Author: "Saad Sene" - Searchworks@Jio Institute Digital Library Search Results

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1. Luminescent Ln3+-based silsesquioxanes with a β-diketonate antenna ligand: toward the design of efficient temperature sensors

Author: Gautier Félix, Alena N. Kulakova, Saad Sene, Victor N. Khrustalev, Miguel A. Hernández-Rodríguez, Elena S. Shubina, Tristan Pelluau, Luís D. Carlos, Yannick Guari, Albano N. Carneiro Neto, Alexey N. Bilyachenko, and Joulia Larionova
Subjects: thermometry, silsesquioxanes, lanthanides, luminescence, magnetism, energy transfer, Chemistry, QD1-999
Abstract: We report the synthesis and single-crystal X-ray diffraction, magnetic, and luminescence measurements of a novel family of luminescent cage-like tetranuclear silsesquioxanes (PhSiO1.5)8(LnO1.5)4(O)(C5H8O2)6(EtOH)2(CH3CN)2⋅2CH3CN (where Ln = Tb, 1; Tb/Eu, 2; and Gd, 3), featuring seven-coordinated lanthanide ions arranged in a one-capped trigonal prism geometry. Compounds 1 and 2 exhibit characteristic Tb3+ and Tb3+/Eu3+-related emissions, respectively, sensitized by the chelating antenna acetylacetonate (acac) ligands upon excitation in the UV and visible spectral regions. Compound 3 is used to assess the energies of the triplet states of the acac ligand. For compound 1, theoretical calculations on the intramolecular energy transfer and multiphonon rates indicate a thermal balance between the 5D4 Stark components, while the mixed Tb3+/Eu3+ analog 2, with a Tb:Eu ratio of 3:1, showcases intra-cluster Tb3+-to-Eu3+ energy transfer, calculated theoretically as a function of temperature. By utilizing the intensity ratio between the 5D4→7F5 (Tb3+) and 5D0→7F2 (Eu3+) transitions in the range 11–373 K, we demonstrate the realization of a ratiometric luminescent thermometer with compound 2, operating in the range 11–373 K with a maximum relative sensitivity of 2.0% K−1 at 373 K. These findings highlight the potential of cage-like silsesquioxanes as versatile materials for optical sensing-enabled applications.
Published: 2024
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2. 4D Printing Nanocomposite Hydrogel Based on PNIPAM and Prussian Blue Nanoparticles Using Stereolithography

Author: Tristan Pelluau, Thomas Brossier, Michel Habib, Saad Sene, Gautier Félix, Joulia Larionova, Sébastien Blanquer, and Yannick Guari
Subjects: 4D printing, light induced polymerization, nanoparticles, poly(N‐isopropylacrylamide), Prussian blue, stereolithography, Materials of engineering and construction. Mechanics of materials, TA401-492, Engineering (General). Civil engineering (General), TA1-2040
Abstract: Abstract The potential of photoactive Prussian blue nanoparticles dispersed in thermo‐responsive PNIPAM hydrogels in 4D printing using a stereolithography is investigated with digital light processing. The proportion of Prussian blue nanoparticles used in the resin is chosen to deliver a significant photothermal effect providing a heating above the volume phase transition temperature of the final nanocomposite hydrogels; while, giving only a limited effect on light scattering during the 3D printing process. Four formulations with various amounts of Prussian blue nanoparticles are used to print 3D structures with different shapes, such as Aztec pyramids, cylinders, gyroid porous cubes, and porous films. The shrinkage effect triggered by light irradiation at 808 nm on the as‐obtained nanocomposite hydrogels is demonstrated through the delivery of a representative molecule fluorescein and a triggered 4D shape‐morphing effect.
Published: 2024
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3. Magnetic Iron Oxide Nanoparticles Coated by Coumarin-Bound Copolymer for Enhanced Magneto- and Photothermal Heating and Luminescent Thermometry

Author: Alexiane Féron, Sylvain Catrouillet, Saad Sene, Gautier Félix, Belkacem Tarek Benkhaled, Vincent Lapinte, Yannick Guari, and Joulia Larionova
Subjects: nanoparticles, polymeric coating, luminescence, thermometry, coumarin, Chemistry, QD1-999
Abstract: In this work, we report on the synthesis and investigation of new hybrid multifunctional iron oxide nanoparticles (IONPs) coated by coumarin-bound copolymer, which combine magneto- or photothermal heating with luminescent thermometry. A series of amphiphilic block copolymers, including Coum-C11-PPhOx27-PMOx59 and Coum-C11-PButOx8-PMOx42 bearing luminescent and photodimerizable coumarin moiety, as well as coumarin-free PPhOx27-PMOx57, were evaluated for their utility as luminescent thermometers and for encapsulating spherical 26 nm IONPs. The obtained IONP@Coum-C11-PPhOx27-PMOx59 nano-objects are perfectly dispersible in water and able to provide macroscopic heating remotely triggered by an alternating current magnetic field (AMF) with a specific absorption rate (SAR) value of 240 W.g−1 or laser irradiation with a photothermal conversion efficiency of η = 68%. On the other hand, they exhibit temperature-dependent emission of coumarin offering the function of luminescent thermometer, which operates in the visible region between 20 °C and 60 °C in water displaying a maximal relative thermal sensitivity (Sr) of 1.53%·°C−1 at 60 °C.
Published: 2024
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4. Magneto-Induced Hyperthermia and Temperature Detection in Single Iron Oxide Core-Silica/Tb3+/Eu3+(Acac) Shell Nano-Objects

Author: Karina Nigoghossian, Basile Bouvet, Gautier Félix, Saad Sene, Luca Costa, Pierre-Emmanuel Milhet, Albano N. Carneiro Neto, Luis D. Carlos, Erwan Oliviero, Yannick Guari, and Joulia Larionova
Subjects: luminescence, lanthanide coordination complexes, nanothermometry, magnetic iron oxide nanoparticles, magnetothermia, hybrid nano-systems, Chemistry, QD1-999
Abstract: Multifunctional nano-objects containing a magnetic heater and a temperature emissive sensor in the same nanoparticle have recently emerged as promising tools towards personalized nanomedicine permitting hyperthermia-assisted treatment under local temperature control. However, a fine control of nano-systems’ morphology permitting the synthesis of a single magnetic core with controlled position of the sensor presents a main challenge. We report here the design of new iron oxide core–silica shell nano-objects containing luminescent Tb3+/Eu3+-(acetylacetonate) moieties covalently anchored to the silica surface, which act as a promising heater/thermometer system. They present a single magnetic core and a controlled thickness of the silica shell, permitting a uniform spatial distribution of the emissive nanothermometer relative to the heat source. These nanoparticles exhibit the Tb3+ and Eu3+ characteristic emissions and suitable magnetic properties that make them efficient as a nanoheater with a Ln3+-based emissive self-referencing temperature sensor covalently coupled to it. Heating capacity under an alternating current magnetic field was demonstrated by thermal imaging. This system offers a new strategy permitting a rapid heating of a solution under an applied magnetic field and a local self-referencing temperature sensing with excellent thermal sensitivity (1.64%·K−1 (at 40 °C)) in the range 25–70 °C, good photostability, and reproducibility after several heating cycles.
Published: 2022
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5. Multifunctionalized Mesostructured Silica Nanoparticles Containing Mn2 Complex for Improved Catalase-Mimicking Activity in Water

Author: Tristan Pelluau, Saad Sene, Beltzane Garcia-Cirera, Belen Albela, Laurent Bonneviot, Joulia Larionova, and Yannick Guari
Subjects: nanoparticle, mesostructured silica, dendritic silica, manganese compounds, catalytic activity, catalase, Chemistry, QD1-999
Abstract: We report the synthesis of a hybrid nanocatalyst obtained through the immobilization of bio-inspired [{Mn(bpy)(H2O)}(µ-2-MeC6H4COO)2(µ-O){Mn(bpy)(NO3)}]NO3 compound into functionalized, monodispersed, mesoporous silica nanoparticles. The in situ dual functionalization sol–gel strategy adopted here leads to the synthesis of raspberry-shaped silica nanoparticles of ca. 72 nm with a large open porosity with preferential localization of 1,4-pyridine within the pores and sulfobetaine zwitterion on the nanoparticles’ periphery. These nano-objects exhibit improved catalase-mimicking activity in water thanks to the encapsulation/immobilization of the catalytic active complex and high colloidal stability in water, as demonstrated through the dismutation reaction of hydrogen peroxide.
Published: 2022
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6. Coordination Networks Based on Boronate and Benzoxaborolate Ligands

Author: Saad Sene, Marie Alix Pizzoccaro, Joris Vezzani, Marc Reinholdt, Philippe Gaveau, Dorothée Berthomieu, Sylvie Bégu, Christel Gervais, Christian Bonhomme, Guillaume Renaudin, Adel Mesbah, Arie van der Lee, Mark E. Smith, and Danielle Laurencin
Subjects: boronate, tri-hydroxyborate, benzoxaborolate, boronic acid, benzoxaborole, coordination polymer, solid state NMR, IR spectroscopy, crystallography, DFT, Crystallography, QD901-999
Abstract: Despite the extensive range of investigations on boronic acids (R-B(OH)2), some aspects of their reactivity still need to be explored. This is the case for the coordination chemistry of boronate anions (R-B(OH)3−), which has only recently been started to be studied. The purpose of this review is to summarize some of the key features of boronate ligands (and of their cyclic derivatives, benzoxaborolates) in materials: (i) coordination properties; (ii) spectroscopic signatures; and (iii) emerging applications.
Published: 2016
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7. Cascade strategy for triggered radical release by magnetic nanoparticles grafted with thermosensitive alkoxyamine

