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1. Ultrafast Synthesis of Calcium Vanadate for Superior Aqueous Calcium-Ion Battery

Author

Liyuan Liu, Yih-Chyng Wu, Patrick Rozier, Pierre-Louis Taberna, and Patrice Simon

Subjects
Science
Abstract

Recently, multivalent aqueous calcium-ion batteries (CIBs) have attracted considerable attention as a possible alternative to Li-ion batteries. However, traditional Ca-ion storage materials show either limited rate capabilities and poor cycle life or insufficient specific capacity. Here, we tackle these limitations by exploring materials having a large interlayer distance to achieve decent specific capacities and one-dimensional architecture with adequate Ca-ion passages that enable rapid reversible (de)intercalation processes. In this work, we report the high-yield, rapid, and low-cost synthesis of 1D metal oxides MV3O8 (M=Li, K), CaV2O6, and CaV6O16·7H2O (CVO) via a molten salt method. Firstly, using 1D CVO as electrode materials, we show high capacity 205 mA h g-1, long cycle life (>97% capacity retention after 200 cycles at 3.0 C), and high-rate performance (117 mA h g-1 at 12 C) for Ca-ion (de)intercalation. This work represents a step forward for the development of the molten salt method to synthesize nanomaterials and to help pave the way for the future growth of Ca-ion batteries.

Published
2019
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2. Unraveling the Capacitive Charge Storage Mechanism of Nitrogen-Doped Porous Carbons by EQCM and ssNMR

Author

En Zhang, Yih-Chyng Wu, Hui Shao, Vytautas Klimavicius, Hanyue Zhang, Pierre-Louis Taberna, Julia Grothe, Gerd Buntkowsky, Fei Xu, Patrice Simon, Stefan Kaskel, Publica, Technische Universität Dresden = Dresden University of Technology (TU Dresden), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), Réseau sur le stockage électrochimique de l'énergie (RS2E), Aix Marseille Université (AMU)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Nantes Université (Nantes Univ)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), Vilnius University [Vilnius], Technische Universität Darmstadt - Technical University of Darmstadt (TU Darmstadt), Fraunhofer Institute Material and Beam Technology [Dresden] (Fraunhofer IWS), Fraunhofer (Fraunhofer-Gesellschaft), and German Science Foundation (Deutsche Forschungsgemeinschaft, grants no. KA 1698/27-1)

Subjects
Ions, X-ray photoelectron spectroscopy, Magnetic Resonance Spectroscopy, Nitrogen, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Lithium, Biochemistry, Catalysis, Carbon, Colloid and Surface Chemistry, Cations, Electrical properties, Quartz Crystal Microbalance Techniques, [CHIM.OTHE]Chemical Sciences/Other, Electrodes, Porosity, Nuclear magnetic resonance spectroscopy
Abstract

International audience; Fundamental understanding of ion electroadsorption processes in porous electrodes on a molecular level provides important guidelines for next-generation energy storage devices like electric double layer capacitors (EDLCs). Porous carbons functionalized by heteroatoms show enhanced capacitive performance, but the underlying mechanism is still elusive, due to the lack of reliable tools to precisely identify multiple N species and establish clear structure property relations. Here, we use advanced analytical techniques such as lowtemperature solid-state NMR (ssNMR) and electrochemical quartz crystal microbalance (EQCM) to relate the complex nitrogen functionalities to the charging mechanisms and capacitive performance. For the first time, it is demonstrated at a molecular level that N-doping strongly influences the electroadsorption mechanism in EDLCs. Without N-doping, anion (SO 4 2−) adsorption−desorption dominates the charging mechanism, whereas after doping, Li + electroadsorption plays a key role. With the help of EQCM, it is demonstrated that SO 4 2− is strongly immobilized on the Ndoped surface, leaving Li + as the main charge carrier. The smaller size and higher concentration of Li + compared to SO 4 2− benefit a higher capacitance. Amine/amide N is responsible for high capacitance, but surprisingly the pyridinic, pyrrolic, and graphitic N groups have no significant influence. 2D 1 H-15 N NMR spectroscopy indicates that the conversion from pyridinium to pyrrolic N gives rise to a slightly decreased capacitance. This work not only demonstrates ssNMR as a powerful tool for surface chemistry characterization of electrode materials but also uncovers the related charging mechanism by EQCM, paving the way toward a comprehensive picture of EDLC chemistry.

