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Wet chemical synthesis and properties of argyrodite sulfide solid electrolytes for solid state lithium batteries

Other ·
OSTI ID:2370137
 [1]
  1. University of Louisville; University of Louisville

The commercialization of the lithium-ion battery (LIB) in 1991 was responsible for the explosion in portable electronic technologies that has been seen over the past 30 years. With the advent of electric vehicles and other high-powered technologies, there is tremendous demand for LIBs with higher energy density and high safety. To achieve this, new electrode materials must be explored. The obvious choice of anode material would be pure metal lithium, which has a theoretical specific capacity of 3860 mAh g-1 . Unfortunately, metal lithium anodes have not been widely commercialized due to their tendency to react violently with the flammable liquid electrolytes used in today’s batteries. Battery safety can best be achieved by adopting solid electrolytes in place of liquid electrolytes. Solid electrolytes are nonvolatile and nonflammable, safely allowing for the combination of high-capacity cathode materials with a Li metal anode. Argyrodite sulfide solid electrolytes such as halogen-doped Li6PS5X (X = Cl, Br, I) are noted for their high ionic conductivity. But before sulfides can be commercially adopted, they possess several disadvantages which must be addressed, including time- and energy-consuming synthesis processes, poor electrochemical stability, and intrinsically poor air stability. This dissertation seeks to address each of these challenges through materials design an synthesis strategies. In this work, we pioneer a solvent-based approach for the synthesis of argyrodite solid electrolytes Li7PS6 and Li6PS5Xinstead of a stringent solid-state synthesis. Nontoxic ethanol is employed as the solvent, enabling a rapid synthetic approach to produce argyrodite solid electrolytes with high phase purity and compositional flexibility. Compared with Li7PS6, halogen doping (i.e. X = F, Cl, Br, I) not only increases the ionic conductivity, but also enhances the electrochemical stability at the interface towards Li metal. Specifically, F-doped argyrodites produce a robust SEI layer containing LiF, contributing to enhanced interfacial stability. Finally, to address the air instability challenge, argyrodite-incorporated composite solid electrolytes (CSEs) are designed and prepared to produce stable and flexible membranes that are demonstrated in solid-state Li metal batteries. These advances push argyrodite sulfide solid electrolyte research further and pave the way for the proliferation of next generation lithium metal batteries.

Research Organization:
University of Louisville
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
DOE Contract Number:
EE0008866
OSTI ID:
2370137
Country of Publication:
United States
Language:
English

References (10)

Highly efficient interface stabilization for ambient-temperature quasi-solid-state sodium metal batteries journal April 2022
Stable and Flexible Sulfide Composite Electrolyte for High-Performance Solid-State Lithium Batteries journal August 2020
Fast Na diffusion and anharmonic phonon dynamics in superionic Na 3 PS 4 journal January 2021
Li0.625Al0.125H0.25Cl0.75O0.25 Superionic Conductor with Disordered Rock-Salt Structure journal July 2021
Rapid and Economic Synthesis of a Li 7 PS 6 Solid Electrolyte from a Liquid Approach journal January 2019
Interface stability of LiCl-rich argyrodite Li6PS5Cl with propylene carbonate boosts high-performance lithium batteries journal December 2020
Regulated lithium ionic flux through well-aligned channels for lithium dendrite inhibition in solid-state batteries journal October 2020
Synthesis of Fluorine-Doped Lithium Argyrodite Solid Electrolytes for Solid-State Lithium Metal Batteries journal February 2022
Halide doping effect on solvent-synthesized lithium argyrodites Li6PS5X (X= Cl, Br, I) superionic conductors journal July 2020
Phase‐Transition Interlayer Enables High‐Performance Solid‐State Sodium Batteries with Sulfide Solid Electrolyte journal April 2021

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