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Title: Interfacial Reactions and Performance of Li7La3Zr2O12-Stabilized Li–Sulfur Hybrid Cell

Abstract

Herein, we report on the characterization of a Li–S hybrid cell containing a garnet solid electrolyte (Li7La3Zr2O12, LLZO) and conventional liquid electrolyte. While the liquid electrolyte provided ionically conductive pathways throughout the porous cathode, the LLZO acted as a physical barrier to protect the Li metal anode and prevent polysulfide shuttling during battery operation. This hybrid cell exhibited an initial capacity of 1000 mAh/g(S) and high Coulombic efficiency (>99%). The interface between the liquid electrolyte and LLZO was studied using electrochemical impedance spectroscopy and X-ray photoelectron spectroscopy (XPS). These results indicate that a spontaneous interfacial reaction layer formed between the LLZO and liquid electrolyte. XPS depth profiling experiments indicate that this layer consisted of Li-enriched phases near the surface (e.g., Li2CO3) and intermediate Li–La–Zr oxides in subsurface regions. The reaction layer extended well beyond the LLZO surface, and bulk pristine LLZO was not observed even at the deepest sputtering depths used in this study (~90 nm). Overall, these results highlight that developing stable electrode/electrolyte interfaces is critical for solid-state batteries and their hybrids.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3];  [4];  [2]; ORCiD logo [3]
  1. Tulane Univ., New Orleans, LA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Mechanical Engineering and Macromolecular Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1606766
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 45; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Liquids; Layers; Electrodes; Electrochemical cells; Electrolytes; hybrid cell; LLZO; electrolyte; Li−S battery

Citation Formats

Naguib, Michael, Sharafi, Asma, Self, Ethan C., Meyer, Harry M., Sakamoto, Jeff, and Nanda, Jagjit. Interfacial Reactions and Performance of Li7La3Zr2O12-Stabilized Li–Sulfur Hybrid Cell. United States: N. p., 2019. Web. doi:10.1021/acsami.9b11439.
Naguib, Michael, Sharafi, Asma, Self, Ethan C., Meyer, Harry M., Sakamoto, Jeff, & Nanda, Jagjit. Interfacial Reactions and Performance of Li7La3Zr2O12-Stabilized Li–Sulfur Hybrid Cell. United States. doi:10.1021/acsami.9b11439.
Naguib, Michael, Sharafi, Asma, Self, Ethan C., Meyer, Harry M., Sakamoto, Jeff, and Nanda, Jagjit. Wed . "Interfacial Reactions and Performance of Li7La3Zr2O12-Stabilized Li–Sulfur Hybrid Cell". United States. doi:10.1021/acsami.9b11439.
@article{osti_1606766,
title = {Interfacial Reactions and Performance of Li7La3Zr2O12-Stabilized Li–Sulfur Hybrid Cell},
author = {Naguib, Michael and Sharafi, Asma and Self, Ethan C. and Meyer, Harry M. and Sakamoto, Jeff and Nanda, Jagjit},
abstractNote = {Herein, we report on the characterization of a Li–S hybrid cell containing a garnet solid electrolyte (Li7La3Zr2O12, LLZO) and conventional liquid electrolyte. While the liquid electrolyte provided ionically conductive pathways throughout the porous cathode, the LLZO acted as a physical barrier to protect the Li metal anode and prevent polysulfide shuttling during battery operation. This hybrid cell exhibited an initial capacity of 1000 mAh/g(S) and high Coulombic efficiency (>99%). The interface between the liquid electrolyte and LLZO was studied using electrochemical impedance spectroscopy and X-ray photoelectron spectroscopy (XPS). These results indicate that a spontaneous interfacial reaction layer formed between the LLZO and liquid electrolyte. XPS depth profiling experiments indicate that this layer consisted of Li-enriched phases near the surface (e.g., Li2CO3) and intermediate Li–La–Zr oxides in subsurface regions. The reaction layer extended well beyond the LLZO surface, and bulk pristine LLZO was not observed even at the deepest sputtering depths used in this study (~90 nm). Overall, these results highlight that developing stable electrode/electrolyte interfaces is critical for solid-state batteries and their hybrids.},
doi = {10.1021/acsami.9b11439},
journal = {ACS Applied Materials and Interfaces},
number = 45,
volume = 11,
place = {United States},
year = {2019},
month = {10}
}

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This content will become publicly available on October 16, 2020
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