Author: Basile Bouvet, Saad Sene, Gautier Félix, Jeffrey Havot, Gerard Audran, Sylvain R. A. Marque, Joulia Larionova, and Yannick Guari
Subjects: General Materials Science
Abstract: The design of smart nanoplatforms presenting well-definite structures able to achieve controlled cascade action remotely triggered by external stimuli presents a great challenge. We report here a new nanosystem consisting of magnetic iron oxide nanoparticles covalently grafted with a thermosensitive radical initiator alkoxyamine, able to provide controlled and localized release of free radicals triggered by an alternating current (ac) magnetic field. These nanoparticles exhibit a high intrinsic loss power of 4.73 nHm
Published: 2023
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8. Hierarchical superparamagnetic metal–organic framework nanovectors as anti-inflammatory nanomedicines

Author: Heng Zhao, Saad Sene, Angelika M. Mielcarek, Sylvain Miraux, Nicolas Menguy, Dris Ihiawakrim, Ovidiu Ersen, Christine Péchoux, Nathalie Guillou, Joseph Scola, Jean-Marc Grenèche, Farid Nouar, Simona Mura, Florent Carn, Florence Gazeau, Eddy Dumas, Christian Serre, Nathalie Steunou, Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-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)-Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre de résonance magnétique des systèmes biologiques (CRMSB), Université de Bordeaux (UB)-Centre National de la Recherche Scientifique (CNRS), Sorbonne Université (SU), 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), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), 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), Université Paris-Saclay, Génétique Animale et Biologie Intégrative (GABI), AgroParisTech-Université Paris-Saclay-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), 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 Galien Paris-Saclay (IGPS), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Matière et Systèmes Complexes (MSC), and Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: Biomedical Engineering, [CHIM]Chemical Sciences, General Materials Science, General Chemistry, General Medicine
Abstract: International audience; Among a plethora of drug nanocarriers, biocompatible nanoscale metal-organic frameworks (nanoMOFs) with a large surface area and an amphiphilic internal microenvironment have emerged as promising drug delivery platforms, mainly for cancer therapy. However, their application in biomedicine still suffers from shortcomings such as a limited chemical and/or colloidal stability and/or toxicity. Here, we report the design of a hierarchically porous nano-object (denoted as USPIO@MIL) combining a benchmark nanoMOF (that is, MIL-100(Fe)) and ultra-small superparamagnetic iron oxide (USPIO) nanoparticles (that is, maghemite) that is synthesized through a one-pot, cost-effective and environmentally friendly protocol. The synergistic coupling of the physico-chemical and functional properties of both nanoparticles confers to these nano-objects valuable features such as high colloidal stability, high biodegradability, low toxicity, high drug loading capacity as well as stimuli-responsive drug release and superparamagnetic properties. This bimodal MIL-100(Fe)/maghemite nanocarrier once loaded with anti-tumoral and anti-inflammatory drugs (doxorubicin and methotrexate) shows high anti-inflammatory and anti-tumoral activities. In addition, the USPIO@MIL nano-object exhibits excellent relaxometric properties and its applicability as an efficient contrast agent for magnetic resonance imaging is herein demonstrated. This highlights the high potential of the maghemite@MOF composite integrating the functions of imaging and therapy as a theranostic anti-inflammatory formulation.
Published: 2023
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9. Composites based on nitroprusside cyano-bridged coordination polymer particles and chitosan for NO delivery

Author: Melvyn Gorra, Frantz Ndebulia Watchou, Maria A. Palacios, Jérôme Long, Saad Sene, Gautier Félix, Nathalie Tanchoux, Françoise Quignard, Joulia Larionova, and Yannick Guari
Subjects: Materials Chemistry, General Chemistry, Catalysis
Abstract: We report the design of new composite films {Fe[Fe(CN)5(NO)]}0.55@C6H11NO4 and {Ag2[Fe(CN)5(NO)]}0.28@ C6H11NO4 based on cyano-bridged coordination polymers FeII[FeII(CN)5(NO)] or Ag2 I[FeII(CN)5(NO)] grown into a chitosan matrix that are able to provide a slow NO radical release under white light irradiation. The characterisation methods such as X-ray diffraction, TGA, SEM-EDX, IR and UV-vis spectroscopies show that these composites are made of ca. 50 wt% of the cyano-bridged coordination polymer as microcrystalline particles embedded into chitosan films. Irradiation for 7 days by using white light results in initiating a 6.5 and 10.6% NO radical delivery for {Fe[Fe(CN)5(NO)]}0.55@C6H11NO4 and {Ag2[Fe(CN)5(NO)]}0.28@C6H11NO4, respectively. The rearrangement of the cyano-bridged coordination compounds after the NO departure leads to the formation of Prussian blue or silver Prussian blue analogues, which limits the unwanted release of cyanide as a side effect., Institut Carnot Chimie Balard Cirimat, SATT AxLR
Published: 2023
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10. New Family of Luminescent Tetranuclear Lanthanide-Based Germsesquioxanes: Luminescence and Temperature Sensing

Author: Gautier Félix, Alena Kulakova, Saad Sene, Clement Charlot, Alexey N. Bilyachenko, Alexander A. Korlyukov, Alexander D. Volodin, Elena S. Shubina, Ilia G. Elizbarian, Yannick Guari, and Joulia Larionova
Subjects: Inorganic Chemistry, Organic Chemistry, Physical and Theoretical Chemistry
Published: 2023
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11. Metal–organic framework/graphene oxide composites for CO2 capture by microwave swing adsorption

Author: Christian Serre, Gilles Patriarche, Nicolas Heymans, Damien Aureau, Alexandros Ploumistos, Mégane Muschi, Rudolf Emmerich, Sabine Devautour-Vinot, Saad Sene, Guy De Weireld, Nathalie Steunou, Amine Geneste, Institut des Matériaux Poreux de Paris (IMAP ), 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)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Service de Thermodynamique et Physique Mathématique - Faculté Polytechnique de Mons, Université de Mons-Hainaut, Fraunhofer Institute for Chemical Technology (Fraunhofer ICT), Fraunhofer (Fraunhofer-Gesellschaft), and Université Paris-Saclay
Subjects: Materials science, Renewable Energy, Sustainability and the Environment, Graphene, Composite number, Oxide, 02 engineering and technology, General Chemistry, Microporous material, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, law.invention, chemistry.chemical_compound, Adsorption, chemistry, law, Desorption, [CHIM]Chemical Sciences, General Materials Science, Metal-organic framework, Composite material, 0210 nano-technology, Microwave
Abstract: Metal–organic frameworks (MOFs)/graphene oxide (GO) composites are of growing interest due to their properties which can exceed those of the pure components, including post-combustion CO2 capture. Series of composites suitable for CO2 capture under flue gas conditions based on the microporous water stable MIL-91(Ti) have been prepared with different GO contents, following two routes, in situ and post-synthetic. It was observed that the 5 wt% GO in situ composite exhibits a semi-conducting behavior, while the post-synthetic materials are insulating, even with high (20 wt%) GO content. As a consequence, this composite absorbs microwave radiation more efficiently compared to the pure MOF and post-synthetic materials. Finally, we report that CO2 desorption is much faster under microwave irradiation compared to direct electric heating on MOF/GO in situ materials, paving the way for future energy-saving microwave swing adsorption processes.
Published: 2021
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12. Temperature sensing in Tb3+/Eu3+-based tetranuclear silsesquioxane cages with tunable emission

Author: Joulia Larionova, Elena S. Shubina, Jérôme Long, Luís D. Carlos, Saad Sene, Gautier Félix, Yannick Guari, Victor N. Khrustalev, Alexey N. Bilyachenko, Karina Nigoghossian, Alena N. Kulakova, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), A. N. Nesmeyanov Institute of Organoelement Compounds (INEOS), Russian Academy of Sciences [Moscow] (RAS), Peoples Friendship University of Russia [RUDN University] (RUDN), Department of Physics and CICECO, and Universidade de Aveiro
Subjects: Materials science, Temperature sensing, General Chemical Engineering, Energy transfer, Analytical chemistry, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, Silsesquioxane, 0104 chemical sciences, chemistry.chemical_compound, chemistry, [CHIM]Chemical Sciences, 0210 nano-technology, Luminescence
Abstract: New luminescent cage-like tetranuclear silsesquioxanes [NEt4][(Ph4Si4O8)2(Tb3Eu)(NO3)4(OH)(EtOH)3(H2O)]·4(EtOH) (1) and [NEt4]2[(Ph4Si4O8)2(Tb2Eu2)(NO3)6(EtOH)2(MeCN)2]·4(MeCN) (2) present a tunable thermosensitive Tb3+-to-Eu3+ energy transfer driven by Tb3+ and Eu3+ emission and may be used as temperature sensors operating in the range 41–100 °C with excellent linearity (R2 = 0.9990) and repeatability (>95%). The thermometer performance was evidenced by the maximum relative sensitivity of 0.63% °C−1 achieved at 68 °C.
Published: 2021
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13. Formation of a Single‐Crystal Aluminum‐Based MOF Nanowire with Graphene Oxide Nanoscrolls as Structure‐Directing Agents

