Influence Mechanism of Interfacial Oxidation of Li₃YCl₆ Solid Electrolyte on Reduction Potential

Wang, Xin1,2; Yang, Zhiqiang2,3,4; Li, Na2; Wu, Kang2; Gao, Kesheng2; Zhao, Enyue2; Han, Songbai3,4; Guo, Wenhan1,5

2024-04-05

10.1002/chem.202303884

CHEMISTRY-A EUROPEAN JOURNAL   影响因子和分区

0947-6539

1521-3765

Halide-based solid electrolytes are promising candidates for all solid-state lithium-ion batteries (ASSLBs) due to their high ionic conductivity, wide electrochemical window, and excellent chemical stability with cathode materials. However, when tested in practice, their intrinsic electrochemical stability windows do not well match the conditions for stable operation of ASSBs. Existing literature reports halide-based ASSBs that still operate well outside the electrochemical stability window, while ASSBs that do not operate within the window are not well studied or the studies are based on the cathode material interface. In this study, we aim to elucidate the mechanism behind all-solid-state battery failure by investigating how the reduction potential of Li3YCl6 solid-state electrolyte itself changes under overcharging conditions. Our findings demonstrate that in Li-In|Li3YCl6|Li3YCl6-C half-cells during the first state of charge, Cl ions participate in charge compensation, resulting in a depletion of ligands. This phenomenon significantly affects the reduction potential of Y3+, causing it to be reduced to Y2Cl3 and ultimately to Y-0 at conditions far exceeding its actual reduction potential. Furthermore, we analyze the interfacial impedance induced by this process and propose a novel perspective on battery failure.

All-solid-state lithium batteries Halide-based electrolytes Reduction potential Interface

SCI ; EI

英语

通讯

National Natural Science Foundation of China["52203361","12105197"] ; Guangdong Basic and Applied Basic Research Foundation["2023A1515012351","2022A1515010319"] ; Open research fund of Songshan Lake Materials Laboratory[2022SLABFK04]

Chemistry

Chemistry, Multidisciplinary

WOS:001173788000001

WILEY-V C H VERLAG GMBH

CHEMISTRY

Web of Science

1.Great Bay Univ, Sch Phys Sci, Dongguan Key Lab Interdisciplinary Sci Adv Mat & L, Dongguan 523000, Guangdong, Peoples R China
2.Songshan Lake Mat Lab, Dongguan 523808, Guangdong, Peoples R China
3.Southern Univ Sci & Technol, Acad Adv Interdisciplinary Studies, Shenzhen 518055, Guangdong, Peoples R China
4.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Guangdong, Peoples R China
5.Great Bay Inst Adv Study, Dongguan 523000, Peoples R China

Wang, Xin,Yang, Zhiqiang,Li, Na,et al. Influence Mechanism of Interfacial Oxidation of Li₃YCl₆ Solid Electrolyte on Reduction Potential[J]. CHEMISTRY-A EUROPEAN JOURNAL,2024,30(20).

Wang, Xin.,Yang, Zhiqiang.,Li, Na.,Wu, Kang.,Gao, Kesheng.,...&Guo, Wenhan.(2024).Influence Mechanism of Interfacial Oxidation of Li₃YCl₆ Solid Electrolyte on Reduction Potential.CHEMISTRY-A EUROPEAN JOURNAL,30(20).

Wang, Xin,et al."Influence Mechanism of Interfacial Oxidation of Li₃YCl₆ Solid Electrolyte on Reduction Potential".CHEMISTRY-A EUROPEAN JOURNAL 30.20(2024).