Self-Sacrificing Reductive Interphase for Robust and High-Performance Sulfide-Based All-Solid-State Lithium Batteries

ADVANCED ENERGY MATERIALS(2024)

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Abstract
All-solid-state lithium-ion batteries (ASSLIBs) based on sulfide solid-state electrolytes (S-SSEs) are considered as one of the most promising choices to address the safety hazards of traditional lithium-ion batteries. However, the high-voltage cathodes, such as LiCoO2 (LCO) with high-valence Co (+3), tend to spontaneously oxidize S-SSEs, causing polarization increase and rapid degradation. Herein, a self-sacrificing reductive interphase consisting of CoO/Li2CO3/C, is in situ constructed on LCO surface via a simple carbon-induced thermal reduction of LCO. With such a design, the Co valence of LCO surface is reduced to +2, reducing the oxidative nature of LCO to avoid reactions with S-SSEs. As a result, ASSLIBs using Li10GeP2S12 (LGPS) S-SSEs achieve a high initial capacity of 144.9 mAh g-1 at 0.2 C and retard 93.1% of initial capacity after 100 cycles. Additionally, excellent rate cyclability of 109.2 mAh g-1 at 1.0 C with 81.5% retentive capacity for 200 cycles is attained as well. Comprehensive evidence strongly demonstrates the effectiveness of this self-sacrificing reductive interphase in inhibiting the interfacial reactions and ensuring long-term cyclability. The proposed concept of a self-sacrificing reductive interface in this study paves the way for stabilizing the cathode/SSEs interface and offers a novel approach for the design of high-performance sulfide-based ASSLIBs. The notion of interface reconstruction through self-sacrificial reduction is proposed. Citric acid is employed as reducing agent for the thermal reduction of LCO, facilitating the generation of an in situ coating on the surface of LCO. This coating is devised to impede the interface reaction, establish stability within the LCO/LGPS interface, and enhance the long-term cycling potential of all-solid-state batteries.image
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Key words
all-solid-state lithium-ion batteries,interfacial reaction,self-sacrificing reductive interphase,sulfide solid electrolyte
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