Synthesis of Fluorine-Doped Lithium Argyrodite Solid Electrolytes for Solid-State Lithium Metal Batteries.

Autor: Arnold W; Department of Mechanical Engineering Department, University of Louisville, 332 Eastern Parkway, Louisville, Kentucky 40292, United States., Shreyas V; Department of Mechanical Engineering Department, University of Louisville, 332 Eastern Parkway, Louisville, Kentucky 40292, United States., Li Y; Department of Mechanical Engineering Department, University of Louisville, 332 Eastern Parkway, Louisville, Kentucky 40292, United States.; Conn Center for Renewable Energy Research, University of Louisville, 216 Eastern Parkway, Louisville, Kentucky 40208, United States., Koralalage MK; Department of Physics & Astronomy, University of Louisville, 102 Natural Science Building, Louisville, Kentucky 40292, United States., Jasinski JB; Conn Center for Renewable Energy Research, University of Louisville, 216 Eastern Parkway, Louisville, Kentucky 40208, United States., Thapa A; Conn Center for Renewable Energy Research, University of Louisville, 216 Eastern Parkway, Louisville, Kentucky 40208, United States., Sumanasekera G; Department of Physics & Astronomy, University of Louisville, 102 Natural Science Building, Louisville, Kentucky 40292, United States., Ngo AT; Materials Science Division, Argonne National Laboratory, 9700 S. Cass Avenue, Lemont, Illinois 60439, United States.; Department of Chemical Engineering, University of Illinois Chicago, 929 W. Taylor St, MC 110, Chicago, Illinois 60607, United States., Narayanan B; Department of Mechanical Engineering Department, University of Louisville, 332 Eastern Parkway, Louisville, Kentucky 40292, United States., Wang H; Department of Mechanical Engineering Department, University of Louisville, 332 Eastern Parkway, Louisville, Kentucky 40292, United States.; Conn Center for Renewable Energy Research, University of Louisville, 216 Eastern Parkway, Louisville, Kentucky 40208, United States.
Jazyk: angličtina
Zdroj: ACS applied materials & interfaces [ACS Appl Mater Interfaces] 2022 Mar 09; Vol. 14 (9), pp. 11483-11492. Date of Electronic Publication: 2022 Feb 23.
DOI: 10.1021/acsami.1c24468
Abstrakt: Solid-state lithium metal batteries (SSLMBs) that utilize novel solid electrolytes (SEs) have garnered much attention because of their potential to yield safe and high-energy-density batteries. Sulfide-based argyrodite-class SEs are an attractive option because of their impressive ionic conductivity. Recent studies have shown that LiF at the interface between Li and SE enhances electrochemical stability. However, the synthesis of F-doped argyrodites has remained challenging because of the high temperatures used in the state-of-the-art solid-state synthesis methods. In this work, for the first time, we report F-doped Li 5+ y PS 5 F y argyrodites with a tunable doping content and dual dopants (F - /Cl - and F - /Br - ) that were synthesized through a solvent-based approach. Among all compositions, Li 6 PS 5 F 0.5 Cl 0.5 exhibits the highest Li-ion conductivity of 3.5 × 10 -4 S cm -1 at room temperature (RT). Furthermore, Li symmetric cells using Li 6 PS 5 F 0.5 Cl 0.5 show the best cycling performance among the tested cells. X-ray photoelectron spectroscopy and ab initio molecular dynamics simulations revealed that the enhanced interfacial stability of Li 6 PS 5 F 0.5 Cl 0.5 SE against Li metal can be attributed to the formation of a stable solid electrolyte interphase (SEI)-containing conductive species (Li 3 P), alongside LiCl and LiF. These findings open new opportunities to develop high-performance SSLMBs using a novel class of F-doped argyrodite electrolytes.
Databáze: MEDLINE