Author: Damien Aureau, Nicolas Menguy, Anusha Lalitha, Saad Sene, Christian Serre, Lucie Rivier, Imène Esteve, Nathalie Steunou, Mathieu Fregnaux, Guillaume Maurin, Naseem A. Ramsahye, Mégane Muschi, Clémence Sicard, Sabine Devautour-Vinot, Institut des Matériaux Poreux de Paris (IMAP ), 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)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-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), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-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)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP UMR8004 FRE2000), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie et de physique des milieux condensés (IMPMC), Université Pierre et Marie Curie - Paris 6 (UPMC)-IPG PARIS-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Muséum national d'Histoire naturelle (MNHN)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de recherche pour le développement [IRD] : UR206-Centre National de la Recherche Scientifique (CNRS), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de recherche pour le développement [IRD] : UR206-Muséum national d'Histoire naturelle (MNHN)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Nanostructure, Oxide, Nanowire, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Catalysis, law.invention, chemistry.chemical_compound, X-ray photoelectron spectroscopy, law, [CHIM]Chemical Sciences, [CHIM.COOR]Chemical Sciences/Coordination chemistry, ComputingMilieux_MISCELLANEOUS, 010405 organic chemistry, Graphene, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, General Medicine, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, Electron diffraction, chemistry, Self-assembly, 0210 nano-technology, Single crystal
Abstract: International audience; Here we propose an innovative strategy to synthesize single-crystal nanowires (NWs) of the Al 3+ dicarboxylate MIL-69(Al) MOF by using graphene oxide nanoscrolls as structure directing agents. MIL-69(Al) NWs with an average diameter of 70 ± 20 nm and lengths up to 2 m were found to preferentially grow along the [001] crystallographic direction. Advanced characterization tools (electron diffraction, TEM, STEM-HAADF, SEM, XPS) and molecular modelling revealed the mechanism of formation of MIL-69(Al) NWs involving size-confinement and templating effects. The formation of MIL-69(Al) seeds and the self-scroll of GO sheets followed by the anisotropic growth of MIL-69(Al) crystals are mediated by specific GO sheets/MOF interactions. This study delivers an unprecedented approach to control the design of 1D MOF nanostructures and superstructures.
Published: 2020
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14. Synergic effect of doxorubicin release and two-photon irradiation of Mn2+-doped Prussian blue nanoparticles on cancer therapy

Author: Saad Sene, Lamiaa M. A. Ali, Fabrice Salles, Maëlle Cahu, Yannick Guari, Joël Chopineau, Jean-Marie Devoisselle, Jérôme Long, Magali Gary-Bobo, Joulia Larionova, Morgane Daurat, Emna Mathlouthi, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Nanomedsyn, Université de Nîmes (UNIMES), Institut des Biomolécules Max Mousseron [Pôle Chimie Balard] (IBMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), and Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)
Subjects: inorganic chemicals, Tunisia, General Chemical Engineering, Nanoparticle, 02 engineering and technology, 010402 general chemistry, Photochemistry, 7. Clean energy, 01 natural sciences, UR/11/ES/19, chemistry.chemical_compound, Two-photon excitation microscopy, medicine, [CHIM]Chemical Sciences, Doxorubicin, Irradiation, ComputingMilieux_MISCELLANEOUS, Prussian blue, Physico-chimie des matériauxà l'état condensé, Doping, Tunis, General Chemistry, Photothermal therapy, 021001 nanoscience & nanotechnology, 3. Good health, 0104 chemical sciences, [SDV.BBM.BP]Life Sciences [q-bio]/Biochemistry, Molecular Biology/Biophysics, des Sciences, chemistry, Cancer cell, 0210 nano-technology, medicine.drug
Abstract: International audience; We demonstrate here that Mn 2+-doped Prussian blue nanoparticles of ca. 55 nm loaded with doxorubicin may be used as efficient therapeutic agents for combined photothermal and chemo-therapy of cancer cells with a synergic effect under two photon irradiation. Photothermal therapy (PTT) is a promising strategy for the therapeutic treatment of tumours, which consists in "burning" cancer cells by laser irradiation at low energy wavelengths in the presence of an NIR photo-adsorbing agent. 1,2 In comparison to conventional cancer treatments, it offers several advantages, such as high specicity, deep penetration, lower tumour recurrence, minimal invasiveness and low toxicity to normal tissues. 3,4 Due to the fact that the treatment efficiency highly depends on the outstanding capacity of the PTT agent to convert light into heat, numerous materials have recently been reported , such as organic dyes 5,6 or various inorganic nano-objects, including metallic nanostructures (Au nanorods or nanoshells, Ag, Pd), carbon based materials (nanotubes, spheres, graphene oxide), transition metal dichalcogenide nanoparticles, metal oxide nano-objects or up-conversion nanocrystals. 7-16 Among these, Prussian blue (PB) nano-objects have been developed as interesting PTT agents since they benet from many advantages, such as: (i) a controlled size ranging from a few to hundreds of nanometers, (ii) easy surface functionali-zation, (iii) excellent absorption properties in the NIR spectral domain due to an Fe 2+ to Fe 3+ intervalence charge transfer band ranging from 650 to 900 nm, (iv) high stability under irradiation , and (v) the fact that bulk PB is validated by the FDA under the brand name Radiogardase® as an antidote for human beings exposed to radioactive Cs +. 17 It has been shown in vitro that PB nanoparticles upon single photon excitation (SPE) (at 808 nm) can convert the laser irradiation into thermal energy contributing to an important temperature increase. 18,19 Their efficiency depends on the nanoparticles' concentration, their chemical composition, the laser power, the mode of irradiation and the irradiation time. Moreover, it has been demonstrated that nano-sized PB presents a higher efficiency in comparison with Au nanorods and a better photothermal stability than organic dyes used as conventional photothermal agents. 19,20 PTT effect of PB nanoparticles has also been demonstrated in vivo through their intra-tumoral injection that causes signicant tumour necrosis 24 h aer NIR irradiation in comparison with non-treated mice. 18 Nevertheless, the complete eradication of cancer cells using solely PTT treatment is rather difficult due to the suboptimal laser energy in deep tissues related to light scattering and absorption effects, a limited light penetration and the insufficient tumour target specicity of PTT agents. Some of these drawbacks may be circumvented using two photon excitation (TPE), which permits to increase the penetration depth and laser focalization allowing selective and efficient destruction of the targeted cancer cells with less damage to healthy tissues. 21-23 In this line of thought, we reported recently Mn 2+-doped PB nanoparticles of ca. 70 nm as efficient multifunctional PTT agents permitting to eradicate 97% of cancer cells 24 h aer irradiation under TPE during 10 min, which may also be followed by Magnetic Resonance Imaging (MRI). 24 However, the comparison between the efficiency of the single and two-photon excitations on the same nano-objects has never been investigated.
Published: 2020
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15. A rational study of the influence of Mn

Author: Maëlle, Cahu, Lamiaa M A, Ali, Saad, Sene, Jérôme, Long, Franck, Camerel, Mathieu, Ciancone, Fabrice, Salles, Joël, Chopineau, Jean-Marie, Devoisselle, Gautier, Felix, Nicolas, Cubedo, Mireille, Rossel, Yannick, Guari, Nadir, Bettache, Joulia, Larionova, and Magali, Gary-Bobo
Subjects: Manganese, Photothermal Therapy, Cell Line, Tumor, Iron, Animals, Humans, Nanoparticles, Antineoplastic Agents, Triple Negative Breast Neoplasms, Photochemical Processes, Xenograft Model Antitumor Assays, Zebrafish, Ferrocyanides
Abstract: We investigated a series of Mn
Published: 2021

16. A rational study of the influence of Mn(2+)-insertion in Prussian blue nanoparticles on their photothermal properties

Author: Joulia Larionova, Lamiaa M. A. Ali, Jérôme Long, Mireille Rossel, Fabrice Salles, Saad Sene, Nicolas Cubedo, Maëlle Cahu, Joël Chopineau, Gautier Félix, Magali Gary-Bobo, Mathieu Ciancone, Franck Camerel, Yannick Guari, Jean-Marie Devoisselle, Nadir Bettache, Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut des Biomolécules Max Mousseron [Pôle Chimie Balard] (IBMM), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Mécanismes moléculaires dans les démences neurodégénératives (MMDN), École Pratique des Hautes Études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Montpellier (UM), The authors thank the University of Montpellier and CNRS for financial support, platform MEA of the University of Montpellier and PAC of ICGM for measurements. This work has been supported by ANR with grant number ANR-18-CE09-0012-01. We acknowledge the imaging facility MRI, member of the national infrastructure France-BioImaging supported by the French National Research Agency (ANR-10-INBS-04, «Investments for the future»). F. C. and J. L. thanks Loïc Charbonnière for his helpful discussions on measurements made in D2O., ANR-18-CE09-0012,NANOBLUE,Nanoparticules de bleu de Prusse pour le théranostic(2018), ANR-10-INBS-0004,France-BioImaging,Développment d'une infrastructure française distribuée coordonnée(2010), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Montpellier (UM)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut National de la Santé et de la Recherche Médicale (INSERM)-École pratique des hautes études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL), École pratique des hautes études (EPHE), Jonchère, Laurent, APPEL À PROJETS GÉNÉRIQUE 2018 - Nanoparticules de bleu de Prusse pour le théranostic - - NANOBLUE2018 - ANR-18-CE09-0012 - AAPG2018 - VALID, and Développment d'une infrastructure française distribuée coordonnée - - France-BioImaging2010 - ANR-10-INBS-0004 - INBS - VALID
Subjects: inorganic chemicals, Prussian blue, Materials science, Morphology (linguistics), Biomedical Engineering, Pulsed laser irradiation, Nanoparticle, One-Step, 02 engineering and technology, General Chemistry, General Medicine, Photothermal therapy, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, chemistry.chemical_compound, Adsorption, chemistry, [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, General Materials Science, 0210 nano-technology, Triple negative, Nuclear chemistry
Abstract: International audience; We investigated a series of Mn(2+)-Prussian blue (PB) nanoparticles Na(z)Mn(x)Fe(1-x)[Fe(CN)(6)](1-y□y)·nH(2)O of similar size, surface state and cubic morphology with various amounts of Mn(2+) synthesized through a one step self-assembly reaction. We demonstrated by a combined experimental-theoretical approach that during the synthesis, Mn(2+) substituted Fe(3+) up to a Mn/Na-Mn-Fe ratio of 32 at% in the PB structure, while for higher amounts, the Mn(2)[Fe(CN)(6)] analogue is obtained. For comparison, the post-synthetic insertion of Mn2+ in PB nanoparticles was also investigated and completed with Monte-Carlo simulations to probe the plausible adsorption sites. The photothermal conversion efficiency (η) of selected samples was determined and showed a clear dependence on the Mn(2+)amount with a maximum efficiency for a Mn/Na-Mn-Fe ratio of 10 at% associated with a dependence on the nanoparticle concentration. Evaluation of the in vitro photothermal properties of these nanoparticles performed on triple negative human breast adenocarcinoma (MDA-MB-231) cells by using continuous and pulsed laser irradiation confirm their excellent PTT efficiency permitting low dose use.
Published: 2021
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17. Temperature sensing in Tb

