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Title: Understanding the electrochemical reaction mechanism of VS2 nanosheets in lithium-ion cells by multiple in situ and ex situ x-ray spectroscopy

Abstract

Recently, 2D layered transition metal dichalcogenides (TMDs) have attracted great scientific interest in electrochemical energy storage research. Vanadium disulfide (VS2) as an important family member of TMDs, is a promising electrode material for lithium-ion cells because of its remarkable electrical conductivity and high Li+ diffusion rate, but its electrochemical reaction mechanism is still poorly understood. Herein, we have prepared VS2 nanosheets as the electrode and systematically investigated its structural and chemical evolution during the electrochemical processes by employing both in situ and ex situ x-ray spectroscopy. The VS2 undergoes intercalation and conversion reactions in sequence during discharge and this process is found to be partially reversible during the subsequent charge. The decreased reversibility of the conversion reaction over extended cycles could be mainly responsible for the capacity fading of the VS2 electrode. Furthermore, the hybridization strength between S and V shows a strong dependence on the states of charge, as directly illustrated by the intensity change of the V-S hybridized states and pure V states. We have additionally found that the solid electrolyte interphase on the electrode surface is dynamically evolved during cycling, which may be a universal phenomenon for the conversion-based electrodes. Our research is expected to be beneficialmore » for the further development of high-performance VS2-based electrodes.« less

Authors:
ORCiD logo [1];  [1];  [2];  [3];  [1];  [3]; ORCiD logo [4];  [5]; ORCiD logo [6]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Los Angeles, CA (United States)
  3. Univ. of Science and Technology of China, Hefei (China)
  4. Wuhan Univ. of Technology (China). State Key Lab. of Advanced Technology for Materials Synthesis and Processing
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1542316
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. D, Applied Physics
Additional Journal Information:
Journal Volume: 51; Journal Issue: 49; Journal ID: ISSN 0022-3727
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Zhang, Liang, Sun, Dan, Wei, Qiulong, Ju, Huanxin, Feng, Jun, Zhu, Junfa, Mai, Liqiang, Cairns, Elton J., and Guo, Jinghua. Understanding the electrochemical reaction mechanism of VS2 nanosheets in lithium-ion cells by multiple in situ and ex situ x-ray spectroscopy. United States: N. p., 2018. Web. doi:10.1088/1361-6463/aadde7.
Zhang, Liang, Sun, Dan, Wei, Qiulong, Ju, Huanxin, Feng, Jun, Zhu, Junfa, Mai, Liqiang, Cairns, Elton J., & Guo, Jinghua. Understanding the electrochemical reaction mechanism of VS2 nanosheets in lithium-ion cells by multiple in situ and ex situ x-ray spectroscopy. United States. https://doi.org/10.1088/1361-6463/aadde7
Zhang, Liang, Sun, Dan, Wei, Qiulong, Ju, Huanxin, Feng, Jun, Zhu, Junfa, Mai, Liqiang, Cairns, Elton J., and Guo, Jinghua. Mon . "Understanding the electrochemical reaction mechanism of VS2 nanosheets in lithium-ion cells by multiple in situ and ex situ x-ray spectroscopy". United States. https://doi.org/10.1088/1361-6463/aadde7. https://www.osti.gov/servlets/purl/1542316.
@article{osti_1542316,
title = {Understanding the electrochemical reaction mechanism of VS2 nanosheets in lithium-ion cells by multiple in situ and ex situ x-ray spectroscopy},
author = {Zhang, Liang and Sun, Dan and Wei, Qiulong and Ju, Huanxin and Feng, Jun and Zhu, Junfa and Mai, Liqiang and Cairns, Elton J. and Guo, Jinghua},
abstractNote = {Recently, 2D layered transition metal dichalcogenides (TMDs) have attracted great scientific interest in electrochemical energy storage research. Vanadium disulfide (VS2) as an important family member of TMDs, is a promising electrode material for lithium-ion cells because of its remarkable electrical conductivity and high Li+ diffusion rate, but its electrochemical reaction mechanism is still poorly understood. Herein, we have prepared VS2 nanosheets as the electrode and systematically investigated its structural and chemical evolution during the electrochemical processes by employing both in situ and ex situ x-ray spectroscopy. The VS2 undergoes intercalation and conversion reactions in sequence during discharge and this process is found to be partially reversible during the subsequent charge. The decreased reversibility of the conversion reaction over extended cycles could be mainly responsible for the capacity fading of the VS2 electrode. Furthermore, the hybridization strength between S and V shows a strong dependence on the states of charge, as directly illustrated by the intensity change of the V-S hybridized states and pure V states. We have additionally found that the solid electrolyte interphase on the electrode surface is dynamically evolved during cycling, which may be a universal phenomenon for the conversion-based electrodes. Our research is expected to be beneficial for the further development of high-performance VS2-based electrodes.},
doi = {10.1088/1361-6463/aadde7},
journal = {Journal of Physics. D, Applied Physics},
number = 49,
volume = 51,
place = {United States},
year = {Mon Sep 17 00:00:00 EDT 2018},
month = {Mon Sep 17 00:00:00 EDT 2018}
}

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