Published
2022
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3. Electrochemical Characterization of Single Layer Graphene/Electrolyte Interface: Effect of Solvent on the Interfacial Capacitance

Author

Yih‐Chyng Wu, Jianglin Ye, Gengping Jiang, Kun Ni, Na Shu, Pierre‐Louis Taberna, Yanwu Zhu, Patrice Simon, University of Science and Technology of China [Hefei] (USTC), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), 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), Wuhan University of Science and Technology, and Collaborative Innovation Center of Chemistry for Energy Materials (iCHEM), Department of Chemistry, University of Science and Technology of China (iCHEM)

Subjects
electrode/electrolyte interface, Supercapacitors | Hot Paper, charge storage, graphene, 02 engineering and technology, General Medicine, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, electrochemical quartz crystal microbalance, 0104 chemical sciences, [CHIM]Chemical Sciences, supercapacitor, 0210 nano-technology, Research Articles, Research Article
Abstract

The development of the basic understanding of the charge storage mechanisms in electrodes for energy storage applications needs deep characterization of the electrode/electrolyte interface. In this work, we studied the charge of the double layer capacitance at single layer graphene (SLG) electrode used as a model material, in neat (EMIm‐TFSI) and solvated (with acetonitrile) ionic liquid electrodes. The combination of electrochemical impedance spectroscopy and gravimetric electrochemical quartz crystal microbalance (EQCM) measurements evidence that the presence of solvent drastically increases the charge carrier density at the SLG/ionic liquid interface. The capacitance is thus governed not only by the electronic properties of the graphene, but also by the specific organization of the electrolyte side at the SLG surface originating from the strong interactions existing between the EMIm+ cations and SLG surface. EQCM measurements also show that the carbon structure, with the presence of sp2 carbons, affects the charge storage mechanism by favoring counter‐ion adsorption on SLG electrode versus ion exchange mechanism in amorphous porous carbons., The charge of the double layer capacitance at a single layer graphene (SLG) electrode was studied in neat (EMIm‐TFSI) and solvated (with acetonitrile) ionic liquid electrodes. Electrochemical impedance spectroscopy and gravimetric electrochemical quartz crystal microbalance measurements evidence that the presence of solvent drastically increases the charge carrier density at the SLG/ionic liquid interface.

Published
2021
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5. Unraveling the Charge Storage Mechanism of Ti3C2Tx MXene Electrode in Acidic Electrolyte

Author

Kui Xu, Hui Shao, Liyuan Liu, Liangti Qu, Yih-Chyng Wu, Patrice Simon, Zifeng Lin, Antonella Iadecola, Encarnacion Raymundo-Piñero, Jixin Zhu, Hongyun Ma, Pierre-Louis Taberna, Centre National de la Recherche Scientifique - CNRS (FRANCE), Collège de France (FRANCE), Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE), Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE), Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE), Institut polytechnique de Grenoble (FRANCE), Université Paris Sciences & Lettres - PSL (FRANCE), Sichuan University - SCU (CHINA), Sorbonne Université (FRANCE), Université Grenoble Alpes - UGA (FRANCE), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Université de Nantes (FRANCE), Université de Picardie Jules Verne (FRANCE), Nanjing Tech University (CHINA), Tsinghua University (CHINA), Université de Pau et des Pays de l'Adour - UPPA (FRANCE), Université de Haute Alsace - UHA (FRANCE), Conditions Extrêmes et Matériaux : Haute Température et Irradiation - CEMHTI (Orléans, France), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-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), Tsinghua University [Beijing] (THU), Conditions Extrêmes et Matériaux : Haute Température et Irradiation (CEMHTI), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université d'Orléans (UO), Sichuan University [Chengdu] (SCU), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), 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), and Université d'Orléans (UO)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Matériaux, Energy Engineering and Power Technology, 02 engineering and technology, Electrolyte, 010402 general chemistry, 01 natural sciences, Redox, Electrolytes, Two dimensional materials, Proton transport, Materials Chemistry, Molecule, Electrodes, Electrode material, Renewable Energy, Sustainability and the Environment, Charge (physics), [CHIM.MATE]Chemical Sciences/Material chemistry, Molecules, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Fuel Technology, Chemical engineering, Chemistry (miscellaneous), Electrode, 0210 nano-technology, MXenes, [CHIM.OTHE]Chemical Sciences/Other, Layers
Abstract

International audience; Two-dimensional Ti3C2Tx MXenes have been extensively studied as pseudocapacitive electrode materials. This Letter aims at providing further insights into the charge storage mechanism of the Ti3C2Tx MXene electrode in the acidic electrolyte by combining experimental and simulation approaches. Our results show that the presence of H2O molecules between the MXene layers plays a critical role in the pseudocapacitive behavior, providing a pathway for proton transport to activate the redox reaction of the Ti atoms. Also, thermal annealing of the samples at different temperatures suggests that the presence of the confined H2O molecules is mainly controlled by the surface termination groups. These findings pave the way for alternative strategies to enhance the high-rate performance of MXenes electrodes by optimizing their surface termination groups.

