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Rational Design for the Potential Substitute of Sulfide in Halide-Based All Solid-State Lithium Metal Batteries

Tianrui Sun, Qiuhan Wang,Jiaxuan Liao,Sizhe Wang

JOURNAL OF COLLOID AND INTERFACE SCIENCE(2025)

Univ Elect Sci & Technol China | Shenzhen Univ

Cited 0|Views5
Abstract
Halide-type solid-state electrolytes (SEs) are regarded as promising candidates for the commercialization of all solid-state lithium metal batteries (ASLMBs). However, the poor reduction stability of their central structural metal cations complicates the direct contact with lithium metal, thus conventionally requiring a sulfide interlayer between the lithium metal anode and halide SE. Concerning this issue, we developed a systematic approach to identify the SE in the halide family with thermodynamic stability, cost-effectiveness, and ionic conductivity to substitute the sulfide buffer layer and support the operation of ASLMBs utilizing solely halide-type SEs. The initial screen results indicate that Li3Y(BrCl)(3) (LYBC) is a promising candidate. Our theoretical calculations confirmed its lower reduction potential of 0.58 V. The lithium symmetrical cell using LYBC was able to cycle for over 1000 hat a current density of 0.255 mA cm(-2) and an areal capacity of 0.255mAh cm(-2). The performance of ASLMBs also notarized the feasibility of our strategy. In addition, according to our experiment, we deduce that the reduced LYBC can still conduct lithium-ion rapidly, which may be the key to supporting the normal operation of the electrochemical system. Combined with our cost analysis, LYBC is identified as one of the most suitable commercial materials for realizing the self-liberation of halide SEs. Our research proposes a novel pathway for the future development of halide SEs.
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Halide,Solid-state Battery,Electrolyte,Superionic Conductor
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要点】:本研究提出了一种系统方法,用以识别具有热力学稳定性、成本效益和离子导电性的卤素基固态电解质,以取代硫化物缓冲层,实现仅使用卤素基固态电解质的固态锂电池的商业化,创新性地选用Li3Y(BrCl)3(LYBC)作为硫化物的潜在替代品。

方法】:通过理论计算评估LYBC的热力学稳定性和还原电位,结合成本分析和电化学性能测试,确定了LYBC作为硫化物替代品的可行性。

实验】:构建了使用LYBC的锂对称电池,该电池在0.255 mA cm^-2的电流密度下能够循环超过1000小时,实验结果表明LYBC在还原状态下仍能快速传导锂离子,证实了其作为固态锂电池中硫化物替代品的可行性。