox Potentials

Author: Ilaria Ciofini, Fabien Tuyèras, Magdaléna Hromadová, Štěpánka Nováková Lachmanová, Philippe P. Lainé, Christian Perruchot, Henri-Pierre Jacquot de Rouville, Philippe Ochsenbein, Grégory Dupeyre, Lubomír Pospíšil, Alexis Gosset, Hyacinthe Randriamahazaka, Romana Sokolová, Liam Wilbraham, Université de Paris, Laboratoire ITODYS, CNRS, F-75006 Paris, Institute of Chemistry for Life and Health Sciences (iCLeHS), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Laboratoire de Chimie Inorganique et Matériaux Moléculaires (CIM2), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Sanofi-Aventis R&D, SANOFI Recherche, Institut de Chimie de Strasbourg, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Electronique et intelligence artificielle (UR ELAN), and Centre national du machinisme agricole, du génie rural, des eaux et forêts (CEMAGREF)
Subjects: [CHIM.ORGA]Chemical Sciences/Organic chemistry, Chemistry, General Chemistry, Electron, 010402 general chemistry, 01 natural sciences, Biochemistry, Inversion (discrete mathematics), Redox, Catalysis, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Solar energy harvesting, Electron storage, Colloid and Surface Chemistry, Chemical bond, Chemical physics, ComputerApplications_MISCELLANEOUS, [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract: International audience; Molecular-level multielectron handling toward electrical storage is a worthwhile approach to solar energy harvesting. Here, a strategy which uses chemical bonds as electron reservoirs is introduced to demonstrate the new concept of "structronics" (a neologism derived from "structure" and "electronics"). Through this concept, we establish, synthesize, and thoroughly study two multicomponent "super-electrophores": 1,8-dipyridyliumnaphtha-lene, 2, and its N,N-bridged cyclophane-like analogue, 3. Within both of them, a covalent bond can be formed and subsequently broken electrochemically. These superelectrophores are based on two electrophoric (pyridinium) units that are, on purpose, spatially arranged by a naphthalene scaffold. A key characteristic of 2 and 3 is that they possess a LUMO that develops through space as the result of the interaction between the closely positioned electrophoric units. In the context of electron storage, this "super-LUMO" serves as an empty reservoir, which can be filled by a two-electron reduction, giving rise to an elongated C−C bond or "super-HOMO". Because of its weakened nature, this bond can undergo an electrochemically driven cleavage at a significantly more anodicyet accessiblepotential, thereby restoring the availability of the electron pair (reservoir emptying). In the representative case study of 2, an inversion of potential in both of the two-electron processes of bond formation and bond-cleavage is demonstrated. Overall, the structronic function is characterized by an electrochemical hysteresis and a chemical reversibility. This structronic superelectrophore can be viewed as the three-dimensional counterpart of benchmark methyl viologen (MV).
Published: 2020
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42. Revealing the sub-50 ms electrochemical conversion of silver halide nanocolloids by stochastic electrochemistry and optical microscopy

Author: Jean-François Lemineur, Jean-Marc Noël, Frédéric Kanoufi, Catherine Combellas, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), ANR-15-CE09-0015,NEOCASTIP,Electrochimie aux échelles nanométriques par screening chimique et localisation optique de trajectoires de nanoparticules individuelles(2015), and ANR-18-IDEX-0001,Université de Paris,Université de Paris(2018)
Subjects: Materials science, Silver halide, Nanoparticle, Context (language use), [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, Redox, 0104 chemical sciences, Nanomaterials, chemistry.chemical_compound, Nanofluid, chemistry, Chemical engineering, Electrode, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, [CHIM]Chemical Sciences, General Materials Science, [CHIM.OTHE]Chemical Sciences/Other, 0210 nano-technology
Abstract: International audience; Silver based ionic crystal nanoparticles (NPs) are interesting nanomaterials for energy storage and conversion, e.g. their colloidal solutions could be used as a reversible redox nanofluid in semi-solid redox flow cells. In this context, the reductive transformation of Brownian silver halide, AgX, NPs into silver NPs is probed by single NP electrochemistry, complemented by operando high resolution monitoring. However, their light sensitivity and poor conductivity make the operando monitoring of their chemical activity challenging. The electrochemical collisions of single AgX NPs onto a negatively biased electrode evidence a full conversion through multiple reduction steps within 3–10 ms. This is further corroborated by simulation of the conversion process and operando through a high resolution optical microscopy technique (Backside Absorbing Layer Microscopy, BALM). Both techniques are interesting strategies to infer at the single NP level the intrinsic charge capacity and charging rate of redox active Brownian nanomaterials, demonstrating the interest of the fast and reversible AgX/Ag system as a redox nanofluid.
Published: 2020
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43. Photo-anodes based on TiO2 and carbon dots for photo-electrocatalytical measurements