Author: Karina, Nigoghossian, Alena N, Kulakova, Gautier, Félix, Victor N, Khrustalev, Elena S, Shubina, Jérôme, Long, Yannick, Guari, Saad, Sene, Luís D, Carlos, Alexey N, Bilyachenko, and Joulia, Larionova
Abstract: New luminescent cage-like tetranuclear silsesquioxanes [NEt
Published: 2021

18. Long-term

Author: Hussein, Awada, Saad, Sene, Danielle, Laurencin, Laurent, Lemaire, Florence, Franconi, Florence, Bernex, Audrey, Bethry, Xavier, Garric, Yannick, Guari, and Benjamin, Nottelet
Subjects: Polyesters, Animals, Magnetic Iron Oxide Nanoparticles, Magnetite Nanoparticles, Magnetic Resonance Imaging, Nanocomposites, Rats
Abstract: There is a growing interest in magnetic nanocomposites in biomaterials science. In particular, nanocomposites that combine poly(lactide) (PLA) nanofibers and superparamagnetic iron oxide nanoparticles (SPIONs), which can be obtained by either electrospinning of a SPION suspension in PLA or by precipitating SPIONs at the surface of PLA, are well documented in the literature. However, these two classical processes yield nanocomposites with altered materials properties, and their long-term
Published: 2021

19. Long-term in vivo performances of polylactide/iron oxide nanoparticles core–shell fibrous nanocomposites as MRI-visible magneto-scaffolds

Author: Florence Bernex, Saad Sene, Danielle Laurencin, Yannick Guari, Laurent Lemaire, Hussein Awada, Benjamin Nottelet, Florence Franconi, Xavier Garric, Audrey Bethry, Institut des Biomolécules Max Mousseron [Pôle Chimie Balard] (IBMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Micro et Nanomédecines Translationnelles (MINT), Université d'Angers (UA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Plate-forme de Recherche en Imagerie et Spectroscopie Multi-modales (PRISM [SFR ICAT - UA]), SFR UA 4208 Interactions Cellulaires et Applications Thérapeutiques (ICAT), Université d'Angers (UA)-Université d'Angers (UA), Institut de Recherche en Cancérologie de Montpellier (IRCM - U1194 Inserm - UM), and CRLCC Val d'Aurelle - Paul Lamarque-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Montpellier (UM)
Subjects: Materials science, Biocompatibility, Biomedical Engineering, Nanotechnology, 02 engineering and technology, hybrid biomaterial, histology, 03 medical and health sciences, chemistry.chemical_compound, In vivo, General Materials Science, implantation, poly(lactide) nanofibers, [SDV.IB.BIO]Life Sciences [q-bio]/Bioengineering/Biomaterials, Magneto, 030304 developmental biology, 0303 health sciences, Lactide, Nanocomposite, iron oxide nanoparticles, 021001 nanoscience & nanotechnology, equipment and supplies, Electrospinning, in vivo, medical resonance imaging (MRI), [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Nanofiber, 0210 nano-technology, Iron oxide nanoparticles
Abstract: International audience; There is a growing interest in magnetic nanocomposites in biomaterials science. In particular, nanocomposites that combine poly(lactide) (PLA) nanofibers and superparamagnetic iron oxide nanoparticles (SPIONs), which can be obtained by either electrospinning of a SPION suspension in PLA or by precipitating SPIONs at the surface of PLA, are well documented in the literature. However, these two classical processes yield nanocomposites with altered materials properties, and their long-term in vivo fate and performances have in most cases only been evaluated over short periods of time. Recently, we reported a new strategy to prepare well-defined PLA@SPION nanofibers with a quasi-monolayer of SPIONs anchored at the surface of PLA electrospun fibers. Herein, we report on a 6-month in vivo rat implantation study with the aim of evaluating the long-term magnetic resonance imaging (MRI) properties of this new class of magnetic nanocomposites, as well as their tissue integration and degradation. Using clinically relevant T2-weighted MRI conditions, we show that the PLA@SPION nanocomposites are clearly visible up to 6 months. We also evaluate here by histological analyses the slow degradation of the PLA@SPIONs, as well as their biocompatibility. Overall, these results make these nanocomposites attractive for the development of magnetic biomaterials for biomedical applications.
Published: 2021
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20. Nanoheterostructures based on nanosized Prussian blue and its Analogues: Design, properties and applications

Author: Yannick Guari, Maëlle Cahu, Gautier Félix, Saad Sene, Jérôme Long, Joël Chopineau, Jean-Marie Devoisselle, and Joulia Larionova
Subjects: Inorganic Chemistry, Materials Chemistry, Physical and Theoretical Chemistry
Published: 2022
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21. Grafted mesoporous silicas for radionuclide uptake: Radiolytic stability under electron irradiation

Author: Guillaume Zante, Vincent Bouniol, Saad Sene, Cyrielle Rey, Jérémy Causse, Joulia Larionova, Yannick Guari, Xavier Deschanels, Sophie Le Caër, 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), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), Institut de Chimie Séparative de Marcoule (ICSM - UMR 5257), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), and ANR-18-CE05-0016,AUTOMACT,SEPARATION SUR SOLIDE ET AUTOCONDITIONNEMENT D'ACTINIDES PROVENANT D'EFFLUENTS CONTAMINES(2018)
Subjects: reaction mechanisms, Mechanics of Materials, electron irradiation, nuclear waste management, actinide adsorption, grafted mesoporous silica, General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, functionalized SBA-15, Condensed Matter Physics
Abstract: International audience; Materials developed for radionuclide adsorption need to resist harsh conditions, i.e. be robust against ionizing radiation. In this work, we evaluated the degradation of mesoporous silicas (SBA-15) grafted with hydroxypiridinone, acetamide phosphonate and propionamide phosphonate ligands under electron irradiation. The ligands contained amide and phosphinic acid functional groups, which made them able to bind to actinides. Degradation of the grafted ligand was assessed by identifying and quantifying the gas produced under irradiation using gas chromatography, as well as characterizing the grafted ligands before and after irradiation by means of FT-IR, XPS and TGA techniques. Irradiation led to the degradation of amide functional groups and to the production of amine and carboxylic acid groups. Corresponding reaction mechanisms are proposed. The sorption behavior of the grafted SBA-15 materials for thorium was also studied. SBA-15 materials grafted with acetamide phosphonate and propionamide phosphonate ligands were shown to be able to adsorb thorium. The propionamide phosphate ligand was the most efficient, with an equilibrium sorption capacity of 95 mg g$^{−1}$. This capacity remains stable up to a 1 MGy irradiation dose and undergoes a 20% decrease after 4 MGy of irradiation. Therefore, this material is potentially interesting for the treatment of liquid outflows contaminated by actinides produced in nuclear facilities.
Published: 2022
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22. Unveiling the Structure and Reactivity of Fatty-Acid Based (Nano)materials Thanks to Efficient and Scalable 17O and 18O-Isotopic Labeling Schemes

