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3. Exploring the bottlenecks of anionic redox in Li-rich layered sulfides

Author

Saha, Sujoy, Assat, Gaurav, Sougrati, Moulay Tahar, Foix, Dominique, Li, Haifeng, Vergnet, Jean, Turi, Soma, Ha, Yang, Yang, Wanli, Cabana, Jordi, Rousse, Gwenaëlle, Abakumov, Artem M, and Tarascon, Jean-Marie

Subjects
Affordable and Clean Energy, Electrical and Electronic Engineering, Environmental Engineering
Abstract

Anionic redox chemistry has emerged as a new paradigm to design higher-energy lithium ion-battery cathode materials such as Li-rich layered oxides. However, they suffer from voltage fade, large hysteresis and sluggish kinetics, which originate intriguingly from the anionic redox activity itself. To fundamentally understand these issues, we decided to act on the ligand by designing new Li-rich layered sulfides Li1.33 – 2y/3Ti0.67 – y/3FeyS2, among which the y = 0.3 member shows sustained reversible capacities of ~245 mAh g−1 due to cumulated cationic (Fe2+/3+) and anionic (S2−/Sn−, n < 2) redox processes. Moreover, its negligible initial cycle irreversibility, mitigated voltage fade upon long cycling, low voltage hysteresis and fast kinetics compare positively with its Li-rich oxide analogues. Moving from the oxygen ligand to the sulfur ligand thus partially alleviates the practical bottlenecks affecting anionic redox, although it penalizes the redox potential and energy density. Overall, these sulfides provide chemical clues to improve the holistic performance of anionic redox electrodes, which may guide us to ultimately exploit the energy benefits of oxygen redox.

Published
2019

11. KFe(C2O4)F : a fluoro-oxalate cathode material for Li/Na-ion batteries

Author

Pramanik, Atin, Manche, Alexis G., Smeaton, Megan T., Sougrati, Moulay-Tahar, Lightfoot, Philip, Armstrong, Anthony Robert, EPSRC, University of St Andrews. School of Chemistry, and University of St Andrews. EaSTCHEM

Subjects
MCC, QC Physics, Cathode materials, Electrochemistry, NDAS, Oxalate, Rechargeable battery, QD, QD Chemistry, Na-ion/Li-ion, QC
Abstract

Funding: The authors want to thank EPSRC (EP/R030472/1) and the Faraday Institution (FIRG018) for their financial support. In addition, AGM wishes to thank the Faraday Institution for financial support and training (Grant number FITG033). The authors also thank EPSRC Light Element Analysis Facility Grant EP/T019298/1 and the EPSRC Strategic Equipment Resource Grant EP/R023751/1. The iron-based polyanionic fluoro-oxalate material, KFe(C2O4)F (KFCF), has been synthesized by hydrothermal methods. This compound shows promising reversible lithium and sodium insertion properties as a cathode material. The material delivered a first-cycle discharge capacity of 120 mAh g-1 at ∼3.3 V (Li+/Li) and 97.4 mAh g-1 at ∼3.0 V (Na+/Na) in LIB and NIB, respectively. Stable cycling performance was observed in both cases. The involvement of reversible Fe2+/Fe3+ redox was confirmed by ex-situ Mössbauer spectroscopy supported by first-principles calculations. This study reveals promising performance from a mixed oxalate-fluoride based polyanionic material thereby opening up further possibilities for materials discovery in the design of new electrode materials. Publisher PDF

Published
2023

14. The structural and magnetic features of perovskite oxides La1–xSrxMnO3+δ (x = 0.05, 0.10, 0.20) depending on the strontium doping content and heat treatment

Author

Pchelina, Diana I., primary, Sedykh, Vera D., additional, Chistyakova, Nataliya I., additional, Rusakov, Vyacheslav S., additional, Alekhina, Yulia A., additional, Tselebrovskiy, Alexey N., additional, Fraisse, Bernard, additional, Stievano, Lorenzo, additional, and Sougrati, Moulay Tahar, additional

Published
2022
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15. KFe(C2O4)F: A Fluoro‐oxalate Cathode Material for Li/Na‐Ion Batteries.

Author

Pramanik, Atin, Manche, Alexis G., Smeaton, Megan T., Sougrati, Moulay‐Tahar, Lightfoot, Philip, and Armstrong, Anthony Robert

Subjects
OXALATES, CATHODES, MOSSBAUER spectroscopy, LITHIUM, STORAGE batteries
Abstract

The iron‐based polyanionic fluoro‐oxalate material, KFe(C2O4)F (KFCF), has been synthesized by hydrothermal methods. This compound shows promising reversible lithium and sodium insertion properties as a cathode material. The material delivered a first‐cycle discharge capacity of 120 mAh g−1 at ∼3.3 V (Li+/Li) and 97.4 mAh g−1 at ∼3.0 V (Na+/Na) in LIB and NIB, respectively. Stable cycling performance was observed in both cases. The involvement of reversible Fe2+/Fe3+ redox was confirmed by ex‐situ Mössbauer spectroscopy supported by first‐principles calculations. This study reveals promising performance from a mixed oxalate‐fluoride based polyanionic material thereby opening up further possibilities for materials discovery in the design of new electrode materials. [ABSTRACT FROM AUTHOR]

Published
2023
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19. Synthesis of silica-polymer core-shell hybrid materials with enhanced mechanical properties using a new bifunctional silane-based photoinitiator as coupling agent

Author

Haouari, Chérazade, Squires, Alexander, Berthelot, Romain, Stievano, Lorenzo, Sougrati, Moulay Tahar, Morgan, Benjamin, Lebedev, Oleg, Iadecola, Antonella, Borkiewicz, Olaf, Dambournet, Damien, Laboratoire catalyse et spectrochimie (LCS), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Matériaux Polymères Interfaces Environnement Marin - EA 4323 (MAPIEM), Université de Toulon (UTLN), Russian Academy of Sciences [Moscow] (RAS), Shemyakin-Ovchinnikov Institute of Bioorganic Chemistry (IBCh RAS), Laser Zentrum Hannover e.V. (LZH), Sechenov First Moscow State Medical University, Department of Chemical Sciences, University of Messina, Department of Advanced Materials for Energy, Catalonia Institute for Energy Research (IREC), University of Antwerp (UA), Dipartimento di Fisica e Astronomia 'Galileo Galilei', Università degli Studi di Padova = University of Padua (Unipd), CIC NanoGUNE BRTA, 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), University of Bath [Bath], The Faraday Institution, Réseau sur le stockage électrochimique de l'énergie (RS2E), Université de Nantes (UN)-Aix Marseille Université (AMU)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA), Argonne National Laboratory [Lemont] (ANL), PHysicochimie des Electrolytes et Nanosystèmes InterfaciauX (PHENIX), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Public Health Expertise [Paris, France], Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Université de Caen Normandie (UNICAEN), Normandie Université (NU), École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), and Normandie Université (NU)-Institut de Chimie du CNRS (INC)