Author: S. Chaguetmi, Souad Ammar, Delphine Schaming, Ari Gurel, Philippe Decorse, Sophie Nowak, Stéphanie Lau, Humay Aliyeva, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Université 20 Août 1955 Skikda
Subjects: Materials science, chemistry.chemical_element, Context (language use), 02 engineering and technology, Conductivity, 010402 general chemistry, 01 natural sciences, 7. Clean energy, [CHIM]Chemical Sciences, General Materials Science, Photocurrent, business.industry, Mechanical Engineering, Doping, Chromophore, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Anode, Semiconductor, chemistry, Mechanics of Materials, Optoelectronics, 0210 nano-technology, business, Carbon
Abstract: Wide band-gap semiconductor TiO2 is an efficient anode material for photo-electrocatalytical (PEC) applications. Its light-sensitivity is limited to the UV but can be extended to the visible by chemical doping or chromophore sensitization. Moreover, its conductivity can be enhanced by coupling with carbon materials, which should limit back electron-hole recombination. In this context, we prepared hetero-nanostructures based on TiO2 nanofibers supported on Ti sheet and impregnated with carbon dots (CDs), and used them as photo-anodes in photo-electrochemical cells. They showed a higher photocurrent than non-CD-impregnated photo-anodes, underlining the importance of CDs for water-splitting processing.
Published: 2019
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44. Surface functionalization of CoFe2O4 nanoparticles for driving the crystallization of the electroactive β-PVDF through judicious tailoring of the hybrid interface

Author: Elise Barthas, Chirine Ben Osman, Philippe Decorse, Fayna Mammeri, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)
Subjects: chemistry.chemical_classification, Materials science, Nanoparticle, 02 engineering and technology, Polymer, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, Miscibility, Ferroelectricity, 0104 chemical sciences, law.invention, Crystallinity, Colloid and Surface Chemistry, Differential scanning calorimetry, chemistry, Chemical engineering, law, [CHIM]Chemical Sciences, Surface modification, Crystallization, 0210 nano-technology
Abstract: Recently, extrinsic polymer-based magnetoelectric multiferroic materials have been investigated for many applications in nanoelectronics and energy harvesting. For that, poly(vinylidene fluoride) (PVDF), crystallized in β-phase, is known to present good ferroelectric and piezoelectric properties. We report here the functionalization of cobalt ferrite nanoparticles, known to be magnetostrictive, by a 1H,2H,2H-Perfluorooctanephosphonic acid (PFOP) for their better miscibility in PVDF. Hybrid self-standing films have been prepared; the degree of crystallinity (Xmc), as well as the fraction of β-polymorph, have been determined as a function of the amount of either functionalized or not nanoparticles, combining infrared (IR) spectroscopy and differential scanning calorimetry (DSC). We evidenced that the use of functionalized nanoparticles induced a better crystallinity degree as well as an improvement of the whole crystallization of β-PVDF polymorph. These results highlight the crucial role of the hybrid interface, when tailored through suitable surface chemistry, on the morphology developed by the hybrid.
Published: 2019
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45. Corrosion Protection of Cu Electrical Cable by W-Ni Composite Coatings Doped with TiO2 Nanoparticles: Influence of Pulse Currents

