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

Journal Article · · Angewandte Chemie (International Edition)
 [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)

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.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1185524
Journal Information:
Angewandte Chemie (International Edition), Vol. 54, Issue 1; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 98 works
Citation information provided by
Web of Science

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Progress of the Interface Design in All-Solid-State Li-S Batteries journal March 2018
The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li 7 La 3 Zr 2 O 12 Interphase journal April 2019
Excellent Compatibility of Solvate Ionic Liquids with Sulfide Solid Electrolytes: Toward Favorable Ionic Contacts in Bulk-Type All-Solid-State Lithium-Ion Batteries journal August 2015
Mesoscopic Framework Enables Facile Ionic Transport in Solid Electrolytes for Li Batteries journal March 2016
Designing Safe Electrolyte Systems for a High-Stability Lithium-Sulfur Battery journal January 2018
Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12 journal April 2019
Chemistry Design Towards a Stable Sulfide-Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12 journal April 2019
Impact of air exposure and surface chemistry on Li–Li 7 La 3 Zr 2 O 12 interfacial resistance journal January 2017
Local Li-ion conductivity changes within Al stabilized Li 7 La 3 Zr 2 O 12 and their relationship to three-dimensional variations of the bulk composition journal January 2019
Oxide Electrolytes for Lithium Batteries journal September 2015