Subjects
Acrylate polymer, Materials science, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, chemistry.chemical_compound, Materials Chemistry, [CHIM]Chemical Sciences, General Materials Science, Bifunctional, Polymer, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Core-shell, Silica, 021001 nanoscience & nanotechnology, Silane, Hybrid, 0104 chemical sciences, Coupling-agent, Silanol, Photopolymer, chemistry, Chemical engineering, Mechanics of Materials, 0210 nano-technology, Hybrid material, Photoinitiator
Abstract

International audience; Here, we report the use of new bifunctional silane-based type-1 photoinitiator (SPI-1) as a coupling agent for photopolymer filler and silica grafting. The SPI-1 is grafted on the surface of silica nanoparticles via interactions between the ethoxy group of the silane and the silanol groups of the silica surface. The grafted particles are then dispersed or embedded in/with acrylate polymer by a direct photopolymerization process. The materials were characterized using different techniques including UV–vis spectroscopy, FTIR, TGA, and TEM. Their mechanical properties and the surface morphology were also investigated using AFM and DMA analyses. A significant change and enhancement of the mechanical properties of the newly synthesized materials were observed with respect to that of the unmodified silica. The analysis of the morphology at the microscale level reveals interesting information on the origin of this enhancement and on the dispersion of the filler in the polymer matrix.

Published
2021
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20. Rhombohedral Iron Trifluoride with a Hierarchized Macroporous/Mesoporous Texture from Gaseous Fluorination of Iron Disilicide

Author

Delbègue Diane, Guérin Katia, Laik Barbara, Pereira-Ramos Jean-Pierre, Sougrati Moulay-Tahar, and Cénac-Morthe Céline

Subjects
Environmental sciences, GE1-350
Abstract

Stable low temperature rhombohedral iron trifluoride has been obtained by the fluorination under the pure fluorine gas of iron disilicide. The combination of both unusual fluorination process and precursor avoids to get unhydrated crystalline FeF3 particles and allows the formation of hierarchized channels of mesoporous/macroporous texture favorable for lithium diffusion. The fluorination mechanism proceeds by temperature steps from the formation, for a fluorination temperature below 200 °C, of an amorphous phase and an intermediate iron difluoride identified mainly by 57Fe Mössbauer spectroscopy before getting, as soon as a fluorination temperature of 260 °C is reached, the rhombohedral FeF3. Both amorphous and crystallized samples display good ability for electrochemical process when used as cathode in lithium-ion battery. The low diameter of rhombohedral structure channels is balanced by an appropriate mesoporous texture and a capacity of 225 mAh.g−1 after 5 cycles for a discharge cut-off of 2.5 V vs. Li+/Li at a current density of C/20 has been obtained and stabilized at 95 mAh.g−1 after 116 cycles.

Published
2017
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21. 2021 roadmap for sodium-ion batteries

Author

Tapia-Ruiz, Nuria, primary, Armstrong, A Robert, additional, Alptekin, Hande, additional, Amores, Marco A, additional, Au, Heather, additional, Barker, Jerry, additional, Boston, Rebecca, additional, Brant, William R, additional, Brittain, Jake M, additional, Chen, Yue, additional, Chhowalla, Manish, additional, Choi, Yong-Seok, additional, Costa, Sara I R, additional, Crespo Ribadeneyra, Maria, additional, Cussen, Serena A, additional, Cussen, Edmund J, additional, David, William I F, additional, Desai, Aamod V, additional, Dickson, Stewart A M, additional, Eweka, Emmanuel I, additional, Forero-Saboya, Juan D, additional, Grey, Clare P, additional, Griffin, John M, additional, Gross, Peter, additional, Hua, Xiao, additional, Irvine, John T S, additional, Johansson, Patrik, additional, Jones, Martin O, additional, Karlsmo, Martin, additional, Kendrick, Emma, additional, Kim, Eunjeong, additional, Kolosov, Oleg V, additional, Li, Zhuangnan, additional, Mertens, Stijn F L, additional, Mogensen, Ronnie, additional, Monconduit, Laure, additional, Morris, Russell E, additional, Naylor, Andrew J, additional, Nikman, Shahin, additional, O’Keefe, Christopher A, additional, Ould, Darren M C, additional, Palgrave, R G, additional, Poizot, Philippe, additional, Ponrouch, Alexandre, additional, Renault, Stéven, additional, Reynolds, Emily M, additional, Rudola, Ashish, additional, Sayers, Ruth, additional, Scanlon, David O, additional, Sen, S, additional, Seymour, Valerie R, additional, Silván, Begoña, additional, Sougrati, Moulay Tahar, additional, Stievano, Lorenzo, additional, Stone, Grant S, additional, Thomas, Chris I, additional, Titirici, Maria-Magdalena, additional, Tong, Jincheng, additional, Wood, Thomas J, additional, Wright, Dominic S, additional, and Younesi, Reza, additional

Published
2021
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23. Correlating ligand-to-metal charge transfer with voltage hysteresis in a Li-rich rock-salt compound exhibiting anionic redox

Author

Li, Biao, Sougrati, Moulay Tahar, Rousse, Gwenaëlle, Morozov, Anatolii V., Dedryvère, Rémi, Iadecola, Antonella, Senyshyn, Anatoliy, Zhang, Leiting, Abakumov, Artem M., Doublet, Marie-Liesse, Tarascon, Jean-Marie, Li, Biao, Sougrati, Moulay Tahar, Rousse, Gwenaëlle, Morozov, Anatolii V., Dedryvère, Rémi, Iadecola, Antonella, Senyshyn, Anatoliy, Zhang, Leiting, Abakumov, Artem M., Doublet, Marie-Liesse, and Tarascon, Jean-Marie

Published
2021
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24. 2021 roadmap for sodium-ion batteries