Author: J.-Y. Hihn, L. Dhouibi, M. Rezrazi, William Sassi, Patrice Berçot, Salah Ammar, Univers, Transport, Interfaces, Nanostructures, Atmosphère et environnement, Molécules (UMR 6213) (UTINAM), Université de Franche-Comté (UFC), Université Bourgogne Franche-Comté [COMUE] (UBFC)-Université Bourgogne Franche-Comté [COMUE] (UBFC)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), Laboratoire de Mécanique Appliquée et Ingénierie [Tunis] (LR-MAI-ENIT), Ecole Nationale d'Ingénieurs de Tunis (ENIT), Université de Tunis El Manar (UTM)-Université de Tunis El Manar (UTM), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Franche-Comté (UFC), Laboratoire de Mécanique Appliquée et Ingénierie (COPROMET), Université Tunis El Manar (UTM), and Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7)
Subjects: 010302 applied physics, Materials science, Mechanical Engineering, Alloy, Composite number, Nanoparticle, chemistry.chemical_element, 02 engineering and technology, engineering.material, 021001 nanoscience & nanotechnology, 01 natural sciences, Copper, Grain size, Corrosion, Coating, chemistry, Mechanics of Materials, 0103 physical sciences, engineering, General Materials Science, Composite material, [PHYS.ASTR]Physics [physics]/Astrophysics [astro-ph], 0210 nano-technology, Porosity, ComputingMilieux_MISCELLANEOUS
Abstract: W-Ni-TiO2 nano-composite layers were electrodeposited on copper surface by both direct (DC) and pulse (PC) currents. The copper substrates are samples from the main electrical cable used for the Renault K-Z (the latest 100% electric vehicle). In order to investigate coating morphology, atomic force microscopy was used, while energy-dispersive x-ray analysis was applied to determine nano-composite composition. Based on surface morphology, the W-Ni-TiO2 (DC) alloy surface was covered by massive agglomerates, especially when the W-Ni-TiO2 (PC) nano-composite coating was more compact, thicker and exhibited smaller grain size. The coated surface revealed different contents such as 43.4 and 65.4% of W in DC and PC coatings, respectively, which are considered to be a novel composition of the W-Ni alloy. XRD studies revealed that the NiW2 phase only occurs in the W-Ni-TiO2 (PC) nano-composite alloy. Electrical and thermal conductivities, microhardness and porosity values are enhanced by the addition of TiO2 to the alloy.
Published: 2019
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46. New Iron Oxide Nanoparticles Catechol-Grafted with Bis(amidoxime)s for Uranium(VI) Depletion of Aqueous Solution

Author: E. Mazario, Alvaro Mayoral, Rémi Losno, Ahmed S. Helal, Claude Lion, Souad Ammar, Jérémy Stemper, Miryana Hémadi, Thierry Le Gall, Philippe Decorse, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Univ Paris Saclay, CEA, Inst Sci Vivant Joliot Curie, Serv Chim Bioorgan & Marquage, Bat 547, F-91191 Gif Sur Yvette, France, MIT, Dept Nucl Sci & Engn, 77 Massachusetts Ave, Cambridge, MA 02139 USA, Nucl Mat Author, POB 540, Cairo, Egypt, Laboratorio de microscopias avanzadas (LMA), University of Zaragoza - Universidad de Zaragoza [Zaragoza], Institut de Physique du Globe de Paris (IPGP), Institut national des sciences de l'Univers (INSU - CNRS)-IPG PARIS-Université de La Réunion (UR)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Service de Chimie Bio-Organique et de Marquage (SCBM), Médicaments et Technologies pour la Santé (MTS), Université Paris-Saclay-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Université Paris-Saclay-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), IPGP multidisciplinary program PARI Paris-IdF region SESAME 12015908, Institut de Physique du Globe de Paris (IPGP (UMR_7154)), and Institut national des sciences de l'Univers (INSU - CNRS)-Université de La Réunion (UR)-Institut de Physique du Globe de Paris (IPG Paris)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: Langmuir, Materials science, genetic structures, Iron Oxide Nanoparticle, Biomedical Engineering, chemistry.chemical_element, Bioengineering, Environmental pollution, 02 engineering and technology, Magnetic Separation, Amidoxime, Spectrophotometry, medicine, General Materials Science, Freundlich equation, Fourier transform infrared spectroscopy, Functionalization, Aqueous solution, medicine.diagnostic_test, Uranium Removal, Sorption, General Chemistry, Uranium, 021001 nanoscience & nanotechnology, Condensed Matter Physics, eye diseases, chemistry, [SDU]Sciences of the Universe [physics], 13. Climate action, sense organs, 0210 nano-technology, Nuclear chemistry
Abstract: International audience; Environmental pollution caused by heavy metals constitutes a serious public health problem. In the case of uranium depletion, amidoxime groups are important because of their high affinity for uranium(VI). New series of bis(amidoxime)s with catechol-derived anchor groups were tested (b-AMD-1 and b-AMD-2). The catechol groups were designed to bind to the surface of maghemite nanoparticles (MNPs), and two nanohybrid devices MNP-b-AMD-1 and MNP-b-AMD-2 were obtained. This strategy makes for efficient removal of U(VI) via its complexation with the bis(amidoxime)s (b-AMD) and also its extraction from aqueous solution by magnetic harvesting of the MNPs. The assynthesized and b-AMD-grafted MNPs were characterized by several techniques: X-ray diffraction (XRD), high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM), X-ray photoelectron spectrophotometry (XPS), thermal analysis (TG/DTA) and Fourier transform infrared spectroscopy (FTIR). Sorption tests were run at pH 6.5, which corresponds to the highest affinity and selectivity of b-AMD for U(VI). After magnetic separation, the chelation ability and the selectivity of MNP-b-AMD-1 and MNP-b-AMD-2 towards U(VI) were evaluated by measuring the residual U(VI) concentration in the supernatant by inductively coupled plasma-mass spectrometry (ICP-MS). The data were plotted according to the Langmuir and Freundlich isotherms; the maximal sorption capacity (q(max)) was 29 and 60 mg U g(-1) for MNP-b-AMD-1 and MNP-b-AMD-2, respectively. This confirms that bis(amidoxime) groups are good candidates for uranium depletion of aqueous solution
Published: 2019
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47. Investigating the effects of different natural molecules on the structure and oligomerization propensity of hen egg-white lysozyme

