Electrochemically primed functional redox mediator generator from the decomposition of solid state electrolyte

Matthew Li, Zhengyu Bai (), Yejing Li, Lu Ma, Alvin Dai, Xuefeng Wang, Dan Luo, Tianpin Wu, Ping Liu, Lin Yang, Khalil Amine, Zhongwei Chen () and Jun Lu ()
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Matthew Li: Henan Normal University
Zhengyu Bai: Henan Normal University
Yejing Li: University of California San Diego
Lu Ma: Argonne National Laboratory
Alvin Dai: Argonne National Laboratory
Xuefeng Wang: University of California San Diego
Dan Luo: University of Waterloo
Tianpin Wu: Argonne National Laboratory
Ping Liu: University of California San Diego
Lin Yang: Henan Normal University
Khalil Amine: Argonne National Laboratory
Zhongwei Chen: University of Waterloo
Jun Lu: Argonne National Laboratory

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: Abstract Recent works into sulfide-type solid electrolyte materials have attracted much attention among the battery community. Specifically, the oxidative decomposition of phosphorus and sulfur based solid state electrolyte has been considered one of the main hurdles towards practical application. Here we demonstrate that this phenomenon can be leveraged when lithium thiophosphate is applied as an electrochemically “switched-on” functional redox mediator-generator for the activation of commercial bulk lithium sulfide at up to 70 wt.% lithium sulfide electrode content. X-ray adsorption near-edge spectroscopy coupled with electrochemical impedance spectroscopy and Raman indicate a catalytic effect of generated redox mediators on the first charge of lithium sulfide. In contrast to pre-solvated redox mediator species, this design decouples the lithium sulfide activation process from the constraints of low electrolyte content cell operation stemming from pre-solvated redox mediators. Reasonable performance is demonstrated at strict testing conditions.

Date: 2019
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DOI: 10.1038/s41467-019-09638-4

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