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钼-氧双掺杂硫银锗矿型电解质助力稳定全固态锂电池

Mo-O Dual-Doped Argyrodite Electrolyte Enables Stable All-Solid-State Lithium Batteries.

作者信息

Cao Panlei, Chen Jinghui, Li Jiejie, Yu Haichuan, Lin Jiale, Tian Ziqi, Liu Gaozhan, Yao Xiayin

机构信息

Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, 315201, P. R. China.

Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

出版信息

Small. 2025 Jun;21(25):e2501901. doi: 10.1002/smll.202501901. Epub 2025 May 2.

Abstract

Sulfide solid electrolytes are one of the most promising solid electrolytes for all-solid-state lithium batteries due to their relatively high ionic conductivity and favorable mechanical properties. Nevertheless, their inferior moisture stability and lithium metal compatibility hinder the practical applications. Herein, a Mo-O dual-doped argyrodite LiP MoS O Cl sulfide electrolytes are synthesized to enhance both moisture stability and electrochemical characteristics. By adjusting the concentrations of dopant and annealing temperature, the optimized LiPMoSOCl sintered at 570 °C exhibits enhanced room-temperature powder cold-pressed ionic conductivity of 3.97 mS cm. Moreover, LiPMoSOCl solid electrolyte produces only one-third of HS gas with 0.58 cm g compared to pristine LiPSCl electrolyte and exhibits excellent structure stability after exposure to air. Benefitting from the generation of a stable LiOCl at the anode interface, LiPMoSOCl solid electrolyte exhibits superior interfacial compatibility and suppression capability of lithium dendrites, realizing a high critical current density of 1.51 mA cm and maintains stable lithium plating/stripping behavior for 5600 h at 0.1 mA cm and 0.1 mAh cm. In addition, the LiCoO/LiPMoSOCl/Li battery presents improved cycling stability at 1C with a capacity retention of 90.3% after 1000 cycles.

摘要

硫化物固体电解质因其相对较高的离子电导率和良好的机械性能,是全固态锂电池最有前途的固体电解质之一。然而,其较差的水分稳定性和锂金属兼容性阻碍了实际应用。在此,合成了一种Mo - O双掺杂的硫银锗矿型LiP MoS O Cl硫化物电解质,以提高其水分稳定性和电化学特性。通过调整掺杂剂浓度和退火温度,在570°C烧结的优化后的LiPMoSOCl表现出增强的室温粉末冷压离子电导率,为3.97 mS cm。此外,与原始的LiPSCl电解质相比,LiPMoSOCl固体电解质产生的H₂S气体仅为其三分之一,在暴露于空气中后表现出优异的结构稳定性。受益于在阳极界面生成稳定的LiOCl,LiPMoSOCl固体电解质表现出优异的界面兼容性和锂枝晶抑制能力,实现了1.51 mA cm的高临界电流密度,并在0.1 mA cm和0.1 mAh cm下保持5600 h的稳定锂电镀/剥离行为。此外,LiCoO₂/LiPMoSOCl/Li电池在1C下表现出改善的循环稳定性,在1000次循环后容量保持率为90.3%。

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