Manipulating Charge-Transfer Kinetics of Lithium-Rich Layered Oxide Cathodes in Halide All-Solid-State Batteries.

Yu, Ruizhi; Wang, Changhong; Duan, Hui; Jiang, Ming; Zhang, Anbang; Fraser, Adam; Zuo, Jiaxuan; Wu, Yanlong et al. · Adv Mater · 2023

basic_science · Level V

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Abstract

Employing lithium-rich layered oxide (LLO) as the cathode of all-solid-state batteries (ASSBs) is highly desired for realizing high energy density. However, the poor kinetics of LLO, caused by its low electronic conductivity and significant oxygen-redox-induced structural degradation, has impeded its application in ASSBs. Here, the charge transfer kinetics of LLO is enhanced by constructing high-efficiency electron transport networks within solid-state electrodes, which considerably minimizes electron transfer resistance. In addition, an infusion-plus-coating strategy is introduced to stabilize the lattice oxygen of LLO, successfully suppressing the interfacial oxidation of solid electrolyte (Li<sub>3</sub> InCl<sub>6</sub> ) and structural degradation of LLO. As a result, LLO-based ASSBs exhibit a high discharge capacity of 230.7 mAh g<sup>-1</sup> at 0.1 C and ultra-long cycle stability over 400 cycles. This work provides an in-depth understanding of the kinetics of LLO in solid-state electrodes, and affords a practically feasible strategy to obtain high-energy-density ASSBs.