Unraveling the Highly Reversible Lithiation/Delithiation of Aluminum in Inorganic All-Solid-State Lithium Batteries

• DOI: 10.1021/acsami.5c00702
• Publication Date: 2025-03-28T05:34:01Z
• Authors: Jiawu Cui; Zhen Wang; Jiewen Tan; Zhanhui Jia; Chao Wu; Zichun Xiao; Xianwei Wang; Xiaowei Wang; Yuping Wu; Wei Tang
• Keywords: Lithium metal

The all-solid-state lithium battery (ASSLB) is widely regarded as one of the most promising systems for future owing to its high energy density and enhanced safety. However, spontaneous reaction between metal solid-state electrolytes (SSEs) results in formation dendrites, which impedes further progress use anodes ASSLBs. Li–In-based have been used address Li anode/SSE interfacial challenges; however, their synthesis cell fabrication compromise applicability Herein, we explore aluminum an anode ASSLBs by dry mixing investigate compatibility with two typical types SSEs: halide-based Li3InCl6 sulfide-based Li5.4PS4.4Cl1.6, show distinguished electrochemical behaviors. In ASSLBs, continuous decomposition reduction cause accumulation indium at interface SSE anode, blocks Li-ion transport, causing impedance increase rapid failure. By sharp contrast, a redox-active interphase formed sulfide during lithiation/delithiation process. consisting highly reversible redox intermediates addresses limiting factor poor reversibility Li–Al alloying, accounts conventionally low Coulombic efficiency Al anodes. This work aims develop sheds light on significance enabling