Author

Tapia-Ruiz, Nuria, Armstrong, A. Robert, Alptekin, Hande, Amores, Marco A., Au, Heather, Barker, Jerry, Boston, Rebecca, Brant, William R., Brittain, Jake M., Chen, Yue, Chhowalla, Manish, Choi, Yong-Seok, Costa, Sara I. R., Crespo Ribadeneyra, Maria, Cussen, Serena A., Cussen, Edmund J., David, William I. F., Desai, Aamod, V, Dickson, Stewart A. M., Eweka, Emmanuel, I, Forero-Saboya, Juan D., Grey, Clare P., Griffin, John M., Gross, Peter, Hua, Xiao, Irvine, John T. S., Johansson, Patrik, Jones, Martin O., Karlsmo, Martin, Kendrick, Emma, Kim, Eunjeong, Kolosov, Oleg, V, Li, Zhuangnan, Mertens, Stijn F. L., Mogensen, Ronnie, Monconduit, Laure, Morris, Russell E., Naylor, Andrew J., Nikman, Shahin, O'Keefe, Christopher A., Ould, Darren M. C., Palgrave, R. G., Poizot, Philippe, Ponrouch, Alexandre, Renault, Steven, Reynolds, Emily M., Rudola, Ashish, Sayers, Ruth, Scanlon, David O., Sen, S., Seymour, Valerie R., Silvan, Begona, Sougrati, Moulay Tahar, Stievano, Lorenzo, Stone, Grant S., Thomas, Chris, I, Titirici, Maria-Magdalena, Tong, Jincheng, Wood, Thomas J., Wright, Dominic S., Younesi, Reza, Tapia-Ruiz, Nuria, Armstrong, A. Robert, Alptekin, Hande, Amores, Marco A., Au, Heather, Barker, Jerry, Boston, Rebecca, Brant, William R., Brittain, Jake M., Chen, Yue, Chhowalla, Manish, Choi, Yong-Seok, Costa, Sara I. R., Crespo Ribadeneyra, Maria, Cussen, Serena A., Cussen, Edmund J., David, William I. F., Desai, Aamod, V, Dickson, Stewart A. M., Eweka, Emmanuel, I, Forero-Saboya, Juan D., Grey, Clare P., Griffin, John M., Gross, Peter, Hua, Xiao, Irvine, John T. S., Johansson, Patrik, Jones, Martin O., Karlsmo, Martin, Kendrick, Emma, Kim, Eunjeong, Kolosov, Oleg, V, Li, Zhuangnan, Mertens, Stijn F. L., Mogensen, Ronnie, Monconduit, Laure, Morris, Russell E., Naylor, Andrew J., Nikman, Shahin, O'Keefe, Christopher A., Ould, Darren M. C., Palgrave, R. G., Poizot, Philippe, Ponrouch, Alexandre, Renault, Steven, Reynolds, Emily M., Rudola, Ashish, Sayers, Ruth, Scanlon, David O., Sen, S., Seymour, Valerie R., Silvan, Begona, Sougrati, Moulay Tahar, Stievano, Lorenzo, Stone, Grant S., Thomas, Chris, I, Titirici, Maria-Magdalena, Tong, Jincheng, Wood, Thomas J., Wright, Dominic S., and Younesi, Reza

Abstract

Increasing concerns regarding the sustainability of lithium sources, due to their limited availability and consequent expected price increase, have raised awareness of the importance of developing alternative energy-storage candidates that can sustain the ever-growing energy demand. Furthermore, limitations on the availability of the transition metals used in the manufacturing of cathode materials, together with questionable mining practices, are driving development towards more sustainable elements. Given the uniformly high abundance and cost-effectiveness of sodium, as well as its very suitable redox potential (close to that of lithium), sodium-ion battery technology offers tremendous potential to be a counterpart to lithium-ion batteries (LIBs) in different application scenarios, such as stationary energy storage and low-cost vehicles. This potential is reflected by the major investments that are being made by industry in a wide variety of markets and in diverse material combinations. Despite the associated advantages of being a drop-in replacement for LIBs, there are remarkable differences in the physicochemical properties between sodium and lithium that give rise to different behaviours, for example, different coordination preferences in compounds, desolvation energies, or solubility of the solid-electrolyte interphase inorganic salt components. This demands a more detailed study of the underlying physical and chemical processes occurring in sodium-ion batteries and allows great scope for groundbreaking advances in the field, from lab-scale to scale-up. This roadmap provides an extensive review by experts in academia and industry of the current state of the art in 2021 and the different research directions and strategies currently underway to improve the performance of sodium-ion batteries. The aim is to provide an opinion with respect to the current challenges and opportunities, from the fundamental properties to the practical applications of this technology.

Published
2021
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25. Metal Oxide Clusters on Nitrogen-Doped Carbon are Highly Selective for CO2Electroreduction to CO

Author

European Commission, Ministerio de Ciencia, Innovación y Universidades (España), Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, Li, Jingkun, Zitolo, Andrea, Garcés-Pineda, Felipe A., Tristan, Asset, Kodali, Mounika, Tang, Peng-Yi, Arbiol, Jordi, Galán-Mascarós, José Ramón, Atanassov, Plamen, Zenyuk, Iryna V., Sougrati, Moulay Tahar, Jaouen, Frédéric, European Commission, Ministerio de Ciencia, Innovación y Universidades (España), Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, Li, Jingkun, Zitolo, Andrea, Garcés-Pineda, Felipe A., Tristan, Asset, Kodali, Mounika, Tang, Peng-Yi, Arbiol, Jordi, Galán-Mascarós, José Ramón, Atanassov, Plamen, Zenyuk, Iryna V., Sougrati, Moulay Tahar, and Jaouen, Frédéric

Abstract

The electrochemical reduction of CO2 (eCO2RR) using renewable energy is an effective approach to pursue carbon neutrality. The eCO2RR to CO is indispensable in promoting C-C coupling through bifunctional catalysis and achieving cascade conversion from CO2 to C2+. This work investigates a series of M/N-C (M = Mn, Fe, Co, Ni, Cu, and Zn) catalysts, for which the metal precursor interacted with the nitrogen-doped carbon support (N-C) at room temperature, resulting in the metal being present as (sub)nanosized metal oxide clusters under ex situ conditions, except for Cu/N-C and Zn/N-C. A volcano trend in their activity toward CO as a function of the group of the transition metal is revealed, with Co/N-C exhibiting the highest activity at -0.5 V versus RHE, while Ni/N-C shows both appreciable activity and selectivity. Operando X-ray absorption spectroscopy shows that the majority of Cu atoms in Cu/N-C form Cu0 clusters during eCO2RR, while Mn/, Fe/, Co/, and Ni/N-C catalysts maintain the metal hydroxide structures, with a minor amount of M0 formed in Fe/, Co/, and Ni/N-C. The superior activity of Fe/, Co/, and Ni/N-C is ascribed to the phase contraction and the HCO3- insertion into the layered structure of metal hydroxides. Our work provides a facile synthetic approach toward highly active and selective electrocatalysts to convert CO2 into CO. Coupled with state-of-the-art NiFe-based anodes in a full-cell device, Ni/N-C exhibits >80% Faradaic efficiency toward CO at 100 mA cm-2.

Published
2021

26. Unveiling redox mechanism at the iron centers in the mechanochemically activated conversion of CO2 in the presence of olivine.