Published
2020
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6. Nanoporous carbon for electrochemical capacitive energy storage

Author

Patrice Simon, Zifeng Lin, Yih-Chyng Wu, Pierre-Louis Taberna, Hui Shao, Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-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), Sichuan University - SCU (CHINA), IUF, Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), 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), Centre National de la Recherche Scientifique - CNRS (FRANCE), Collège de France (FRANCE), Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE), Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE), Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE), Institut polytechnique de Grenoble (FRANCE), Institut universitaire de France - IUF (FRANCE), Université Paris Sciences & Lettres - PSL (FRANCE), Sorbonne Université (FRANCE), Université Grenoble Alpes - UGA (FRANCE), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Université de Nantes (FRANCE), Université de Picardie Jules Verne (FRANCE), Université de Pau et des Pays de l'Adour - UPPA (FRANCE), and Université de Haute Alsace - UHA (FRANCE)

Subjects
Energie électrique, Carbone, Materials science, Matériaux, chemistry.chemical_element, Nanotechnology, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, Double layer (biology), Nanoporous, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Characterization (materials science), Electrochimie, Nanopore, chemistry, Electrode, 0210 nano-technology, Carbon, Stockage capactif, Energie
Abstract

International audience; The urgent need for efficient energy storage devices has stimulated a great deal of research on electrochemical double layer capacitors (EDLCs). This review aims at summarizing the recent progress in nanoporous carbons, as the most commonly used EDLC electrode materials in the field of capacitive energy storage, from the viewpoint of materials science and characterization techniques. We discuss the key advances in the fundamental understanding of the charge storage mechanism in nanoporous carbon-based electrodes, including the double layer formation in confined nanopores. Special attention will be also paid to the important development of advanced in situ analytical techniques as well as theoretical studies to better understand the carbon pore structure, electrolyte ion environment and ion fluxes in these confined pores. We also highlight the recent progress in advanced electrolytes for EDLCs. The better understanding of the charge storage mechanism of nanoporous carbon-based electrodes and the rational design of electrolytes should shed light on developing the next-generation of EDLCs.

Published
2020
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7. Ultrafast Synthesis of Calcium Vanadate for Superior Aqueous Calcium-Ion Battery

Author

Yih-Chyng Wu, Patrice Simon, Pierre-Louis Taberna, Patrick Rozier, Liyuan Liu, Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), 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), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC), 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), Centre National de la Recherche Scientifique - CNRS (FRANCE), Collège de France (FRANCE), Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE), Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE), Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE), Institut polytechnique de Grenoble (FRANCE), Université Paris Sciences & Lettres - PSL (FRANCE), Sorbonne Université (FRANCE), Université Grenoble Alpes - UGA (FRANCE), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Université de Nantes (FRANCE), Université de Picardie Jules Verne (FRANCE), Université de Pau et des Pays de l'Adour - UPPA (FRANCE), and Université de Haute Alsace - UHA (FRANCE)

Subjects
Battery (electricity), Long cycle, Energie électrique, Materials science, Matériaux, Science, Intercalation (chemistry), chemistry.chemical_element, Nanotechnology, 02 engineering and technology, Calcium, 010402 general chemistry, 01 natural sciences, Nanomaterials, Vanadate, Molten salt, Multidisciplinary, Aqueous solution, Traitements de Surface, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, Revetements, 0210 nano-technology, Traitements de Surface -Superior Aqueous Calcium-Ion Battery, Research Article
Abstract

Recently, multivalent aqueous calcium-ion batteries (CIBs) have attracted considerable attention as a possible alternative to Li-ion batteries. However, traditional Ca-ion storage materials show either limited rate capabilities and poor cycle life or insufficient specific capacity. Here, we tackle these limitations by exploring materials having a large interlayer distance to achieve decent specific capacities and one-dimensional architecture with adequate Ca-ion passages that enable rapid reversible (de)intercalation processes. In this work, we report the high-yield, rapid, and low-cost synthesis of 1D metal oxides M V 3 O 8 ( M = Li , K), CaV 2 O 6 , and CaV 6 O 16 ·7H 2 O (CVO) via a molten salt method. Firstly, using 1D CVO as electrode materials, we show high capacity 205 mA h g -1 , long cycle life (>97% capacity retention after 200 cycles at 3.0 C), and high-rate performance (117 mA h g -1 at 12 C) for Ca-ion (de)intercalation. This work represents a step forward for the development of the molten salt method to synthesize nanomaterials and to help pave the way for the future growth of Ca-ion batteries.

