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Title: Mechanism of Formation of Li 7 P 3 S 11 Solid Electrolytes through Liquid Phase Synthesis

Abstract

Crystalline Li7P3S11 is a promising solid electrolyte for all solid state lithium/lithium ion batteries. A controllable liquid phase synthesis of Li7P3S11 is more desirable compared to conventional mechanochemical synthesis, but recent attempts suffer from reduced ionic conductivities. Here we elucidate the formation mechanism of crystalline Li7P3S11 synthesized in the liquid phase (acetonitrile, or ACN). We conclude that the crystalline Li7P3S11 forms through a two-step reaction: 1) formation of solid Li3PS4∙ACN and amorphous Li2S∙P2S5 phases in the liquid phase; 2) solid-state conversion of the two phases. The implication of this two-step reaction mechanism to the morphology control and the transport properties of liquid phase synthesized Li7P3S11 is identified and discussed.

Authors:
 [1]; ORCiD logo [1];  [2]; ORCiD logo [2]; ORCiD logo [2];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
  2. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1427919
Report Number(s):
PNNL-SA-130713
Journal ID: ISSN 0897-4756; 49321; 48379; VT1201000
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Chemistry of Materials; Journal Volume: 30; Journal Issue: 3
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Wang, Yuxing, Lu, Dongping, Bowden, Mark, El Khoury, Patrick Z., Han, Kee Sung, Deng, Zhiqun Daniel, Xiao, Jie, Zhang, Ji-Guang, and Liu, Jun. Mechanism of Formation of Li 7 P 3 S 11 Solid Electrolytes through Liquid Phase Synthesis. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.7b04842.
Wang, Yuxing, Lu, Dongping, Bowden, Mark, El Khoury, Patrick Z., Han, Kee Sung, Deng, Zhiqun Daniel, Xiao, Jie, Zhang, Ji-Guang, & Liu, Jun. Mechanism of Formation of Li 7 P 3 S 11 Solid Electrolytes through Liquid Phase Synthesis. United States. doi:10.1021/acs.chemmater.7b04842.
Wang, Yuxing, Lu, Dongping, Bowden, Mark, El Khoury, Patrick Z., Han, Kee Sung, Deng, Zhiqun Daniel, Xiao, Jie, Zhang, Ji-Guang, and Liu, Jun. Mon . "Mechanism of Formation of Li 7 P 3 S 11 Solid Electrolytes through Liquid Phase Synthesis". United States. doi:10.1021/acs.chemmater.7b04842.
@article{osti_1427919,
title = {Mechanism of Formation of Li 7 P 3 S 11 Solid Electrolytes through Liquid Phase Synthesis},
author = {Wang, Yuxing and Lu, Dongping and Bowden, Mark and El Khoury, Patrick Z. and Han, Kee Sung and Deng, Zhiqun Daniel and Xiao, Jie and Zhang, Ji-Guang and Liu, Jun},
abstractNote = {Crystalline Li7P3S11 is a promising solid electrolyte for all solid state lithium/lithium ion batteries. A controllable liquid phase synthesis of Li7P3S11 is more desirable compared to conventional mechanochemical synthesis, but recent attempts suffer from reduced ionic conductivities. Here we elucidate the formation mechanism of crystalline Li7P3S11 synthesized in the liquid phase (acetonitrile, or ACN). We conclude that the crystalline Li7P3S11 forms through a two-step reaction: 1) formation of solid Li3PS4∙ACN and amorphous Li2S∙P2S5 phases in the liquid phase; 2) solid-state conversion of the two phases. The implication of this two-step reaction mechanism to the morphology control and the transport properties of liquid phase synthesized Li7P3S11 is identified and discussed.},
doi = {10.1021/acs.chemmater.7b04842},
journal = {Chemistry of Materials},
number = 3,
volume = 30,
place = {United States},
year = {Mon Jan 22 00:00:00 EST 2018},
month = {Mon Jan 22 00:00:00 EST 2018}
}