Author

Farina, Valeria, Simula, Maria Domenica, Taras, Alessandro, Cappai, Luca, Sougrati, Moulay Tahar, Mulas, Gabriele, Garroni, Sebastiano, Enzo, Stefano, and Stievano, Lorenzo

Subjects
OLIVINE, IRON, IRON silicates, MOSSBAUER spectroscopy, WEATHERING, IRON oxides, OXIDATION-reduction reaction
Abstract

The transformation of olivine during the conversion of CO2 to light hydrocarbons activated by mechanochemical treatments at different impact frequencies was studied by a combination of several complementary characterization methods including X-ray diffraction, Raman and 57Fe Mössbauer spectroscopy. Several olivine samples were studied as a function of the milling time, indicating the gradual transformation of FeII-containing olivine into new FeIII-containing weathering products including iron oxides, magnesium iron carbonates and silicates. The results presented here complement those of a previous study on the weathering process of olivine promoted by mechanochemical activation, by demonstrating the role of the redox activity of the iron species during the activation process. These additional spectroscopic results allow us to thoroughly understand the complex weathering mechanism and to correlate it with the efficiency of the CO2 conversion and storage properties of mechanochemically activated olivine. [ABSTRACT FROM AUTHOR]

Published
2022
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27. The evolution pathway from iron compounds to Fe 1 (II)-N 4 sites through gas-phase iron during pyrolysis

Author

Richard, Lynne Larochelle, Sougrati, Moulay Tahar, Li, Jingkun, Jiao, Li, Wegener, Evan, Richard, Lynne, Liu, Ershuai, Zitolo, Andrea, Sougrati, Moulay, Mukerjee, Sanjeev, Zhao, Zipeng, Huang, Yu, Yang, Fan, Zhong, Sichen, Xu, Hui, Kropf, A. Jeremy, Jaouen, Frederic, Myers, Deborah, Jia, Qingying, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), 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)-Institut de Chimie du CNRS (INC)

Subjects
Absorption spectroscopy, chemistry.chemical_element, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 01 natural sciences, Biochemistry, Catalysis, 0104 chemical sciences, Gas phase, Colloid and Surface Chemistry, chemistry, Polymer chemistry, Atom, Oxygen reduction reaction, Carbon, Pyrolysis, ComputingMilieux_MISCELLANEOUS
Abstract

Pyrolysis is indispensable for synthesizing highly active Fe-N-C catalysts for the oxygen reduction reaction (ORR) in acid, but how Fe, N, and C precursors transform to ORR-active sites during pyrolysis remains unclear. This knowledge gap obscures the connections between the input precursors and the output products, clouding the pathway toward Fe-N-C catalyst improvement. Herein, we unravel the evolution pathway of precursors to ORR-active catalyst comprised exclusively of single-atom Fe1(II)-N4 sites via in-temperature X-ray absorption spectroscopy. The Fe precursor transforms to Fe oxides below 300 °C and then to tetrahedral Fe1(II)-O4 via a crystal-to-melt-like transformation below 600 °C. The Fe1(II)-O4 releases a single Fe atom that diffuses into the N-doped carbon defect forming Fe1(II)-N4 above 600 °C. This vapor-phase single Fe atom transport mechanism is verified by synthesizing Fe1(II)-N4 sites via "noncontact pyrolysis" wherein the Fe precursor is not in physical contact with the N and C precursors during pyrolysis.

Published
2020
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28. P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction:[Inkl. Correction]

Author

Luo, Fang, Roy, Aaron, Silvioli, Luca, Cullen, David A., Zitolo, Andrea, Sougrati, Moulay Tahar, Oguz, Ismail Can, Mineva, Tzonka, Teschner, Detre, Wagner, Stephan, Wen, Ju, Dionigi, Fabio, Kramm, Ulrike I., Rossmeisl, Jan, Jaouen, Frédéric, Strasser, Peter, Luo, Fang, Roy, Aaron, Silvioli, Luca, Cullen, David A., Zitolo, Andrea, Sougrati, Moulay Tahar, Oguz, Ismail Can, Mineva, Tzonka, Teschner, Detre, Wagner, Stephan, Wen, Ju, Dionigi, Fabio, Kramm, Ulrike I., Rossmeisl, Jan, Jaouen, Frédéric, and Strasser, Peter

Abstract

This contribution reports the discovery and analysis of a p-block Sn-based catalyst for the electroreduction of molecular oxygen in acidic conditions at fuel cell cathodes; the catalyst is free of platinum-group metals and contains single-metal-atom actives sites coordinated by nitrogen. The prepared SnNC catalysts meet and exceed state-of-the-art FeNC catalysts in terms of intrinsic catalytic turn-over frequency and hydrogen–air fuel cell power density. The SnNC-NH3 catalysts displayed a 40–50% higher current density than FeNC-NH3 at cell voltages below 0.7 V. Additional benefits include a highly favourable selectivity for the four-electron reduction pathway and a Fenton-inactive character of Sn. A range of analytical techniques combined with density functional theory calculations indicate that stannic Sn(iv)Nx single-metal sites with moderate oxygen chemisorption properties and low pyridinic N coordination numbers act as catalytically active moieties. The superior proton-exchange membrane fuel cell performance of SnNC cathode catalysts under realistic, hydrogen–air fuel cell conditions, particularly after NH3 activation treatment, makes them a promising alternative to today’s state-of-the-art Fe-based catalysts.

Published
2020

29. Porous Si/Cu6Sn5/C composite containing native oxides as anode material for lithium-ion batteries.

Author

He, Yawen, Ye, Zhongbin, Chamas, Mohamad, Sougrati, Moulay Tahar, and Lippens, Pierre-Emmanuel

Subjects
LITHIUM-ion batteries, X-ray photoelectron spectroscopy, ALUMINUM-lithium alloys, MECHANICAL alloying, MOSSBAUER spectroscopy, CHEMICAL milling
Abstract

Porous Si/Cu6Sn5/C composite containing native oxides was prepared via solid-state mechanical milling and wet chemical etching. This composite was used as anode material for Li-ion batteries. X-ray diffraction, scanning electron microscopy, 119Sn Mössbauer spectroscopy, and X-ray photoelectron spectroscopy show that the composite has a pitaya-like morphology based on porous Si and embedded Cu6Sn5 non-porous microparticles with surface native oxides. Both Si and Cu6Sn5 are electrochemically active, and the activation process during the first charge–discharge improves the nanostructuration of the composite that helps buffer the volume variations of the Li-Si and Li-Sn alloying reactions. The porous composite delivers a reversible and stable capacity of 900 mAh g−1 at a galvanostatic current density of 422 mA g−1 with a retention of 90% for 100 cycles, which is higher than porous Si (53%). The stability during cycling is explained by buffering effect, enhanced electrode conductivity, and stable SEI due to the presence of native oxides and the use of FEC-containing electrolyte. [ABSTRACT FROM AUTHOR]

Published
2022
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32. In situ/operandoMössbauer spectroscopy for probing heterogeneous catalysis

Author

Zeng, Yaqiong, Li, Xuning, Wang, Junhu, Sougrati, Moulay Tahar, Huang, Yanqiang, Zhang, Tao, and Liu, Bin

Abstract

In situ/operandoMössbauer spectroscopy is one of the most powerful techniques to quantitatively monitor the coordination and electronic structure of Mössbauer isotopes (119Sn, 57Fe, etc.) contained in heterogeneous catalysts under practical reaction conditions. To promote further progress in identifying the real structure of catalytic site(s) and revealing the underlying catalytic mechanism, herein we thoroughly summarize the recent advances of in situ/operandoMössbauer technique for probing heterogeneous catalysts and electrode materials for sustainable energy applications, including electrocatalysis, thermocatalysis, Li-ion batteries, etc. The unique role of this technique in different catalytic system is discussed with emphasis placed on several typical research advances. Moreover, the recent emerging operandoMössbauer technique for the study of single-atom catalysts, which is considered as a new eye for providing electronic-level insight into catalytic mechanism, is highlighted. Finally, the outlooks and challenges are discussed toward further application and rising influence of in situ/operandoMössbauer spectroscopy in heterogeneous catalysis.

