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Title: Electrochemical Reaction Mechanism of the MoS 2 Electrode in a Lithium-Ion Cell Revealed by in Situ and Operando X-ray Absorption Spectroscopy

Abstract

As a typical transition metal dichalcogenide, MoS 2 offers numerous advantages for nanoelectronics and electrochemical energy storage due to its unique layered structure and tunable electronic properties. When used as the anode in lithium-ion cells, MoS 2 undergoes intercalation and conversion reactions in sequence upon lithiation, and the reversibility of the conversion reaction is an important but still controversial topic. Here, we clarify unambiguously that the conversion reaction of MoS 2 is not reversible, and the formed Li 2S is converted to sulfur in the first charge process. Li 2S/sulfur becomes the main redox couple in the subsequent cycles and the main contributor to the reversible capacity. In addition, due to the insulating nature of both Li 2S and sulfur, a strong relaxation effect is observed during the cycling process. This study clearly reveals the electrochemical lithiation-delithiation mechanism of MoS 2, which can facilitate further developments of high-performance MoS 2-based electrodes.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [3]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1530338
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 2; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Zhang, Liang, Sun, Dan, Kang, Jun, Feng, Jun, Bechtel, Hans A., Wang, Lin-Wang, Kang, Jun, and Guo, Jinghua. Electrochemical Reaction Mechanism of the MoS2 Electrode in a Lithium-Ion Cell Revealed by in Situ and Operando X-ray Absorption Spectroscopy. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.7b05246.
Zhang, Liang, Sun, Dan, Kang, Jun, Feng, Jun, Bechtel, Hans A., Wang, Lin-Wang, Kang, Jun, & Guo, Jinghua. Electrochemical Reaction Mechanism of the MoS2 Electrode in a Lithium-Ion Cell Revealed by in Situ and Operando X-ray Absorption Spectroscopy. United States. doi:10.1021/acs.nanolett.7b05246.
Zhang, Liang, Sun, Dan, Kang, Jun, Feng, Jun, Bechtel, Hans A., Wang, Lin-Wang, Kang, Jun, and Guo, Jinghua. Fri . "Electrochemical Reaction Mechanism of the MoS2 Electrode in a Lithium-Ion Cell Revealed by in Situ and Operando X-ray Absorption Spectroscopy". United States. doi:10.1021/acs.nanolett.7b05246. https://www.osti.gov/servlets/purl/1530338.
@article{osti_1530338,
title = {Electrochemical Reaction Mechanism of the MoS2 Electrode in a Lithium-Ion Cell Revealed by in Situ and Operando X-ray Absorption Spectroscopy},
author = {Zhang, Liang and Sun, Dan and Kang, Jun and Feng, Jun and Bechtel, Hans A. and Wang, Lin-Wang and Kang, Jun and Guo, Jinghua},
abstractNote = {As a typical transition metal dichalcogenide, MoS2 offers numerous advantages for nanoelectronics and electrochemical energy storage due to its unique layered structure and tunable electronic properties. When used as the anode in lithium-ion cells, MoS2 undergoes intercalation and conversion reactions in sequence upon lithiation, and the reversibility of the conversion reaction is an important but still controversial topic. Here, we clarify unambiguously that the conversion reaction of MoS2 is not reversible, and the formed Li2S is converted to sulfur in the first charge process. Li2S/sulfur becomes the main redox couple in the subsequent cycles and the main contributor to the reversible capacity. In addition, due to the insulating nature of both Li2S and sulfur, a strong relaxation effect is observed during the cycling process. This study clearly reveals the electrochemical lithiation-delithiation mechanism of MoS2, which can facilitate further developments of high-performance MoS2-based electrodes.},
doi = {10.1021/acs.nanolett.7b05246},
journal = {Nano Letters},
issn = {1530-6984},
number = 2,
volume = 18,
place = {United States},
year = {2018},
month = {1}
}

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Cited by: 8 works
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Figures / Tables:

Figure 1 Figure 1: Electrochemical characterization of the electrodes with different discharge cut-off voltages. (a) Discharge/charge voltage profiles, (b) cycling performance and Coulombic efficiency, and (c) cyclic voltammograms of MoS2 electrode with a discharge cut-off voltage of 0.8 V. (d) Discharge/charge voltage profiles, (e) cycling performance and Coulombic efficiency, and (f) cyclicmore » voltammograms of MoS2 electrode with a discharge cut-off voltage of 0.05 V.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.