Author: Kuizhi Chen, Dorothée Berthomieu, Thomas-Xavier Métro, Zhehong Gan, Danielle Laurencin, Guillaume Cazals, Saad Sene, Sébastien Mittelette, Chia-Hsin Chen, Jessica Špačková, Aurélien Lebrun, Christel Gervais, Emeline Gaillard, Charlyn Fabra, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut des Biomolécules Max Mousseron [Pôle Chimie Balard] (IBMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), National High Magnetic Field Laboratory (NHMFL), Florida State University [Tallahassee] (FSU), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), 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), National Science Foundation Cooperative Agreement No. DMR-1644779, HPC resources from GENCI-IDRIS (Grant 097535), National Science Foundation (DMR-1039938 and DMR-0603042), National Institute of Health P41 GM122698, European Project: 772204,MISOTOP, and Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM)
Subjects: Magnetic Resonance Spectroscopy, Infrared spectroscopy, Context (language use), 02 engineering and technology, Oxygen Isotopes, 010402 general chemistry, 01 natural sciences, Biochemistry, Article, Catalysis, Isotopic labeling, chemistry.chemical_compound, Colloid and Surface Chemistry, Molecule, Reactivity (chemistry), chemistry.chemical_classification, Fatty acid, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Combinatorial chemistry, Nanostructures, 0104 chemical sciences, Oleic acid, Solid-state nuclear magnetic resonance, chemistry, Isotope Labeling, 0210 nano-technology, Stearic Acids, Oleic Acid
Abstract: International audience; Fatty acids are ubiquitous in biological systems and widely used in materials science, including for the formulation of drugs and the surface-functionalization of nanoparticles. However, important questions regarding the structure and reactivity of these molecules are still to be elucidated, including their mode of binding to certain metal cations or materials surfaces. In this context, we have developed novel, efficient, user-friendly, and cost-effective synthetic protocols based on ball-milling, for the 17O and 18O isotopic labeling of two key fatty acids which are widely used in (nano)materials science, namely stearic and oleic acid. Labeled molecules were analyzed by 1H and 13C solution NMR, IR spectroscopy, and mass spectrometry (ESI-TOF and LC-MS), as well as 17O solid state NMR (for the 17O labeled species). In both cases, the labeling procedures were scaled-up to produce up to gram quantities of 17O- or 18O-enriched molecules in just half-a-day, with very good synthetic yields (all ≥84%) and enrichment levels (up to an average of 46% per carboxylic oxygen). The 17O-labeled oleic acid was then used for the synthesis of a metal soap (Zn-oleate) and the surface-functionalization of ZnO nanoparticles (NPs), which were characterized for the first time by high-resolution 17O NMR (at 14.1 and 35.2 T). This allowed very detailed insight into (i) the coordination mode of the oleate ligand in Zn-oleate to be achieved (including information on Zn···O distances) and (ii) the mode of attachment of oleic-acid at the surface of ZnO (including novel information on its photoreactivity upon UV-irradiation). Overall, this work demonstrates the high interest of these fatty acid-enrichment protocols for understanding the structure and reactivity of a variety of functional (nano)materials systems using high resolution analyses like 17O NMR.
Published: 2020
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23. New insights into the degradation mechanism of metal-organic frameworks drug carriers

Author: Junxun M Zhang, Christian Serre, Saad Sene, S. Safi, Xiaojian Li, Jean-Marc Greneche, Ruxandra Gref, L. Lachmanski, Calcul Naturel (CANA), Laboratoire d'Informatique et Systèmes (LIS), Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de mécanique des sols, structures et matériaux (MSSMat), CentraleSupélec-Centre National de la Recherche Scientifique (CNRS), Physico-chimie, pharmacotechnie, biopharmacie (PCPB), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), and Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Surface Properties, Simulated body fluid, lcsh:Medicine, 02 engineering and technology, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, 010402 general chemistry, Spectrum Analysis, Raman, 01 natural sciences, Article, chemistry.chemical_compound, [CHIM]Chemical Sciences, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Carboxylate, lcsh:Science, Metal-Organic Frameworks, ComputingMilieux_MISCELLANEOUS, Mossbauer spectrometry, Drug Carriers, Multidisciplinary, lcsh:R, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Amorphous solid, chemistry, Chemical engineering, Particle, Surface modification, Metal-organic framework, lcsh:Q, 0210 nano-technology, Drug carrier
Abstract: A versatile method based on Raman microscopy was developed to follow the degradation of iron carboxylate Metal Organic Framework (MOF) nano- or micro-particles in simulated body fluid (phosphate buffer). The analysis of both the morphology and chemical composition of individual particles, including observation at different regions on the same particle, evidenced the formation of a sharp erosion front during particle degradation. Interestingly, this front separated an intact non eroded crystalline core from an amorphous shell made of an inorganic network. According to Mössbauer spectrometry investigations, the shell consists essentially of iron phosphates. Noteworthy, neither drug loading nor surface modification affected the integrity of the tridimensional MOF network. These findings could be of interest in the further development of next generations of MOF drug carriers.
Published: 2017
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24. Maghemite-nanoMIL-100(Fe) Bimodal Nanovector as a Platform for Image-Guided Therapy

Author: Patricia Horcajada, Jeanne Volatron, Clotilde Menet, Florence Gazeau, Christian Serre, Nathalie Guillou, Saad Sene, M. Teresa Marcos-Almaraz, Jean-Marc Greneche, Joseph Scola, Nicolas Menguy, Sylvain Miraux, Richard Rouland, Nathalie Steunou, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de recherche pour le développement [IRD] : UR206-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Matière et Systèmes Complexes (MSC (UMR_7057)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), 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), Centre de résonance magnétique des systèmes biologiques (CRMSB), Centre National de la Recherche Scientifique (CNRS)-Université de Bordeaux (UB), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de réactivité, électrochimie et microporosite (IREM), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut de recherche pour le développement [IRD] : UR206-Centre National de la Recherche Scientifique (CNRS)-Muséum national d'Histoire naturelle (MNHN)-Université Pierre et Marie Curie - Paris 6 (UPMC), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Le Mans Université (UM), Résonance magnétique des systèmes biologiques (RMSB), and Université Bordeaux Segalen - Bordeaux 2-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, General Chemical Engineering, MRI contrast agent, Nanoparticle, Maghemite, Nanotechnology, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, 02 engineering and technology, engineering.material, 010402 general chemistry, 01 natural sciences, Biochemistry, Colloid, Materials Chemistry, [CHIM]Chemical Sciences, Environmental Chemistry, ComputingMilieux_MISCELLANEOUS, Mossbauer spectrometry, Low toxicity, Biochemistry (medical), [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, engineering, 0210 nano-technology, Mesoporous material, Superparamagnetism
Abstract: Summary We report here the design of nano-objects (i.e., denoted as MIL/USPIO-cit) that consist of nanoparticles of mesoporous iron trimesate metal-organic framework MIL-100(Fe), whose surface is decorated by maghemite nanoparticles. Not only is this bimodal nanovector produced through a cost-effective and reliable green approach, but it also exhibits excellent colloidal stability under simulated intravenous conditions, and its ability to encapsulate and progressively release drugs (doxorubicin here) is preserved. According to vibrating sample magnetometry and 57 Fe Mossbauer spectrometry, MIL-USPIO-cit presents a superparamagnetic behavior characterized by a high saturation magnetization at room temperature. More importantly, it combines low toxicity with high anti-tumoral activity and can be used in vivo as an efficient MRI contrast agent because of its excellent relaxivity properties. All these properties make this nano-object a potential candidate as a bimodal therapeutic nanovector coupling drug-delivery and MRI properties.
Published: 2017
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25. Synergic effect of doxorubicin release and two-photon irradiation of Mn

Author: Lamiaa M A, Ali, Emna, Mathlouthi, Maëlle, Cahu, Saad, Sene, Morgane, Daurat, Jérôme, Long, Yannick, Guari, Fabrice, Salles, Joël, Chopineau, Jean-Marie, Devoisselle, Joulia, Larionova, and Magali, Gary-Bobo
Abstract: We demonstrate here that Mn
Published: 2019

26. Cellular Uptake, Intracellular Trafficking, and Stability of Biocompatible Metal-Organic Framework (MOF) Particles in Kupffer Cells

Author: Christian Kroll, Saad Sene, Mikhail Durymanov, Anastasia Permyakova, Mónica Giménez-Marqués, Christian Serre, Joshua Reineke, Ailin Guo, Department of Pharmaceutical Sciences, College of Pharmacy and Allied Health ProfessionsSouth Dakota State UniversityBrookingsUSA, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Instituto de Ciencia Molecular (ICMol), and Universitat de València (UV)
Subjects: Kupffer Cells, Phagosome acidification, media_common.quotation_subject, Kinetics, Endocytic cycle, Pharmaceutical Science, 02 engineering and technology, 030226 pharmacology & pharmacy, 03 medical and health sciences, 0302 clinical medicine, Drug Discovery, [SDV.BC.IC]Life Sciences [q-bio]/Cellular Biology/Cell Behavior [q-bio.CB], medicine, Humans, Internalization, Metal-Organic Frameworks, ComputingMilieux_MISCELLANEOUS, media_common, Microscopy, Chemistry, fungi, Kupffer cell, [CHIM.MATE]Chemical Sciences/Material chemistry, Flow Cytometry, 021001 nanoscience & nanotechnology, medicine.anatomical_structure, Drug delivery, Biophysics, Molecular Medicine, Nanocarriers, 0210 nano-technology, Intracellular
Abstract: Rapid intracellular degradation of current drug-delivery nanocarriers presents a challenge for achieving ideal controlled drug-release kinetics. Recent in vivo studies have shown that porous hybrid metal-organic frameworks (MOFs), belonging to the Materials of Institute Lavoisier (MIL) family, display prolonged biodegradation behavior. In this study, we investigated stability of these materials in Kupffer cells, a relevant target for the treatment of several life-threatening immune-mediated liver diseases. For this aim, we selected fluorescently labeled microporous MOF particles of MIL88A and MIL88B-NH2, built from trimers of Fe(III) octahedra, as an inorganic component, and fumarate (MIL88A) or 2-amino terephthalate (MIL88B-NH2), as an organic linker. Cell uptake inhibition analysis of MOF particles by a Kupffer cell line (KUP5) has shown that phagocytosis is the major endocytic pathway involved in MIL88B-NH2 internalization. Investigation of MOF interaction with KUP5 cells by real-time microscopy indicated that the structure of MIL88B-NH2 MOFs stays intact up to 15 min after uptake, followed by MOF accumulation in acidic cell compartments and slow degradation, reaching a minimum of 10-15% decomposition over 24 h. MIL88A particles demonstrated similar degradation kinetics. Analysis of the mechanisms of MOF degradation has shown that inhibition of phagosome acidification as well as protease activity does not prevent decomposition of MIL88B-NH2 particles. Thus, our study demonstrates the relative stability of the MOF structure in the phagolysosomal environment of Kupffer cells, revealing potential use of these materials for controlled drug delivery in a case of immune-mediated liver diseases.
Published: 2019
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27. Metal Organic Framework (MOF) Particles as Potential Bacteria-Mimicking Delivery Systems for Infectious Diseases: Characterization and Cellular Internalization in Alveolar Macrophages

