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Abstract
The intercalation compounds with various electrochemically active or inactive elements in the layered structure have been the subject of increasing interest due to their high capacities, good reversibility, simple structures, and ease of synthesis. However, their reversible intercalation/deintercalation redox chemistries in previous compounds involve a single cationic redox reaction or a cumulative cationic and anionic redox reaction. Here we report an anionic redox chemistry and structural stabilization of layered sodium chromium sulfide. It was discovered that the sulfur in sodium chromium sulfide is electrochemically active, undergoing oxidation/reduction rather than chromium. Significantly, sodium ions can successfully move out and into without changing its lattice parameter c, which is explained in terms of the occurrence of chromium/sodium vacancy antisite during desodiation and sodiation processes. Our present work not only enriches the electrochemistry of layered intercalation compounds, but also extends the scope of investigation on high-capacity electrodes.
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Details
1 Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials, Department of Chemistry & Laser Chemistry Institute, Fudan University, Shanghai, China; Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA
2 Department of Material Science, Fudan University, Shanghai, China
3 School of Materials Science and Engineering, Shanghai University, Shanghai, China
4 Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials, Department of Chemistry & Laser Chemistry Institute, Fudan University, Shanghai, China
5 State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Science, Shanghai, China
6 Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China
7 School of Materials Science and Engineering, Shanghai University, Shanghai, China; Materials Genome Institute, Shanghai University, Shanghai, China