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Title: Excellent stability of a lithium-ion-conducting solid electrolyte upon reversible Li +/H + exchange in aqueous solutions

Abstract

Batteries with an aqueous catholyte and a Li metal anode have attracted interest owing to their exceptional energy density and high charge/discharge rate. The long-term operation of such batteries requires that the solid electrolyte separator between the anode and aqueous solutions must be compatible with Li and stable over a wide pH range. Unfortunately, no such compound has yet been reported. In this study, an excellent stability in neutral and strongly basic solutions was observed when using the cubic Li 7La 3Zr 2O 12 garnet as a Li-stable solid electrolyte. The material underwent a Li +/H + exchange in aqueous solutions. Nevertheless, its structure remained unchanged even under a high exchange rate of 63.6%. When treated with a 2 M LiOH solution, the Li +/H + exchange was reversed without any structural change. Furthermore, these observations suggest that cubic Li 7La 3Zr 2O 12 is a promising candidate for the separator in aqueous lithium batteries.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Michigan State Univ., East Lansing, MI (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1185524
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 54; Journal Issue: 1; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium batteries; solid electrolytes; garnet; proton exchange; electron microscopy

Citation Formats

Ma, Cheng, Rangasamy, Ezhiylmurugan, Liang, Chengdu, Sakamoto, Jeffrey, More, Karren Leslie, and Chi, Miaofang. Excellent stability of a lithium-ion-conducting solid electrolyte upon reversible Li+/H+ exchange in aqueous solutions. United States: N. p., 2014. Web. doi:10.1002/anie.201408124.
Ma, Cheng, Rangasamy, Ezhiylmurugan, Liang, Chengdu, Sakamoto, Jeffrey, More, Karren Leslie, & Chi, Miaofang. Excellent stability of a lithium-ion-conducting solid electrolyte upon reversible Li+/H+ exchange in aqueous solutions. United States. doi:10.1002/anie.201408124.
Ma, Cheng, Rangasamy, Ezhiylmurugan, Liang, Chengdu, Sakamoto, Jeffrey, More, Karren Leslie, and Chi, Miaofang. Tue . "Excellent stability of a lithium-ion-conducting solid electrolyte upon reversible Li+/H+ exchange in aqueous solutions". United States. doi:10.1002/anie.201408124. https://www.osti.gov/servlets/purl/1185524.
@article{osti_1185524,
title = {Excellent stability of a lithium-ion-conducting solid electrolyte upon reversible Li+/H+ exchange in aqueous solutions},
author = {Ma, Cheng and Rangasamy, Ezhiylmurugan and Liang, Chengdu and Sakamoto, Jeffrey and More, Karren Leslie and Chi, Miaofang},
abstractNote = {Batteries with an aqueous catholyte and a Li metal anode have attracted interest owing to their exceptional energy density and high charge/discharge rate. The long-term operation of such batteries requires that the solid electrolyte separator between the anode and aqueous solutions must be compatible with Li and stable over a wide pH range. Unfortunately, no such compound has yet been reported. In this study, an excellent stability in neutral and strongly basic solutions was observed when using the cubic Li7La3Zr2O12 garnet as a Li-stable solid electrolyte. The material underwent a Li+/H+ exchange in aqueous solutions. Nevertheless, its structure remained unchanged even under a high exchange rate of 63.6%. When treated with a 2 M LiOH solution, the Li+/H+ exchange was reversed without any structural change. Furthermore, these observations suggest that cubic Li7La3Zr2O12 is a promising candidate for the separator in aqueous lithium batteries.},
doi = {10.1002/anie.201408124},
journal = {Angewandte Chemie (International Edition)},
number = 1,
volume = 54,
place = {United States},
year = {Tue Oct 21 00:00:00 EDT 2014},
month = {Tue Oct 21 00:00:00 EDT 2014}
}

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Free Publicly Available Full Text
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Cited by: 22 works
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Works referenced in this record:

A study on lithium/air secondary batteries—Stability of NASICON-type glass ceramics in acid solutions
journal, September 2010


Study on lithium/air secondary batteries—Stability of NASICON-type lithium ion conducting glass–ceramics with water
journal, April 2009


Fast Lithium Ion Conduction in Garnet-Type Li7La3Zr2O12
journal, October 2007

  • Murugan, Ramaswamy; Thangadurai, Venkataraman; Weppner, Werner
  • Angewandte Chemie International Edition, Vol. 46, Issue 41, p. 7778-7781
  • DOI: 10.1002/anie.200701144

Li-Redox Flow Batteries Based on Hybrid Electrolytes: At the Cross Road between Li-ion and Redox Flow Batteries
journal, June 2012

  • Wang, Yarong; He, Ping; Zhou, Haoshen
  • Advanced Energy Materials, Vol. 2, Issue 7, p. 770-779
  • DOI: 10.1002/aenm.201200100