Published
2021
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34. Role of iron in Na1.5Fe0.5Ti1.5(PO4)(3)/C as electrode material for Na-ion batteries studied by operando Mossbauer spectroscopy

Author

Difi, Siham, Saadoune, Ismael, Sougrati, Moulay Tahar, Hakkou, Rachid, Edström, Kristina, Lippens, Pierre-Emmanuel, Difi, Siham, Saadoune, Ismael, Sougrati, Moulay Tahar, Hakkou, Rachid, Edström, Kristina, and Lippens, Pierre-Emmanuel

Abstract

The role of iron in Na1.5Fe0.5Ti1.5(PO4)(3)/C electrode material for Na batteries has been studied by Fe-57 Mossbauer spectroscopy in operando mode. The potential profile obtained in the galvanostatic regime shows three plateaus at different voltages due to different reaction mechanisms. Two of them, at 2.2 and 0.3 V vs Na+/Na-0, have been associated to redox processes involving iron and titanium in Na1.5Fe0.5Ti1.5(PO4)(3). The role of titanium was previously elucidated for NaTi2(PO4)(3) and the effect of the substitution of Fe for Ti was investigated with 57Fe Mossbauer spectroscopy. We show that iron is an electrochemically active center at 2.2 V with the reversible Fe3+/Fe2+ transformation and then remains at the oxidation state Fe2+ along the sodiation until the end of discharge at 0 V.

Published
2016
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36. Investigation of Na Removal/Insertion Mechanism in Na1.86Fe3(PO4) 3 Cathode Material

Author

Rachid Essehli, Hamdi Ben Yahia, Kenza Maher, Sougrati Moulay Tahar, Ali Abouimrane, Jin-Bum Park, Yang-Kook Sun, Mariam Almaadeed, and Ilias Belharouak

Abstract

In recent years, sodium batteries have raised interest as cheap rechargeable batteries for large format rechargeable battery applications such as the grid storage. A number of promising cathode materials has already been tested, however their electrochemical performances remain below their lithium counterpart cathodes. Complete structural and electrochemical investigations are needed to improve the characteristics of existing sodium electrode materials, design and synthesis of new ones with improved battery performance. Phosphate based materials are considered as promising cathode materials for sodium batteries due to their low cost and the variety of structural arrangements. In addition, it is predicted that phosphate cathode materials are thermally and electrochemically stable due to the presence of strong P-O bonds. The alluaudite-type structure, with the general formula AA’BB’2(PO4)3 (A and A’ = Li, Na; B is a large six coordinated cation; B’ is a small six coordinated cation), has been intensively studied as electrode materials for LIBs and/or NIBs. In the present work, we report on the synthesis, characterization and electrochemical performance of a new Na1.86Fe3(PO4)3 alluaudite-type structure compound. The material delivers ~ 109 mAhg-1 as a reversible capacity at ~ 3 V with a small capacity fade during cycling. The refinement of the structure by the Rietveld method and results of Mössbauer experiments indicate the presence of sodium deficiency and a Fe2+/Fe3+ ratio below 2/1 in the pristine material. Detailed study on the mechanism of sodium removal/insertion will be presented using X-ray, galvanometric cycling, cyclic voltammetry and Mössbauer techniques.

Published
2016
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37. Magnetic interactions at the origin of abnormal magnetic fabrics in lava flows: a case study from Kerguelen flood basalts

Author

FANJAT, Gregory, Camps, Pierre, Shcherbakov, Valera, BAROU, Fabrice, Sougrati, Moulay Tahar, Perrin, Mireille, Manteau et Interfaces, Géosciences Montpellier, Université des Antilles et de la Guyane (UAG)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Université des Antilles et de la Guyane (UAG)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de météorologie physique (LaMP), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Institut Universitaire de Technologie de Montluçon (IUT), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), 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), Franche-Comté Électronique Mécanique, Thermique et Optique - Sciences et Technologies (UMR 6174) (FEMTO-ST), Université de Technologie de Belfort-Montbeliard (UTBM)-Ecole Nationale Supérieure de Mécanique et des Microtechniques (ENSMM)-Centre National de la Recherche Scientifique (CNRS)-Université de Franche-Comté (UFC), Université Bourgogne Franche-Comté [COMUE] (UBFC)-Université Bourgogne Franche-Comté [COMUE] (UBFC), Recherches en Psychopathologie, nouveaux symptômes et lien social (EA 4050), Université de Poitiers-Université de Brest (UBO)-Université Catholique de l'Ouest (UCO)-Université de Rennes 2 (UR2), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES), Université de Franche-Comté (UFC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Mécanique et des Microtechniques (ENSMM)-Université de Technologie de Belfort-Montbeliard (UTBM), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - 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 national des sciences de l'Univers (INSU - CNRS)-Université de Montpellier (UM)-Université des Antilles (UA)-Centre National de la Recherche Scientifique (CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), 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), Université des Antilles et de la Guyane (UAG)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Montpellier (UM)-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), Université de Franche-Comté (UFC), and Université Bourgogne Franche-Comté [COMUE] (UBFC)-Université Bourgogne Franche-Comté [COMUE] (UBFC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Mécanique et des Microtechniques (ENSMM)-Université de Technologie de Belfort-Montbeliard (UTBM)

Subjects
Rock and mineral magnetism, [SDU.STU.GP]Sciences of the Universe [physics]/Earth Sciences/Geophysics [physics.geo-ph], [SDE.MCG]Environmental Sciences/Global Changes, [PHYS.PHYS.PHYS-GEO-PH]Physics [physics]/Physics [physics]/Geophysics [physics.geo-ph], Eruption mechanisms and flow emplacement, Magnetic fabrics and anisotropy, Indian Ocean
Abstract

