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Title: Reversible Conversion Reactions and Small First Cycle Irreversible Capacity Loss in Metal Sulfide-Based Electrodes Enabled by Solid Electrolytes

Abstract

Solid-state batteries can potentially enable new classes of electrode materials which are unstable against liquid electrolytes. Here, SnS nanocrystals, synthesized by a wet chemical method, are used to fabricate a Li-ion electrode, and the electrochemical properties of this electrode are examined in both solid and liquid electrolyte designs. The SnS-based solid-state cell delivers a capacity of 629 mAh g -1 after 100 cycles and exhibits an unprecedentedly small irreversible capacity in the first cycle (8.2%), while the SnS-based liquid cell shows a rapid capacity decay and large first cycle irreversible capacity (44.6%). Cyclic voltammetry (CV) experiments show significant solid electrolyte interphase (SEI) formation in the liquid cell during the first discharge while SEI formation by electrolyte reduction in the solid-state cell appears negligible. Along with CV, X-ray photoelectron spectroscopy and energy dispersive spectroscopy are used to investigate the differences between the solid-state and liquid cells. The reaction chemistry of SnS in solid-state cells is also studied in detail by ex situ X-ray diffraction and X-ray absorption spectroscopy. The overarching findings are that use of a solid electrolyte suppresses materials degradation and electrolyte reduction which leads to a small first cycle irreversible capacity and stable cycling.

Authors:
 [1];  [1]; ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [1]
  1. Univ. of Illinois, Urbana-Champaign, IL (United States). Beckman Inst. for Advanced Science and Technology, Materials Research Lab.
  2. Univ. of Illinois, Urbana-Champaign, IL (United States). Beckman Institute for Advanced Science and Technology, Materials Research Lab.
  3. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Materials Science and Engineering
  4. Univ. of Illinois, Urbana-Champaign, IL (United States). Materials Research Lab.
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1560010
Alternate Identifier(s):
OSTI ID: 1509945
Report Number(s):
BNL-212023-2019-JAAM
Journal ID: ISSN 1616-301X
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 27; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE

Citation Formats

Kim, Sanghyeon, Choi, Jaewon, Bak, Seong‐Min, Sang, Lingzi, Li, Qun, Patra, Arghya, and Braun, Paul V. Reversible Conversion Reactions and Small First Cycle Irreversible Capacity Loss in Metal Sulfide-Based Electrodes Enabled by Solid Electrolytes. United States: N. p., 2019. Web. doi:10.1002/adfm.201901719.
Kim, Sanghyeon, Choi, Jaewon, Bak, Seong‐Min, Sang, Lingzi, Li, Qun, Patra, Arghya, & Braun, Paul V. Reversible Conversion Reactions and Small First Cycle Irreversible Capacity Loss in Metal Sulfide-Based Electrodes Enabled by Solid Electrolytes. United States. doi:10.1002/adfm.201901719.
Kim, Sanghyeon, Choi, Jaewon, Bak, Seong‐Min, Sang, Lingzi, Li, Qun, Patra, Arghya, and Braun, Paul V. Mon . "Reversible Conversion Reactions and Small First Cycle Irreversible Capacity Loss in Metal Sulfide-Based Electrodes Enabled by Solid Electrolytes". United States. doi:10.1002/adfm.201901719.
@article{osti_1560010,
title = {Reversible Conversion Reactions and Small First Cycle Irreversible Capacity Loss in Metal Sulfide-Based Electrodes Enabled by Solid Electrolytes},
author = {Kim, Sanghyeon and Choi, Jaewon and Bak, Seong‐Min and Sang, Lingzi and Li, Qun and Patra, Arghya and Braun, Paul V.},
abstractNote = {Solid-state batteries can potentially enable new classes of electrode materials which are unstable against liquid electrolytes. Here, SnS nanocrystals, synthesized by a wet chemical method, are used to fabricate a Li-ion electrode, and the electrochemical properties of this electrode are examined in both solid and liquid electrolyte designs. The SnS-based solid-state cell delivers a capacity of 629 mAh g-1 after 100 cycles and exhibits an unprecedentedly small irreversible capacity in the first cycle (8.2%), while the SnS-based liquid cell shows a rapid capacity decay and large first cycle irreversible capacity (44.6%). Cyclic voltammetry (CV) experiments show significant solid electrolyte interphase (SEI) formation in the liquid cell during the first discharge while SEI formation by electrolyte reduction in the solid-state cell appears negligible. Along with CV, X-ray photoelectron spectroscopy and energy dispersive spectroscopy are used to investigate the differences between the solid-state and liquid cells. The reaction chemistry of SnS in solid-state cells is also studied in detail by ex situ X-ray diffraction and X-ray absorption spectroscopy. The overarching findings are that use of a solid electrolyte suppresses materials degradation and electrolyte reduction which leads to a small first cycle irreversible capacity and stable cycling.},
doi = {10.1002/adfm.201901719},
journal = {Advanced Functional Materials},
number = 27,
volume = 29,
place = {United States},
year = {2019},
month = {4}
}

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Works referenced in this record:

Electrochemical and In Situ X-Ray Diffraction Studies of the Reaction of Lithium with Tin Oxide Composites
journal, January 1997

  • Courtney, Ian A.; Dahn, J. R.
  • Journal of The Electrochemical Society, Vol. 144, Issue 6, p. 2045-2052
  • DOI: 10.1149/1.1837740