Published
2019
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8. Charge Storage Mechanisms of Single-Layer Graphene in Ionic Liquid

Author

Na Shu, Yanwu Zhu, Jianglin Ye, Kui Xu, Yih-Chyng Wu, Patrice Simon, Kun Ni, Pierre-Louis Taberna, University of Science and Technology of China [Hefei] (USTC), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), 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), Aix-Marseille Université - AMU (FRANCE), Centre National de la Recherche Scientifique - CNRS (FRANCE), Collège de France (FRANCE), Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE), Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE), Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE), Institut polytechnique de Grenoble (FRANCE), Sorbonne Université (FRANCE), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Université de Nantes (FRANCE), Université de Picardie Jules Verne (FRANCE), Université de Pau et des Pays de l'Adour - UPPA (FRANCE), Université de Haute Alsace - UHA (FRANCE), Université de Montpellier (FRANCE), University of Science and Technology of China - USTC (CHINA), Centre Interuniversitaire de Recherche et d'Ingénierie des Matériaux - CIRIMAT (Toulouse, France), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC), 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), and Institut National Polytechnique de Toulouse - INPT (FRANCE)

Subjects
Energie électrique, Matériaux, Interfaces, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, Biochemistry, Capacitance, Catalysis, law.invention, Ion, [SPI.MAT]Engineering Sciences [physics]/Materials, chemistry.chemical_compound, Colloid and Surface Chemistry, law, Two dimensional materials, Electrodes, Ions, Graphene, [SPI.NRJ]Engineering Sciences [physics]/Electric power, General Chemistry, Quartz crystal microbalance, 0104 chemical sciences, Dielectric spectroscopy, chemistry, Chemical engineering, Ionic liquid, Electrical properties
Abstract

International audience; Graphene-based carbon materials are promising candidates for electrical double-layer (EDL) capacitors, and there is considerable interest in understanding the structure and properties of the graphene/electrolyte interface. Here, electrochemical impedance spectroscopy (EIS) and electrochemical quartz crystal microbalance (EQCM) are used to characterize the ion fluxes and adsorption on single-layer graphene in neat ionic liquid (EMI-TFSI) electrolyte. It is found that a positively charged ion-species desorption and ion reorganization dominate the double-layer charging during positive and negative polarizations, respectively, leading to the increase in EDL capacitance with applied potential.

Published
2019
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9. Back Cover: Electrochemical Characterization of Single Layer Graphene/Electrolyte Interface: Effect of Solvent on the Interfacial Capacitance (Angew. Chem. Int. Ed. 24/2021)

Author

Yih-Chyng Wu, Pierre-Louis Taberna, Na Shu, Gengping Jiang, Kun Ni, Patrice Simon, Jianglin Ye, and Yanwu Zhu

Subjects
Supercapacitor, Materials science, Graphene, Interfacial capacitance, General Chemistry, Electrolyte, Electrochemistry, Catalysis, law.invention, Characterization (materials science), Solvent, Chemical engineering, law, Single layer graphene
Published
2021
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10. Rücktitelbild: Electrochemical Characterization of Single Layer Graphene/Electrolyte Interface: Effect of Solvent on the Interfacial Capacitance (Angew. Chem. 24/2021)

Author

Patrice Simon, Pierre-Louis Taberna, Yanwu Zhu, Jianglin Ye, Na Shu, Kun Ni, Yih-Chyng Wu, and Gengping Jiang

Subjects
Supercapacitor, Solvent, Materials science, Chemical engineering, Graphene, law, Interface (computing), Single layer graphene, General Medicine, Electrolyte, Electrochemistry, law.invention, Characterization (materials science)
Published
2021
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11. Tracking ionic fluxes in porous carbon electrodes from aqueous electrolyte mixture at various pH

Author

Pierre-Louis Taberna, Patrice Simon, Yih-Chyng Wu, Centre National de la Recherche Scientifique - CNRS (FRANCE), Collège de France (FRANCE), Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE), Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE), Institut National Polytechnique de Toulouse - INPT (FRANCE), Institut polytechnique de Grenoble (FRANCE), Sorbonne Université (FRANCE), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Université de Nantes (FRANCE), Université de Picardie Jules Verne (FRANCE), Université de Pau et des Pays de l'Adour - UPPA (FRANCE), Université de Haute Alsace - UHA (FRANCE), Université de Montpellier (FRANCE), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), 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), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC), 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), and Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE)

