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All-climate all-solid-state batteries enabled by high-entropy amorphous oxyhalide solid electrolytes
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DOI：10.1039/D5GC03551A.png)
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Abstract
En 中文
Conventional lithium-ion batteries (LIBs) based on organic liquid electrolytes are limited to an operation temperature range of approximately −20 to +50 °C; mainly due to electrolyte decomposition and associated safety hazards; such as thermal runaway. All-solid-state batteries (ASSBs) provide inherent safety benefits but remain constrained by the limited temperature adaptability of solid electrolytes (SEs). Here; we address this challenge through a high-entropy design strategy; developing a high-entropy amorphous oxyhalide SE (Li1.6Ta(PSiB)0.15O1.65Cl5Br0.1) that incorporates three synergistic features: (1) high-entropy multication mixing (Ta5+/P5+/Si4+/B3+) creating efficient ion-conduction pathways; (2) mixed-anion engineering (O2−/Cl−/Br−) lowering ionic migration barriers; and (3) the incorporation of non-metallic cations (P5+/Si4+/B3+) improving reduction stability; all within an amorphous framework that suppresses interfacial degradation. The optimized electrolyte exhibits an exceptional ionic conductivity of 7.1 mS cm−1 at 25 °C alongside enhanced electrochemical stability. ASSBs fabricated with this high-entropy SE; a single-crystalline LiNi0.8Co0.1Mn0.1O2 (scNCM811) cathode; and a Li–In anode demonstrate outstanding wide-temperature-range-operation performance. An 82% capacity retention is achieved after 2400 cycles at 2C and 25 °C; with an ultra-low fading rate of 0.007 mAh per g per cycle. Zero capacity fade over 100 cycles at −30 °C and 80% capacity retention following 1300 cycles under 10C fast charging at 60 °C are demonstrated.
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