Author: Mikhail Durymanov, Christian Serre, Ailin Guo, Saad Sene, Joshua Reineke, Anastasia Permyakova, Department of Pharmaceutical Sciences, College of Pharmacy and Allied Health ProfessionsSouth Dakota State UniversityBrookingsUSA, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut des Matériaux Poreux de Paris (IMAP ), 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)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), and Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDV]Life Sciences [q-bio], Sus scrofa, Endocytic cycle, Pharmaceutical Science, Nanoparticle, 02 engineering and technology, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, 030226 pharmacology & pharmacy, 0302 clinical medicine, Anti-Infective Agents, Biomimetics, Macrophage, Pharmacology (medical), Internalization, Metal-Organic Frameworks, ComputingMilieux_MISCELLANEOUS, media_common, Drug Carriers, Chemistry, Pinocytosis, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Endocytosis, 3. Good health, Mannosylation, Molecular Medicine, 0210 nano-technology, Biotechnology, Surface Properties, media_common.quotation_subject, [SDV.BC]Life Sciences [q-bio]/Cellular Biology, Communicable Diseases, Cell Line, 03 medical and health sciences, Phagocytosis, Macrophages, Alveolar, Animals, [CHIM]Chemical Sciences, Pharmacology, Bacteria, Molecular Mimicry, fungi, Organic Chemistry, Hexosamines, Kinetics, Surface coating, Targeted drug delivery, Biophysics, Nanoparticles, Mannose
Abstract: Intramacrophagic bacteria pose a great challenge for the treatment of infectious diseases despite many macrophage targeted drug delivery approaches explored. The use of biomimetic approaches for treating infectious diseases is promising, but not studied extensively. The study purpose is to evaluate iron-based metal-organic frameworks (MOF) as a potential bacteria-mimicking delivery system for infectious diseases. Two types of carboxylated MOFs, MIL-88A(Fe) and MIL-100(Fe) were developed as “pathogen-like” particles by surface coating with mannose. MOF morphology, cellular uptake kinetics, and endocytic mechanisms in 3D4/21 alveolar macrophages were characterized. MIL-88A(Fe) is rod-shape (aspect ratio 1:5) with a long-axis size of 3628 ± 573 nm and MIL-100(Fe) is spherical with diameter of 103.9 ± 7.2 nm. Cellular uptake kinetics of MOFs showed that MIL-100(Fe) nanoparticles were internalized at a faster rate and higher extent compared to MIL-88A(Fe) microparticles. Mannosylation did not improve the uptake of MIL-100(Fe) particles, whereas it highly increased MIL-88A(Fe) cellular uptake and number of cells involved in internalization. Cell uptake inhibition studies indicated that macropinocytosis/phagocytosis was the main endocytic pathway for internalization of MOFs. Accumulation of MOF particles in acidic compartments was clearly observed. The successfully synthesized “pathogen-like” particles provide a novel application of MOF-based particles as biomimetic delivery system for intramacrophagic-based infections.
Published: 2019
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28. Design of Laccase–Metal Organic Framework-Based Bioelectrodes for Biocatalytic Oxygen Reduction Reaction

Author: Christian Serre, Saad Sene, Christine Mousty, Ludovic Legrand, Annie Chaussé, Snehangshu Patra, Nathalie Steunou, Laboratoire Analyse et Modélisation pour la Biologie et l'Environnement (LAMBE - UMR 8587), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Cergy Pontoise (UCP), Université Paris-Seine-Université Paris-Seine-Université d'Évry-Val-d'Essonne (UEVE)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Clermont-Ferrand (ICCF), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Sigma CLERMONT (Sigma CLERMONT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Analyse et Modélisation pour la Biologie et l'Environnement (LAMBE), Université Paris-Seine-Université Paris-Seine-Université d'Évry-Val-d'Essonne (UEVE)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Université Paris-Seine-Université Paris-Seine-Université d'Évry-Val-d'Essonne (UEVE)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Laccase, oxygen reduction reaction, ABTS, bioelectrocatalysis, Chemistry, MIL-100(Fe), Inorganic chemistry, 02 engineering and technology, Porosimetry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, MOFs, 0104 chemical sciences, laccase, chemistry.chemical_compound, Electrode, Molecule, Ionic conductivity, [CHIM]Chemical Sciences, General Materials Science, Metal-organic framework, 0210 nano-technology, Mesoporous material
Abstract: International audience; Laccase in combination with 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) as a mediator is a well-known bioelectrocatalyst for the 4-electron oxygen reduction reactions (ORR). The present work deals with the first exploitation of mesoporous iron(III) trimesate-based metal organic frameworks (MOF) MIL-100(Fe) (MIL stands for materials from Institut Lavoisier) as a new and efficient immobilization matrix of laccase for the building up of biocathodes for ORR. First, the immobilization of ABTS in the pores of the MOF was studied by combining micro-Raman spectroscopy, X-ray powder diffraction (XRPD), and N2 porosimetry. The ABTS-MIL-100(Fe)-based modified electrode presents excellent properties in terms of charge transfer kinetics and ionic conductivity as well as a very stable and reproducible electrochemical response, showing that MIL-100(Fe) provides a suitable and stabilizing microenvironment for electroactive ABTS molecules. In a second step, laccase was further immobilized on the MIL-100(Fe)-ABTS matrix. The Lac-ABTS-MIL-100(Fe)-CIE bioelectrode presents a high electrocatalytic current density of oxygen reduction and a reproducible electrochemical response characterized by a high stability over a long period of time (3 weeks). These results constitute a significant advance in the field of laccase-based bioelectrocatalysts for ORR. According to our work, it appears that the high catalytic efficiency of Lac-ABTS-MIL-100(Fe) for ORR may result from a synergy of chemical and catalytic properties of MIL-100(Fe) and laccase.
Published: 2016
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29. Adsorption of benzoxaboroles on hydroxyapatite phases

Author: Danielle Laurencin, Ondrej Nikel, Deepak Vashishth, Marie Alix Pizzoccaro, Coralie Philippe, P. Hubert Mutin, Sylvie Bégu, Saad Sene, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), department of Biomedical Engineering (RPI - BME), Rensselaer Polytechnic Institute (RPI), ANR, ERG, ANR-13-JS08-0004,BOROMAT,Développement d'une nouvelle classe de matériaux hybrides organique-inorganique incorporant des boronates/ benzoxaborolates(2013), European Project: 239206,EC:FP7:PEOPLE,FP7-PEOPLE-ERG-2008,CONTRELL(2009), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), and Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Magnetic Resonance Spectroscopy, Materials science, Kinetics, Biomedical Engineering, benzoxaborole, Mineralogy, Ionic bonding, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biochemistry, Article, Apatite, Biomaterials, Adsorption, X-Ray Diffraction, Molecule, Hydroxyapatites, Molecular Biology, hydroxyapatite, General Medicine, Nuclear magnetic resonance spectroscopy, [CHIM.MATE]Chemical Sciences/Material chemistry, Bridged Bicyclo Compounds, Heterocyclic, 021001 nanoscience & nanotechnology, Combinatorial chemistry, 0104 chemical sciences, Durapatite, adsorption, visual_art, visual_art.visual_art_medium, Surface modification, 0210 nano-technology, Biotechnology
Abstract: Benzoxaboroles are a family of molecules that are finding an increasing number of applications in the biomedical field, particularly as a “privileged scaffold” for the design of new drugs. Here, for the first time, we determine the interaction of these molecules with hydroxyapatites, in view of establishing (i) how benzoxaborole drugs may adsorb onto biological apatites, as this could impact on their bioavailability, and (ii) how apatite-based materials can be used for their formulation. Studies on the adsorption of the benzoxaborole motif (C 7 H 7 BO 2 , referred to as BBzx) on two different apatite phases were thus performed, using a ceramic hydroxyapatite (HA ceram ) and a nanocrystalline hydroxyapatite (HA nano ), the latter having a structure and composition more similar to the one found in bone mineral. In both cases, the grafting kinetics and mechanism were studied, and demonstration of the surface attachment of the benzoxaborole under the form of a tetrahedral benzoxaborolate anion was established using 11 B solid state NMR (including 11 B- 31 P correlation experiments). Irrespective of the apatite used, the grafting density of the benzoxaborolates was found to be low, and more generally, these anions demonstrated a poor affinity for apatite surfaces, notably in comparison with other anions commonly found in biological media, such as carboxylates and (organo)phosphates. The study was then extended to the adsorption of a molecule with antimicrobial and antifungal properties (3-piperazine-bis(benzoxaborole)), showing, on a more general perspective, how hydroxyapatites can be used for the development of novel formulations of benzoxaborole drugs. Statement of Significance Benzoxaboroles are an emerging family of molecules which have attracted much attention in the biomedical field, notably for the design of new drugs. However, the way in which these molecules, once introduced in the body, may interact with bone mineral is still unknown, and the possibility of associating benzoxaboroles to calcium phosphates for drug-formulation purposes has not been looked into. Here, we describe the first study of the adsorption of benzoxaboroles on hydroxyapatite, which is the main mineral phase present in bone. We describe the mode of grafting of benzoxaboroles on this material, and show that they only weakly bind to its surface, especially in comparison to other ionic species commonly found in physiological media, such as phosphates and carboxylates. This demonstrates that administered benzoxaborole drugs are unlikely to remain adsorbed on hydroxyapatite surfaces for long periods of time, which means that their biodistribution will not be affected by such phenomena. Moreover, this work shows that the formulation of benzoxaborole drugs by association to calcium phosphates like hydroxyapatite will lead to a rapid release of the molecules.
Published: 2016
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30. Formulation of benzoxaborole drugs in PLLA: from materials preparation to in vitro releasekinetics and cellular assays