Subjects
Energie électrique, Materials science, Energy storage, Matériaux, Inorganic chemistry, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, Ion, [SPI.MAT]Engineering Sciences [physics]/Materials, lcsh:Chemistry, Adsorption, Microporous carbon, Ion dynamics, Electrochemical quartz crystal microbalance, Polarization (electrochemistry), Supercapacitor, Aqueous solution, [SPI.NRJ]Engineering Sciences [physics]/Electric power, Quartz crystal microbalance, 021001 nanoscience & nanotechnology, 0104 chemical sciences, lcsh:Industrial electrochemistry, lcsh:QD1-999, Cyclic voltammetry, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other, lcsh:TP250-261
Abstract

Electrochemical quartz crystal microbalance (EQCM) and cyclic voltammetry (CV) techniques were used to study ion dynamics in porous carbide-derived carbon (CDC) electrodes in various aqueous electrolytes. Although the cyclic voltammetries look similar, EQCM revealed different ion transfer depending on the electrolyte during both positive and negative polarization. During polarization in neutral K2SO4 electrolyte, partial desolvation of cation and anion were observed in carbon micropores. In EMI+-HSO4− electrolyte, the main charge carrier during cation adsorption was not found to be bulkier EMI+, but smaller and highly mobile H+. Furthermore, ionic fluxes during charging/discharging were monitored and identified in multi-ions aqueous system, which was ambiguous according to the CV plots. EQCM shows its powerful ability to serve as an accurate gravimetry probe to study the electrolyte concentration and compositional changes in porous materials. Keywords: Electrochemical quartz crystal microbalance, Supercapacitor, Microporous carbon, Ion dynamics, Energy storage

Published
2018
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12. (Invited) Study of Ion Adsorption-Transfer Mechanisms in Nanoporous Carbon Electrodes: Application to Supercapacitors

Author

Yih-Chyng Wu, Wan-Yu Tsai, Patrice Simon, and Pierre-Louis Taberna

Abstract

Research into the design of electrolytes of ionic liquids (ILs) for supercapacitor applications has grown in popularity in recent years. Unlike Li batteries where the composition of the electrolyte and the stability must meet several requirements (formation of SEI, electrochemical kinetics), the use of ionic liquids in supercapacitors opens interesting perspectives, in particular thanks to their high electrochemical stability. [1]. In this communication, it will be presented the results of an experimental study conducted using quartz crystal microbalance (eQCM) on nanoporous carbon based electrodes in contact with different electrolytes : neat IL and solvated IL as well as electrolyte mixture. EQCM turns out to be an effective analytic tool to bring new insights regarding the charge compensation mechanisms occurring while polarizing the carbon based electrode. In particular, it will be shown that charge compensation can involve different levels of desolvation of the counter-ions and that co-ions can also be used when the carbon electrode is polarized [2,3,4]. Références : [1] P. Simon et Y. Gogotsi, Nature Materials, 7 (2008) 845-854. [2] W.-Y. Tsai et al. JACS 8722−8728 (2014) [3] J. Griffin et al., Nature Materials, 22 juin 2015 (doi: 10.1038 / nmat4318). [4] Y.-C. Wu, P.-L. Taberna, P. Simon, Communications en électrochimie. 93, 119-122 (2018).

Published
2019
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14. ZnO nanoparticle based highly efficient CdS/CdSe quantum dot-sensitized solar cells

Author

Martin Søndergaard, Qingbo Meng, Chunhui Li, Dongmei Li, Yanhong Luo, Junyan Xiao, Bo B. Iversen, Yih-Chyng Wu, and Lei Yang

Subjects
Materials science, business.industry, Energy conversion efficiency, General Physics and Astronomy, Nanotechnology, Sulfides, Quantum dot solar cell, Electric Power Supplies, Zno nanoparticles, Quantum dot, Quantum Dots, Cadmium Compounds, Solar Energy, Nanoparticles, Optoelectronics, Zinc Oxide, Physical and Theoretical Chemistry, Selenium Compounds, Mesoporous material, business
Abstract

20 nm ZnO nanoparticles are used to fabricate the mesoporous photoanode of the CdS/CdSe quantum dot-sensitized solar cells by the simple doctor blade method. A maximum power conversion efficiency of 4.46% has been achieved, which indicated exciting prospects for ZnO nanoparticle based quantum dot-sensitized solar cells.

Published
2013
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