Author: Ali Chaari, Christine Fahy, Alexandre Chevillot-Biraud, Mohamed Rholam, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Laboratoire de génétique et biologie cellulaire (LGBC), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)
Subjects: Amyloid, [SDV]Life Sciences [q-bio], DLS, 02 engineering and technology, Protein aggregation, Fibril, Trp, Biochemistry, Aggregation kinetics Amyloidosis Aggregation inhibitors Anti-amyloidogenic Hen-egg-white lysozyme Natural compounds HEWL, Protein Aggregates, 03 medical and health sciences, chemistry.chemical_compound, hen egg white lysozyme, Structural Biology, medicine, tryptophan, Molecular Biology, 030304 developmental biology, Biological Products, 0303 health sciences, atomic force microscopy, Dose-Response Relationship, Drug, thioflavin T, Chemistry, Amyloidosis, Tryptophan, attenuated total reflectance-Fourier transform infrared, dynamic light scattering, General Medicine, 021001 nanoscience & nanotechnology, medicine.disease, Small molecule, In vitro, 3. Good health, Kinetics, ThT, Biophysics, Muramidase, Protein Multimerization, AFM, Lysozyme, 0210 nano-technology, ATR-FTIR
Abstract: International audience; The formation of amyloid aggregates is the hallmark of systemic and neurodegenerative diseases, also known as amyloidosis. Many proteins have been found to aggregate into amyloid-like fibrils and thus process is recognized as general tendency of polypeptides. Inhibition of protein aggregation and fibril formation is thus one of the important strategies in the prevention and treatment of such disease. There is a growing interest of identification of small molecules mainly natural compounds that can prevent or delay amyloid fibril formation. In this work, we report the effect of various compounds from different groups on the amyloid fibrillation of hen egg white lysozyme, a model protein for amyloid formation. Herein, a range of biophysical techniques have been employed in order to establish a systematic approach to study the effect of candidate inhibitors on amyloid aggregation. Results demonstrated that the strategy used show that the different techniques are complimentary in order to elucidate a complete in vitro picture of the effect of the used compounds on HEWL aggregation. Moreover, compared to the data obtained by other groups for the inhibition of lysozyme fibril formation, this work provides new insights into the structural changes (local, secondary, oligomeric, fibrillar structures) undergone by HEWL during aggregation in the presence and absence of inhibitors.
Published: 2019
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48. Enhanced output voltage of nano energy harvester with diverse textiles

Author: Jae Hoon Ko, Su-Young Choi, Jong-Hyoung Kim, Sohee Lee, Hyeok Kim, Kyungmin Lim, Alexandra Tibaldi, Do-Kyung Kim, Tae-Young Ma, Jin-Hyuk Bae, Swarup Biswas, Hanchul Cho, Suwoong Lee, Philippe Lang, Jae Bum Jeong, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, ComputerApplications_COMPUTERSINOTHERSYSTEMS, 02 engineering and technology, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Energy harvester, Hardware_GENERAL, Nano, [CHIM]Chemical Sciences, General Materials Science, Nano energy harvester, Triboelectric effect, Wearable technology, [PHYS]Physics [physics], triboelectricity, business.industry, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Engineering physics, textiles, 0104 chemical sciences, 0210 nano-technology, business, Energy (signal processing), Voltage
Abstract: International audience; We demonstrate the electrical properties of nano energy harvesters (NEHs) with various textiles for smart textiles that can be applied to the next generation wearable electronics. Output voltages and currents of NEHs with various fabrics, such as a cotton, rayon and wool that have different triboelectricity were measured. Cotton, rayon and wool shows the maximum output voltages of 1.250, 3.313 and 4.063 V, respectively. In addition, output currents of those textiles were 0.75, 4.4, 1.063 lA, respectively. Wool, in particular, which has the highest triboelectricity of 350 V exhibits the highest output voltage.
Published: 2019
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49. Bottom-up assembly of Au@Ag plasmonic nanocrystals: Issues to be addressed to achieve a good SERS substrate