International audience; Anisotropy of low-field magnetic susceptibility (AMS) of basaltic lava flows can give some clues about post-emplacement tilting occurring in volcanic sequences. Such a study has been carried out on a sequence of 19 successive lava flows from Kerguelen Archipelago. Surprisingly, two different patterns were observed. The first one - herein called normal fabric - is consistent with the lava-flow direction inferred from geological observations, whereas the second one observed for about 70 per cent of the analysed samples - herein called abnormal fabric - appears to be unrelated to the shear history of the lava flows during their emplacements. These abnormal fabrics are not strictly inverse fabric but seem to have a more complex origin. The unusual nature of these abnormal fabrics has been confirmed by lattice preferred orientation of plagioclases obtained from high-resolution electron backscattered diffraction measurements. The aim of this study is to propose a physical interpretation of these fabrics. A first step in our understanding was to clearly identify the nature and the magnetic properties of the Fe-Ti oxides assemblage. Thus, we present a comprehensive rock magnetic analysis relying on low- and high-temperature thermomagnetic curves (K-T), crossover diagrams, first-order reversal curves, ore-microscopy, Mössbauer measurements and electron backscattered images. We found that in the present case the abnormal fabrics are probably linked to a mixture of prevailing single domain (SD) strongly interacting grains population and a subsidiary multidomain grains population. SD grains are identified as small magnetite crystallized within the interstitial glass in globular aggregates along the silicate framework. Then a question arises: to what extent such SD interacting grains in globular aggregates can affect the magnetic susceptibility and its anisotropy? To answer this question, we developed a physical model in which the total energy density of an SD grain with an uniaxial anisotropy is minimized. In this model, the distribution function of the direction of the magnetic interaction field is comprised between two boundary states. It is either isotropic, which formally corresponds to the thermal demagnetized state, or it is ordered, which formally corresponds to the Alternative Field demagnetized state. We show that in both cases the degree of anisotropy decreases as the interaction field increases. Thus, we conclude that the abnormal fabric encountered in this study can be simply explained by strong magnetostatic interactions that would explain the large scattering of AMS often observed in basaltic lava flows.

Published
2012
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38. Mechanisms and Performances of Na1.5Fe0.5Ti1.5(PO4)(3)/C Composite as Electrode Material for Na-Ion Batteries

Author

Difi, Siham, Saadoune, Ismael, Sougrati, Moulay Tahar, Hakkou, Rachid, Edström, Kristina, Lippens, Pierre-Emmanuel, Difi, Siham, Saadoune, Ismael, Sougrati, Moulay Tahar, Hakkou, Rachid, Edström, Kristina, and Lippens, Pierre-Emmanuel

Abstract

The properties, insertion mechanisms, and electrochemical performances of the Na1.5Fe0.5Ti1.5(PO4)(3)/C composite as electrode material for Na-ion batteries are reported. The composite was obtained by solid-state reaction and consists of porous secondary particles of submicron-sized particles coated by carbon. Detailed characterizations were performed by combining theoretical and experimental tools. This includes the determination of the crystal structure of Na1.5Fe0.5Ti1.5(PO4)(3) from both first-principles calculations and X-ray diffraction providing Na distribution over M1 and M2 interstitial sites, which is of importance for ionic conductivity. Na1.5Fe0.5Ti1.5(PO4)(3)/C was used as an electrode material at 2.2 V versus Na+/Na-0, exhibiting good Na-storage ability with a specific capacity of 125 mAh g(-1), close to the theoretical value, for the first discharge at C/10, good capacity retention, and Coulombic efficiency of 95% and 99.5% at the 60th cycle, respectively, and high power rate with a decrease of the specific capacity of only 14% from C/10 to 2C. These good performances have been related to the morphology of the composite and substitution of Fe for Ti, leading to an insertion mechanism that differs from that of NaTi2(PO4)(3). This mechanism was quantitatively analyzed from operand Fe-57 Mossbauer spectroscopy used for the first time in both galvanostatic and GITT modes.

Published
2015
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39. Influence of relative humidity on the structure and electrochemical performance of sustainable LiFeSO4F electrodes for Li-ion batteries

Author

Zhang, Leiting, Tarascon, Jean-Marie, Sougrati, Moulay Tahar, Rousse, Gwenaelle, Chen, Guohua, Zhang, Leiting, Tarascon, Jean-Marie, Sougrati, Moulay Tahar, Rousse, Gwenaelle, and Chen, Guohua

Abstract

Material abundance and eco-efficient synthetic protocols are becoming the overriding factors for developing sustainable Li-ion batteries, and hence today there is great interest in LiFePO4. The recently reported tavorite-type LiFeSO4F cathode material, which shows a redox potential of 3.6 V and a practical capacity of similar to 130 mA h g-1 without the need for sophisticated carbon coating or particle downsizing, stands presently as a serious contender to LiFePO4. However, its synthesis is still not routinely reproducible. Herein, we offer a direct explanation by showing the strong effect of the room temperature relative humidity on both LiFeSO4F aging stability and its electrochemical performances. We demonstrate the complete degradation of tavorite-type LiFeSO4F into FeSO4 · nH2O (n = 1, 4, 7) and LiF in environments with relative humidities greater than 62%, and also show the feasibility of triggering in situ formation of a F--free (Li)FeSO4OH phase within the cell. This work, which we also extend to the 3.9 V triplite-type LiFeSO4F polymorph, provides a foundation for achieving the consistent production and handling of LiFeSO4F electrodes in view of large-scale manufacturing. This moisture sensitivity issue, which can be mitigated by surface treatments, is inherent to sulfate-based electrode materials and the battery community must be aware of it.

Published
2015

45. Study of the series Ti1−y Nb y SnSb with 0 ≤ y ≤ 1 as anode material for Li-ion batteries.

Author

Marino, Cyril, Sougrati, Moulay Tahar, Darwiche, A., Fullenwarth, Julien, Fraisse, Bernard, Jumas, Jean Claude, and Monconduit, Laure

Subjects
*LITHIUM-ion batteries, *TITANIUM alloys, *ANODES, *NEGATIVE electrode, *SUBSTITUTION reactions, *X-ray diffraction
Abstract

Abstract: TiSnSb shows an excellent behavior as negative electrode for Li-ion batteries. However the role of Ti is still unclear in the mechanism. To better understand the role played by the transition metal on both the mechanism and the performance of TiSnSb, a progressive substitution of Ti by Nb has been achieved. A full study focuses on the electrochemical mechanisms of the Ti1−y Nb y SnSb system with 0 ≤ y ≤ 1 vs Li by combining in situ XRD and Mössbauer, and EXAFS analyses. The electrochemical mechanism is found to be a reversible conversion mechanism: MSnSb + 7Li ↔ Li3Sb + 1/2 Li7Sn2 + M0. The lithium is found to react simultaneously with both Sn and Sb. Nb-rich alloys have been found also to be very promising negative electrode demonstrating the versatility of the MSnSb electrode material family for Li-ion battery application. Using the appropriate electrode formulation, the good cycling life of TiSnSb is not affected by its substitution by Nb. [Copyright &y& Elsevier]

Published
2013
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46. Investigating the Cycling Stability of Fe 2 WO 6 Pseudocapacitive Electrode Materials.