Author: Sylvie Bégu, Nicholas J. Schaub, Danielle Laurencin, Joshua S. McLane, Saad Sene, Lee A. Ligon, Ryan J. Gilbert, P. Hubert Mutin, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Rensselaer Polytechnic Institute (RPI), ANR, Partner University Fund, and ANR-13-JS08-0004,BOROMAT,Développement d'une nouvelle classe de matériaux hybrides organique-inorganique incorporant des boronates/ benzoxaborolates(2013)
Subjects: Materials science, Kinetics, Biomedical Engineering, Antifungal drug, benzoxaborole, Context (language use), Nanotechnology, formulation, 02 engineering and technology, engineering.material, 010402 general chemistry, 01 natural sciences, chemistry.chemical_compound, Molecule, General Materials Science, Materials preparation, General Chemistry, General Medicine, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Combinatorial chemistry, In vitro, 0104 chemical sciences, 3. Good health, chemistry, engineering, Hydroxide, Biopolymer, 0210 nano-technology, biomaterials
Abstract: International audience; Benzoxaboroles are a family of organoboron molecules, which have been finding over the past few years an increasing number of biological applications, notably for the design of new drugs. Given that these molecules are still relatively new in the biomedical context, very few investigations regarding their formulation have been reported to date. Here, a complete study on the formulation of benzoxaboroles in a biopolymer, poly-L-lactic acid (PLLA), is reported. The incorporation of two small benzoxaboroles, namely the simplest benzoxaborole molecule (BBzx) and the antifungal drug tavaborole (AN2690), inside PLLA films was investigated. Different variations in the film composition and texture were looked into, by performing a heat-treatment on the PLLA films, or by preparing PLLA–PEO (polyethylene oxide) blends or PLLA–LDH (layered double hydroxide) composites. In each case, the impact of these changes in formulation on the local environment of the benzoxaboroles in the material (as determined by multinuclear solid state NMR), and on the kinetics of release in physiological media were analyzed, showing that a variety of release profiles could be achieved. Finally, cellular assays were carried out looking at the migration of MDA-MB-231 cancer cells. These tests revealed for the first time that benzoxaboroles like AN2690 and BBzx inhibited the migration of these cells. Moreover, the molecules incorporated in the films were found to remain active, and their effect on cancer cells was directly related to the release kinetics from the films. All in all, PLLA-based materials appear as highly versatile and attractive matrices for formulating benzoxaborole-based drugs.
Published: 2016
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31. Intercalation of benzoxaborolate anions in layered double hydroxides: toward hybrid formulations for benzoxaborole drugs

Author: Saad Sene, Arie van der Lee, Christian Bonhomme, Guillaume Renaudin, Danielle Laurencin, Adel Mesbah, Sylvie Bégu, P. Hubert Mutin, Mark E. Smith, Christel Gervais, Jean-Marie Nedelec, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Clermont-Ferrand (ICCF), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Séparative de Marcoule (ICSM - UMR 5257), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Lancaster University, University of Warwick [Coventry], Institut Européen des membranes (IEM), ANRMarie Curie ERG, ANR-13-JS08-0004,BOROMAT,Développement d'une nouvelle classe de matériaux hybrides organique-inorganique incorporant des boronates/ benzoxaborolates(2013), European Project: 239206,EC:FP7:PEOPLE,FP7-PEOPLE-ERG-2008,CONTRELL(2009), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Sigma CLERMONT (Sigma CLERMONT), Interfaces de Matériaux en Evolution (LIME), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM), Solid State NMR Group, University of Warwick, Université de Montpellier (UM)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Ecole Nationale Supérieure de Chimie de Paris- Chimie ParisTech-PSL (ENSCP)-Centre National de la Recherche Scientifique (CNRS), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut de Chimie du CNRS (INC)-SIGMA Clermont (SIGMA Clermont)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Centre National de la Recherche Scientifique (CNRS), and Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)
Subjects: General Chemical Engineering, Intercalation (chemistry), Antifungal drug, Layered double hydroxides, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, engineering.material, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, Combinatorial chemistry, Characterization (materials science), chemistry.chemical_compound, Solid-state nuclear magnetic resonance, chemistry, Materials Chemistry, engineering, Hydroxide, Organic chemistry, [CHIM]Chemical Sciences, Reactivity (chemistry), Inorganic matrix, ComputingMilieux_MISCELLANEOUS
Abstract: International audience; Benzoxaboroles are a family of cyclic derivatives of boronic acids, whose reactivity makes them interesting candidates for the development of novel drugs. In this study, we describe the preparation of the first hybrid organic-inorganic materials involving benzoxaboroles, as a first step towards their use as new formulations for such drugs. The materials were prepared by intercalation of the simplest benzoxaborole (C7H6BO(OH), BBzx) or of its fluorinated analogue (C7H5FBO(OH), AN2690, a recently developed antifungal drug), both taken under their anionic form (benzoxaborolate), into a biodegradable inorganic matrix (a Mg-Al layered double hydroxide). Extensive characterization was carried out on the materials, notably by powder X-ray diffraction and multinuclear (11B, 27Al, 13C, 19F, 25Mg, 1H) solid state NMR, in order to describe their structure, particularly in the vicinity of the organoboron species. Three crystalline phases involving benzoxaborolate anions in association with Ca2+ or Mg2+ cations were also prepared as part of this work (Mg(C7H6BO(OH)2)2•10H2O, Mg(C7H6BO(OH)2)2•7H2O and Ca3(C7H6BO(OH)2)5(C7H6BO2)•3H2O), in order to assist in the interpretation of the spectroscopic data. A DFT computational model of the interlayer space was proposed, which is consistent with the experimental observations. Several properties of the materials were then determined with a view of using them as part of novel formulations, namely the maximum loading capacity towards benzoxaborol(at)es, the optimal storage conditions, and the release kinetics in simulated physiological media. All in all, this study serves as a benchmark not only for the development of novel formulations for benzoxaborole drugs, but more generally for the preparation of a novel class of organic-inorganic materials involving benzoxaborol(at)es.
Published: 2015
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32. Coordination polymers based on alkylboronate ligands: synthesis, characterization, and computational modelling

Author: Mark E. Smith, Dorothée Berthomieu, Danielle Laurencin, Christel Gervais, Guillaume Renaudin, Marc Reinholdt, Saad Sene, Christian Bonhomme, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC), Institut de Chimie de Clermont-Ferrand (ICCF), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Solid State NMR Group, University of Warwick, University of Warwick [Coventry], ANR, Marie Curie ERG, ANR-13-JS08-0004,BOROMAT,Développement d'une nouvelle classe de matériaux hybrides organique-inorganique incorporant des boronates/ benzoxaborolates(2013), European Project: 239206,EC:FP7:PEOPLE,FP7-PEOPLE-ERG-2008,CONTRELL(2009), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: chemistry.chemical_classification, Alkaline earth metal, Coordination polymer, Stereochemistry, Infrared spectroscopy, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, Synchrotron, Spectral line, law.invention, Inorganic Chemistry, Crystallography, chemistry.chemical_compound, Microcrystalline, chemistry, law, Phase (matter)
Abstract: International audience; Boronate ligands (R-B(OH)3-) have recently started to attract attention for the elaboration of coordination polymer networks. Here, three new crystalline structures involving butyl and octylboronate ligands are described: Sr(Bu-B(OH)3)2, Ca(Oct-B(OH)3)2 and Sr(Oct-B(OH)3)2. All were obtained as microcrystalline powders, and their structures were solved using synchrotron powder X-ray diffraction data. IR and multinuclear (13C, 11B, 43Ca, 87Sr and 1H) solid state NMR characterizations were carried out on the materials. Computational models of the novel Sr(Bu-B(OH)3)2 phase and of the previously reported Sr(Ph-B(OH)3)2.H2O structure were then developed. IR O-H stretching modes and NMR parameters were calculated for these models, and discussed in view of the experimental spectra. This work confirms the importance of performing computational studies on boronate phases, to determine the nature of the H-bond network within the materials, and better understand their spectroscopic signatures.
Published: 2015
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33. A combined experimental-computational study of benzoxaborole crystal structures

