All-Solid-State Lithium–Sulfur Batteries Enhanced by Redox Mediators

Gao, Xin; Zheng, Xueli; Tsao, Yuchi; Zhang, Pu; Xiao, Xin; Ye, Yusheng; Li, Jun; Yang, Yufei; Xu, Rong; Bao, Zhenan; Cui, Yi

doi:10.1021/jacs.1c07754

Title: All-Solid-State Lithium–Sulfur Batteries Enhanced by Redox Mediators

Journal Article · Fri Oct 22 00:00:00 EDT 2021 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.1c07754· OSTI ID:1874795

^[1];

^[1]; Tsao, Yuchi ^[1]; Zhang, Pu ^[1];

^[1];

^[1]; Yang, Yufei ^[1]; Xu, Rong ^[1];

^[1];

^[2]

Stanford University, CA (United States)
Stanford University, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

We report redox mediators (RMs) play a vital role in some liquid electrolyte-based electrochemical energy storage systems. However, the concept of redox mediator in solid-state batteries remains unexplored. Here, we selected a group of RM candidates and investigated their behaviors and roles in all-solid-state lithium-sulfur batteries (ASSLSBs). The soluble-type quinone-based RM (AQT) shows the most favorable redox potential and the best redox reversibility that functions well for lithium sulfide (Li₂S) oxidation in solid polymer electrolytes. Accordingly, Li₂S cathodes with AQT RMs present a significantly reduced energy barrier (average oxidation potential of 2.4 V) during initial charging at 0.1 C at 60 °C and the following discharge capacity of 1133 mAh g_s^-1. Using operando sulfur K-edge X-ray absorption spectroscopy, we directly tracked the sulfur speciation in ASSLSBs and proved that the solid-polysulfide-solid reaction of Li₂S cathodes with RMs facilitated Li₂S oxidation. In contrast, for bare Li₂S cathodes, the solid-solid Li₂S-sulfur direct conversion in the first charge cycle results in a high energy barrier for activation (charge to ~4 V) and low sulfur utilization. The Li₂S@AQT cell demonstrates superior cycling stability (average Coulombic efficiency 98.9% for 150 cycles) and rate capability owing to the effective AQT-enhanced Li-S reaction kinetics. This work reveals the evolution of sulfur species in ASSLSBs and realizes the fast Li-S reaction kinetics by designing an effective sulfur speciation pathway

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1874795

Journal Information:: Journal of the American Chemical Society, Vol. 143, Issue 43; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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