Author

Espinosa-Angeles, Julio César, Goubard-Bretesché, Nicolas, Quarez, Eric, Payen, Christophe, Sougrati, Moulay-Tahar, Crosnier, Olivier, and Brousse, Thierry

Subjects
SUPERCAPACITORS, MOSSBAUER spectroscopy, NEGATIVE electrode, SURFACE analysis, AQUEOUS electrolytes
Abstract

The stability upon cycling of Fe2WO6 used as a negative electrode material for electrochemical capacitors was investigated. The material was synthesized using low temperature conditions for the first time (220 °C). The electrochemical study of Fe2WO6 in a 5 M LiNO3 aqueous electrolyte led to a specific and volumetric capacitance of 38 F g−1 and 240 F cm−3 when cycled at 2 mV·s−1, respectively, associated with a minor capacitance loss after 10,000 cycles. In order to investigate this very good cycling stability, both surface and bulk characterization techniques (such as Transmission Electron Microscopy, Mössbauer spectroscopy, and magnetization measurements) were used. Only a slight disordering of the Fe3+ cations was observed in the structure, explaining the good stability of the Fe2WO6 upon cycling. This study adds another pseudocapacitive material to the short list of compounds that exhibit such a behavior up to now. [ABSTRACT FROM AUTHOR]

Published
2021
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47. Synthesis of Li2FeSiO4/carbon nano-composites by impregnation method.

Author

Sun, Shijiao, Matei Ghimbeu, Camelia, Vix-Guterl, Cathie, Sougrati, Moulay-Tahar, Masquelier, Christian, and Janot, Raphaël

Subjects
*NANOCRYSTALS, *CRYSTAL structure, *CARBON foams, *LITHIUM ions, *ELECTROCHEMISTRY, *NANOCOMPOSITE materials
Abstract

Nanocrystalline lithium iron silicate/carbon (Li 2 FeSiO 4 /C) composites were successfully prepared by impregnation of a commercial porous carbon using ethanolic solutions of the different metallic precursors, followed by thermal annealing at 600 °C. The effects of Li 2 FeSiO 4 loading content on the structure and organization of the Li 2 FeSiO 4 /C composites at the nanoscale were investigated. Through optimization of the synthesis conditions, small Li 2 FeSiO 4 nanocrystals (4–12 nm) are formed and well dispersed in the porous conductive carbon. The electrochemical performances of these composites were tested as positive electrodes for lithium-ion batteries. The Li 2 FeSiO 4 /C composite with the lowest Li 2 FeSiO 4 loading exhibits the best rate capability with a significant capacity contribution from carbon. It was found that the presence of carbon delays the lowering of the Fe 3+ /Fe 2+ redox voltage usually reported for Li 2 FeSiO 4 (from 3.1/3.0 to 2.8/2.7 V vs. Li + /Li), due to a stabilization effect of the initial Li 2 FeSiO 4 crystal structure. For the Li 2 FeSiO 4 /C composite (81/19 weight ratio), a discharge capacity of 81 mAh g −1 can be achieved at 55 °C for a charge/discharge rate of 2C, with 86% capacity retention after 500 cycles, showing the positive effect of the porous carbon addition for long term cycling stability. [ABSTRACT FROM AUTHOR]

Published
2015
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48. 2021 roadmap for sodium-ion batteries

Author

John T. S. Irvine, Emma Kendrick, Valerie R. Seymour, Aamod V. Desai, Edmund J. Cussen, Peter Gross, Andrew J. Naylor, Maria-Magdalena Titirici, Jake M. Brittain, Rebecca Boston, Ruth Sayers, Stewart A. M. Dickson, Sudeshna Sen, Sara I. R. Costa, Zhuangnan Li, Ashish Rudola, Heather Au, Dominic S. Wright, Nuria Tapia-Ruiz, Yongseok Choi, Hande Alptekin, John M. Griffin, Martin O. Jones, Marco Amores, Shahin Nikman, Eun Jeong Kim, A. Robert Armstrong, Reza Younesi, Maria Crespo Ribadeneyra, Laure Monconduit, William I. F. David, Christopher I Thomas, Patrik Johansson, Serena A. Cussen, Grant S. Stone, Jincheng Tong, Russell E. Morris, Clare P. Grey, Alexandre Ponrouch, Oleg Kolosov, Emmanuel I. Eweka, Darren M. C. Ould, Robert G. Palgrave, Thomas J. Wood, Yue Chen, Jerry Barker, Ronnie Mogensen, Stijn F. L. Mertens, Philippe Poizot, Juan Forero-Saboya, David O. Scanlon, Manish Chhowalla, Lorenzo Stievano, Emily M. Reynolds, Xiao Hua, Moulay Tahar Sougrati, William R. Brant, Martin Karlsmo, Stéven Renault, Christopher A. O’Keefe, Begoña Silván, Lancaster University, Harwell Science and Innovation Campus, Imperial College London, University of Sheffield [Sheffield], Faradion Limited, University of Virginia [Charlottesville], University of Oxford [Oxford], University of Cambridge [UK] (CAM), University College of London [London] (UCL), University of St Andrews [Scotland], AUTRES, Institut de Ciència de Materials de Barcelona (ICMAB-CSIC), Chalmers University of Technology [Gothenburg, Sweden], Science and Technology Facilities Council (STFC), University of Birmingham [Birmingham], Uppsala University, 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), Réseau sur le stockage électrochimique de l'énergie (RS2E), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Aix Marseille Université (AMU)-Université de Pau et des Pays de l'Adour (UPPA)-Université de Nantes (UN)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Institut des Matériaux Jean Rouxel (IMN), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN), Alistore, European Commission, Swedish Research Council, Swedish Energy Agency, Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning, Ministerio de Economía, Industria y Competitividad (España), Faraday Institution, Austrian Science Fund, Innovate UK, Tapia-Ruiz, Nuria [0000-0002-5005-7043], Armstrong, A Robert [0000-0003-1937-0936], Alptekin, Hande [0000-0001-6065-0513], Au, Heather [0000-0002-1652-2204], Barker, Jerry [0000-0002-8791-1119], Brant, William R [0000-0002-8658-8938], Choi, Yong-Seok [0000-0002-3737-2989], Costa, Sara I R [0000-0001-8105-207X], Crespo Ribadeneyra, Maria [0000-0001-6455-4430], Cussen, Serena A [0000-0002-9303-4220], Desai, Aamod V [0000-0001-7219-3428], Forero-Saboya, Juan D [0000-0002-3403-6066], Griffin, John M [0000-0002-8943-3835], Irvine, John T S [0000-0002-8394-3359], Johansson, Patrik [0000-0002-9907-117X], Karlsmo, Martin [0000-0002-0437-6860], Kendrick, Emma [0000-0002-4219-964X], Kolosov, Oleg V [0000-0003-3278-9643], Mertens, Stijn F L [0000-0002-5715-0486], Monconduit, Laure [0000-0003-3698-856X], Naylor, Andrew J [0000-0001-5641-7778], Poizot, Philippe [0000-0003-1865-4902], Renault, Stéven [0000-0002-6500-0015], Rudola, Ashish [0000-0001-9368-0698], Sayers, Ruth [0000-0003-1289-0998], Seymour, Valerie R [0000-0003-3333-5512], Silván, Begoña [0000-0002-1273-3098], Sougrati, Moulay Tahar [0000-0003-3740-2807], Stievano, Lorenzo [0000-0001-8548-0231], Thomas, Chris I [0000-0001-8090-4541], Titirici, Maria-Magdalena [0000-0003-0773-2100], Tong, Jincheng [0000-0001-7762-1460], Wood, Thomas J [0000-0002-5893-5664], Younesi, Reza [0000-0003-2538-8104], Apollo - University of Cambridge Repository, Kim, Eunjeong [0000-0002-2941-068], Kim, Eunjeong [0000-0002-2941-0682], University of Virginia, University of Oxford, 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), Université de Nantes (UN)-Aix Marseille Université (AMU)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Tapia-Ruiz, N [0000-0002-5005-7043], Armstrong, AR [0000-0003-1937-0936], Alptekin, H [0000-0001-6065-0513], Au, H [0000-0002-1652-2204], Barker, J [0000-0002-8791-1119], Brant, WR [0000-0002-8658-8938], Choi, YS [0000-0002-3737-2989], Costa, SIR [0000-0001-8105-207X], Ribadeneyra, MC [0000-0001-6455-4430], Cussen, SA [0000-0002-9303-4220], Desai, AV [0000-0001-7219-3428], Forero-Saboya, JD [0000-0002-3403-6066], Griffin, JM [0000-0002-8943-3835], Irvine, JTS [0000-0002-8394-3359], Johansson, P [0000-0002-9907-117X], Karlsmo, M [0000-0002-0437-6860], Kendrick, E [0000-0002-4219-964X], Kolosov, OV [0000-0003-3278-9643], Mertens, SFL [0000-0002-5715-0486], Monconduit, L [0000-0003-3698-856X], Naylor, AJ [0000-0001-5641-7778], Poizot, P [0000-0003-1865-4902], Renault, S [0000-0002-6500-0015], Rudola, A [0000-0001-9368-0698], Sayers, R [0000-0003-1289-0998], Seymour, VR [0000-0003-3333-5512], Silván, B [0000-0002-1273-3098], Sougrati, MT [0000-0003-3740-2807], Stievano, L [0000-0001-8548-0231], Thomas, CI [0000-0001-8090-4541], Titirici, MM [0000-0003-0773-2100], Tong, J [0000-0001-7762-1460], Wood, TJ [0000-0002-5893-5664], Younesi, R [0000-0003-2538-8104], The Faraday Institution, University of St Andrews. School of Chemistry, University of St Andrews. Centre for Energy Ethics, University of St Andrews. Centre for Designer Quantum Materials, and University of St Andrews. EaSTCHEM

