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Title: Antisite occupation induced single anionic redox chemistry and structural stabilization of layered sodium chromium sulfide

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 all previous compounds involve a single cationic redox reaction or a cumulative cationic and anionic redox reaction. Here we report an anionic redox only chemistry and structural stabilization of layered sodium chromium sulfide. It is discovered that sulfur in sodium chromium sulfide is electrochemical active undergoing oxidation/reduction of sulfur 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. Here, our present work not only enriches the electrochemistry of layered intercalation compounds, but also extends the scope of investigation on high-capacity electrodes.

Authors:
 [1];  [2];  [3];  [3];  [2];  [4];  [4];  [4];  [3];  [2]
  1. Fudan Univ., Shanghai (People's Republic of China); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Fudan Univ., Shanghai (People's Republic of China)
  3. Shanghai Univ., Shanghai (People's Republic of China)
  4. Chinese Academy of Sciences, Beijing (People's Republic of China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1377061
Report Number(s):
BNL-114211-2017-JA
Journal ID: ISSN 2041-1723; R&D Project: MA453MAEA; VT1201000
Grant/Contract Number:
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; National Synchrotron Light Source

Citation Formats

Shadike, Zulipiya, Zhou, Yong -Ning, Chen, Lan -Li, Wu, Qu, Yue, Ji -Li, Zhang, Nian, Gu, Lin, Liu, Xiaosong, Shi, Si -Qi, and Fu, Zheng -Wen. Antisite occupation induced single anionic redox chemistry and structural stabilization of layered sodium chromium sulfide. United States: N. p., 2017. Web. doi:10.1038/s41467-017-00677-3.
Shadike, Zulipiya, Zhou, Yong -Ning, Chen, Lan -Li, Wu, Qu, Yue, Ji -Li, Zhang, Nian, Gu, Lin, Liu, Xiaosong, Shi, Si -Qi, & Fu, Zheng -Wen. Antisite occupation induced single anionic redox chemistry and structural stabilization of layered sodium chromium sulfide. United States. doi:10.1038/s41467-017-00677-3.
Shadike, Zulipiya, Zhou, Yong -Ning, Chen, Lan -Li, Wu, Qu, Yue, Ji -Li, Zhang, Nian, Gu, Lin, Liu, Xiaosong, Shi, Si -Qi, and Fu, Zheng -Wen. Wed . "Antisite occupation induced single anionic redox chemistry and structural stabilization of layered sodium chromium sulfide". United States. doi:10.1038/s41467-017-00677-3. https://www.osti.gov/servlets/purl/1377061.
@article{osti_1377061,
title = {Antisite occupation induced single anionic redox chemistry and structural stabilization of layered sodium chromium sulfide},
author = {Shadike, Zulipiya and Zhou, Yong -Ning and Chen, Lan -Li and Wu, Qu and Yue, Ji -Li and Zhang, Nian and Gu, Lin and Liu, Xiaosong and Shi, Si -Qi and Fu, Zheng -Wen},
abstractNote = {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 all previous compounds involve a single cationic redox reaction or a cumulative cationic and anionic redox reaction. Here we report an anionic redox only chemistry and structural stabilization of layered sodium chromium sulfide. It is discovered that sulfur in sodium chromium sulfide is electrochemical active undergoing oxidation/reduction of sulfur 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. Here, our present work not only enriches the electrochemistry of layered intercalation compounds, but also extends the scope of investigation on high-capacity electrodes.},
doi = {10.1038/s41467-017-00677-3},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {Wed Aug 30 00:00:00 EDT 2017},
month = {Wed Aug 30 00:00:00 EDT 2017}
}

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