Author: Christel Gervais, Joris Vezzani, Danielle Laurencin, Dominique Granier, Sébastien Richeter, Bruno Donnadieu, Dorothée Berthomieu, P. Hubert Mutin, Saad Sene, Sylvie Bégu, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-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), and Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: MOLECULAR-CRYSTALS, Antifungal drug, ARYLBORONIC ACIDS, Crystal structure, 010402 general chemistry, 01 natural sciences, AUGMENTED-WAVE METHOD, Spectral line, INTERMOLECULAR INTERACTIONS, Computational chemistry, [CHIM.CRIS]Chemical Sciences/Cristallography, Molecule, General Materials Science, MEDICINAL CHEMISTRY, 1ST-PRINCIPLES CALCULATIONS, SPECTROSCOPY, 010405 organic chemistry, Chemistry, Intermolecular force, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, Condensed Matter Physics, BORON, 0104 chemical sciences, SOLID-STATE NMR, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Solid-state nuclear magnetic resonance, Polymorphism (materials science), Density functional theory, ULTRASOFT PSEUDOPOTENTIALS
Abstract: International audience; Benzoxaboroles are organoboron molecules which are gaining growing interest in different fields, notably for the development of new drugs. However, extensive characterization of these molecules in the solid state is still lacking. Here, questions related to the structure and spectroscopic signatures of crystalline benzoxaborole phases are thus addressed, using a combined experimental-computational approach. Two simple benzoxaboroles were studied: 1,3-dihydro-1-hydroxy-2,1-benzoxaborole (denoted as BBzx) and 5-fluoro-1,3-dihydro-1-hydroxy-2,1-benzoxaborole (also referred to as AN2690, a newly developed antifungal drug). First, the crystal structures of AN2690 and BBzx at room temperature are discussed, emphasizing the intermolecular interactions which play an important role in their formation. Then, results of IR and multinuclear (H-1, B-11, C-13 and F-19) solid state NMR characterization are presented, together with density functional theory (DFT) calculations which were carried out to assist in the interpretation of the spectra. Finally, the influence of polymorphism and anisotropic thermal expansion properties of the crystal structures on the NMR parameters of BBzx and AN2690 is discussed
Published: 2014
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34. Structural study of calcium phosphonates: a combined synchrotron powder diffraction, solid-state NMR and first-principle calculations approach

Author: Christian Bonhomme, Sylvie Bégu, Boris Bouchevreau, Saad Sene, Mark E. Smith, Danielle Laurencin, Philippe Gaveau, Francesco Mauri, Charlotte Martineau, P. Hubert Mutin, Christel Gervais, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-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), Institut de minéralogie et de physique des milieux condensés (IMPMC), Université Pierre et Marie Curie - Paris 6 (UPMC)-IPG PARIS-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Solid State NMR Group, University of Warwick, University of Warwick [Coventry], Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Université Paris Diderot - Paris 7 (UPD7)-Institut de Physique du Globe de Paris (IPG Paris)-Centre National de la Recherche Scientifique (CNRS)
Subjects: GIPAW, media_common.quotation_subject, Analytical chemistry, Ab initio, NMR crystallography, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 01 natural sciences, Asymmetry, chemistry.chemical_compound, Phase (matter), General Materials Science, 43Ca NMR, media_common, calcium, Isotropy, General Chemistry, Gauge (firearms), 021001 nanoscience & nanotechnology, Condensed Matter Physics, Phosphonate, 0104 chemical sciences, Solid-state nuclear magnetic resonance, chemistry, First principle, phosphonate, 0210 nano-technology
Abstract: International audience; The structures of four Ca-phosphonate phases are reported here: Ca(C6H5-PO3H)2 (1), Ca(C6H5-PO3)*2H2O (2), Ca(C4H9-PO3H)2 (3) and Ca(C4H9-PO3)*H2O (4). Structural models were obtained ab initio by using a combined synchrotron powder diffraction, solid-state nuclear magnetic resonance, and gauge including projector augmented wave (GIPAW) calculation approach. The 1H, 13C, 31P and 43Ca NMR parameters calculated from these structural models were found to be in good agreement with the experimental values, thereby indicating the high accuracy of the DFT-optimized structures. Correlations between the NMR parameters and structural features around the phosphonate were then analyzed, showing in particular the high sensitivity of the 31P asymmetry parameter ηCS and the 43Ca isotropic chemical shift to changes in local structure around the phosphonate groups and the Ca2+, respectively. Finally, the NMR data of a new mixed Na-Ca phosphonate phase, Ca1.5Na(C4H9-PO3)2, are reported.
Published: 2013
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35. Boronate Ligands in Materials: Determining Their Local Environment by Using a Combination of IR/Solid-State NMR Spectroscopies and DFT Calculations

Author: Christian Bonhomme, Sylvie Bégu, Danielle Laurencin, Dorothée Berthomieu, Yaroslav Filinchuk, P. Hubert Mutin, Guillaume Renaudin, Christel Gervais, Mark E. Smith, Philippe Gaveau, Claudio M. Zicovich-Wilson, Marc Reinholdt, Saad Sene, Jean-Marie Nedelec, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut de Chimie de Clermont-Ferrand (ICCF), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Facultad de Ciencias, Universidad Autonoma del Estado de Morelos (UAEM), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-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), Institut de la matière condensée et des nanosciences / Institute of Condensed Matter and Nanosciences (IMCN), Université Catholique de Louvain = Catholic University of Louvain (UCL), Solid State NMR Group, University of Warwick, University of Warwick [Coventry], Lancaster University, and Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Magnetic Resonance Spectroscopy, GIPAW, Spectrophotometry, Infrared, boronic acid, Analytical chemistry, Infrared spectroscopy, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, Ligands, 01 natural sciences, Catalysis, Spectral line, modelling, chemistry.chemical_compound, Phase (matter), Molecule, solid state NMR, 010405 organic chemistry, Ligand, Organic Chemistry, boronate, General Chemistry, Nuclear magnetic resonance spectroscopy, [CHIM.MATE]Chemical Sciences/Material chemistry, Boronic Acids, 0104 chemical sciences, Solid-state nuclear magnetic resonance, chemistry, 13. Climate action, IR, Physical chemistry, Quantum Theory, Boronic acid
Abstract: Boronic acids (R-B(OH)(2)) are a family of molecules that have found a large number of applications in materials science. In contrast, boronate anions (R-B(OH)(3)(-)) have hardly been used so far for the preparation of novel materials. Here, a new crystalline phase involving a boronate ligand is described, Ca[C(4)H(9)-B(OH)(3)](2), which is then used as a basis for the establishment of the spectroscopic signatures of boronates in the solid state. The phase was characterized by IR and multinuclear solid-state NMR spectroscopy ((1)H, (13)C, (11)B and (43)Ca), and then modeled by periodic DFT calculations. Anharmonic OH vibration frequencies were calculated as well as NMR parameters (by using the Gauge Including Projector Augmented Wave--GIPAW--method). These data allow relationships between the geometry around the OH groups in boronates and the IR and (1)H NMR spectroscopic data to be established, which will be key to the future interpretation of the spectra of more complex organic-inorganic materials containing boronate building blocks.
Published: 2013
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36. Cover Picture: Boronate Ligands in Materials: Determining Their Local Environment by Using a Combination of IR/Solid-State NMR Spectroscopies and DFT Calculations (Chem. Eur. J. 3/2013)

Author: Yaroslav Filinchuk, Jean-Marie Nedelec, Saad Sene, Danielle Laurencin, Marc Reinholdt, Philippe Gaveau, Claudio M. Zicovich-Wilson, P. Hubert Mutin, Christel Gervais, Christian Bonhomme, Mark E. Smith, Dorothée Berthomieu, Sylvie Bégu, and Guillaume Renaudin
Subjects: Solid-state nuclear magnetic resonance, Computational chemistry, Chemistry, Organic Chemistry, Infrared spectroscopy, chemistry.chemical_element, Local environment, Cover (algebra), General Chemistry, Nuclear magnetic resonance spectroscopy, Boron, Catalysis
Published: 2013
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37. Intercalation of Benzoxaborolate Anions in LayeredDouble Hydroxides: Toward Hybrid Formulations for Benzoxaborole Drugs.

Author: Saad Sene, Sylvie Bégu, Christel Gervais, Guillaume Renaudin, Adel Mesbah, Mark E. Smith, P. Hubert Mutin, Arie van der Lee, Jean-Marie Nedelec, Christian Bonhomme, and Danielle Laurencin
Subjects: *EXCIPIENTS, *PHARMACEUTICAL industry, *HYDROXIDES, *BORONIC acids, *ANTIFUNGAL agents, *THERAPEUTICS
Abstract: Benzoxaboroles are a family of cyclicderivatives of boronic acids,whose reactivity makes them interesting candidates for the developmentof novel drugs. In this study, we describe the preparation of thefirst hybrid organic–inorganic materials involving benzoxaboroles,as a first step toward their use as new formulations for such drugs.The materials were prepared by intercalation of the simplest benzoxaborole(C7H6BO(OH), BBzx) or of its fluorinated analogue(C7H5FBO(OH), AN2690, a recently developed antifungaldrug), both taken under their anionic form (benzoxaborolate), intoa biodegradable inorganic matrix (a Mg–Al layered double hydroxide).Extensive characterization was carried out on the materials, notablyby powder X-ray diffraction and multinuclear (11B, 27Al, 13C, 19F, 25Mg, and 1H) solid state NMR, in order to describe their structure,particularly in the vicinity of the organoboron species. Three crystallinephases involving benzoxaborolate anions in association with Ca2+or Mg2+cations were also prepared as part ofthis work (Mg(C7H6BO(OH)2)2·10H2O, Mg(C7H6BO(OH)2)2·7H2O and Ca3(C7H6BO(OH)2)5(C7H6BO2)·3H2O), in order to assist in theinterpretation of the spectroscopic data. A DFT computational modelof the interlayer space was proposed, which is consistent with theexperimental observations. Several properties of the materials werethen determined with a view of using them as part of novel formulations,namely the maximum loading capacity toward benzoxaborol(at)es, theoptimal storage conditions, and the release kinetics in simulatedphysiological media. All in all, this study serves as a benchmarknot only for the development of novel formulations for benzoxaboroledrugs, but more generally for the preparation of a novel class oforganic–inorganic materials involving benzoxaborol(at)es. [ABSTRACT FROM AUTHOR]
Published: 2015
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