Subjects
Chemical process, Technology, Computer science, PAIR DISTRIBUTION FUNCTION, HIGH-ENERGY DENSITY, ELECTROCHEMICAL PROPERTIES, Materialkemi, 02 engineering and technology, 01 natural sciences, 7. Clean energy, Materials Chemistry, QD, LITHIUM-ION, Energy demand, Scope (project management), anodes, NA2TI3O7 NANOSHEETS, [CHIM.MATE]Chemical Sciences/Material chemistry, sodium ion, 021001 nanoscience & nanotechnology, Variety (cybernetics), General Energy, Roadmap, T-DAS, Lithium, 0210 nano-technology, Battery (electricity), energy materials, Energy & Fuels, HIGH-CAPACITY ANODE, batteries, Materials Science (miscellaneous), Materials Science, chemistry.chemical_element, Materials Science, Multidisciplinary, electrolytes, 010402 general chemistry, Energy storage, MECHANISTIC INSIGHTS, SDG 7 - Affordable and Clean Energy, STRUCTURAL EVOLUTION, SOLID-ELECTROLYTE INTERPHASE, Science & Technology, QD Chemistry, 0104 chemical sciences, chemistry, 13. Climate action, Sustainability, HIGH-PERFORMANCE CATHODE, Biochemical engineering, cathodes
Abstract

Tapia-Ruiz, Nuria et al., Increasing concerns regarding the sustainability of lithium sources, due to their limited availability and consequent expected price increase, have raised awareness of the importance of developing alternative energy-storage candidates that can sustain the ever-growing energy demand. Furthermore, limitations on the availability of the transition metals used in the manufacturing of cathode materials, together with questionable mining practices, are driving development towards more sustainable elements. Given the uniformly high abundance and cost-effectiveness of sodium, as well as its very suitable redox potential (close to that of lithium), sodium-ion battery technology offers tremendous potential to be a counterpart to lithium-ion batteries (LIBs) in different application scenarios, such as stationary energy storage and low-cost vehicles. This potential is reflected by the major investments that are being made by industry in a wide variety of markets and in diverse material combinations. Despite the associated advantages of being a drop-in replacement for LIBs, there are remarkable differences in the physicochemical properties between sodium and lithium that give rise to different behaviours, for example, different coordination preferences in compounds, desolvation energies, or solubility of the solid–electrolyte interphase inorganic salt components. This demands a more detailed study of the underlying physical and chemical processes occurring in sodium-ion batteries and allows great scope for groundbreaking advances in the field, from lab-scale to scale-up. This roadmap provides an extensive review by experts in academia and industry of the current state of the art in 2021 and the different research directions and strategies currently underway to improve the performance of sodium-ion batteries. The aim is to provide an opinion with respect to the current challenges and opportunities, from the fundamental properties to the practical applications of this technology., The authors gratefully acknowledge RS2E and Alistore-ERI for funding their research into Na-ion batteries. The funding received from the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 646433 (NAIADES), the Swedish Research Council, the Swedish Energy Agency (#37671-1), and the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning (FORMAS), are all gratefully acknowledged. The many fruitful discussions within ALISTORE-ERI, and especially with M Rosa Palacín, have been most valuable. P J is also grateful for the continuous support from several of the Chalmers Areas of Advance: Materials Science and Energy. Funding from the European Union’s innovation program H2020 is acknowledged: H2020-MSCA-COFUND-2016 (DOC-FAM, Grant Agreement No. 754397). A Ponrouch is grateful to the Spanish Ministry for Economy, Industry and Competitiveness Severo Ochoa Programme for Centres of Excellence in R&D (SEV-2015-0496).

Published
2021
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