Author: Leïla Boubekeur-Lecaque, Israa Haidar, Alexandre Chevillot-Biraud, Umberto Martino, Axelle Day, Nordin Félidj, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7)
Subjects: Materials science, Nanoparticle, Substrate (chemistry), Nanotechnology, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, symbols.namesake, Nanocrystal, symbols, [CHIM]Chemical Sciences, General Materials Science, 0210 nano-technology, Spectroscopy, Raman spectroscopy, ComputingMilieux_MISCELLANEOUS, Plasmon, Raman scattering, Macromolecule
Abstract: Plasmonic substrate is a key component in surface-enhanced Raman scattering (SERS) spectroscopy to boost the Raman signal of analytes. The quality of SERS substrate is assessed primarily on the basis of its sensitivity, reproducibility and robustness. Despite major achievements in the field over the last decade, reliable SERS substrates fabricated by the bottom-up assembly of colloids are still rare on the market not to say absent in routine analytics. In this work, we investigated several important aspects from the optimization of colloids organization on solid support to the SERS analytical performance (sensitivity, stability and reproducibility) for detecting pesticides such as thiram. We show that the surfactant surrounding colloids usually considered as a limitation for the detection of macromolecules, proved to be a major advantage to induce assembly of nanoparticles on solid support and to improve the affinity of hydrophobic analytes for metallic surface and for the long-term stability of the substrate.
Published: 2019
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50. Optical Nanoimpacts of Dielectric and Metallic Nanoparticles on Gold Surface by Reflectance Microscopy: Adsorption or Bouncing?

Author: Claire Smadja, Catherine Combellas, Jean-François Lemineur, Jérôme Médard, Talia Jane Stockmann, Frédéric Kanoufi, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Institut Galien Paris-Sud (IGPS), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Laboratoires Sciences Analytiques, Bioanalytiques et Miniaturisation, ESPCI ParisTech-Centre National de la Recherche Scientifique (CNRS), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Sud - Paris 11 (UP11)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Sciences Analytiques, Bioanalytiques, et Miniaturisation (LSABM), Chimie-Biologie-Innovation (UMR 8231) (CBI), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)
Subjects: Materials science, Microscope, Microfluidics, Nanoparticle, 02 engineering and technology, Dielectric, 010402 general chemistry, 01 natural sciences, Analytical Chemistry, law.invention, chemistry.chemical_compound, Adsorption, law, Microscopy, Materials Chemistry, Electrochemistry, [CHIM]Chemical Sciences, Environmental Chemistry, Instrumentation, Spectroscopy, business.industry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, Electrode, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, Optoelectronics, Polystyrene, [CHIM.OTHE]Chemical Sciences/Other, 0210 nano-technology, business
Abstract: International audience; Optical modeling coupled to experiments show that a microscope operating in reflection mode allows imaging, through solutions or even a microfluidic cover, various kinds of nanoparticles, NPs, over a (reflecting) sensing surface, here a gold (Au) surface. Optical modeling suggests that this configuration enables the interferometric imaging of single NPs which can be characterized individually from local change in the surface reflectivity. The interferometric detection improves the optical limit of detection compared to classical configurations exploiting only the light scattered by the NPs. The method is then tested experimentally, to monitor in situ and in real time, the collision of single Brownian NPs, or optical nanoimpacts, with an Au-sensing surface. First, mimicking a microfluidic biosensor platform, the capture of 300 nm FeOx maghemite NPs from a convective flow by a surface-functionalized Au surface is dynamically monitored. Then, the adsorption or bouncing of individual dielectric (100 nm polystyrene) or metallic (40 and 60 nm silver) NPs is observed directly through the solution. The influence of the electrolyte on the ability of NPs to repetitively bounce or irreversibly adsorb onto the Au surface is evidenced. Exploiting such visualization mode of single-NP optical nanoimpacts is insightful for comprehending single-NP electrochemical studies relying on NP collision on an electrode (electrochemical nanoimpacts).
Published: 2019
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635 results on '"Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086))"'

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