Highly reversible Li2RuO3 cathodes in sulfide-based all solid-state lithium batteries

Wu, Yuqi; Zhou, Ke; Ren, Fucheng; Ha, Yang; Liang, Ziteng; Zheng, Xuefan; Wang, Zhenyu; Yang, Wu; Zhang, Maojie; Luo, Mingzeng; Battaglia, Corsin; Yang, Wanli; Zhu, Lingyun; Gong, Zhengliang; Yang, Yong

doi:10.1039/d2ee01067d

Highly reversible Li₂RuO₃ cathodes in sulfide-based all solid-state lithium batteries

Journal Article · Wed Jul 06 00:00:00 EDT 2022 · Energy & Environmental Science

DOI:https://doi.org/10.1039/d2ee01067d· OSTI ID:1963045

Wu, Yuqi ^[1]; Zhou, Ke ^[2]; Ren, Fucheng ^[1]; ^[3]; Liang, Ziteng ^[1]; Zheng, Xuefan ^[1]; Wang, Zhenyu ^[4]; Yang, Wu ^[1]; Zhang, Maojie ^[1]; Luo, Mingzeng ^[1]; Battaglia, Corsin ^[5]; ^[3]; Zhu, Lingyun ^[4]; ^[1]; ^[1]

Xiamen Univ. (China)
Xiamen Univ. (China); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Guilin Electrical Equipment Scientific Research Institute Co., Ltd, Guilin (China)
Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)

The practical application of high-capacity lithium-rich cathode materials in lithium-ion batteries has been largely restricted by severe side reactions with electrolytes. Herein, we report a highly stable lithium-rich Li₂RuO₃ cathode by forming a passivating solid electrolyte interphase at the interface with a sulfide solid electrolyte such as Li₆PS₅Cl in all-solid-state lithium batteries (ASSLBs), which efficiently suppresses serious parasitic interfacial reactions and fast-increasing interfacial impedance normally observed in liquid electrolytes. The exceptionally high interfacial stability of the Li₂RuO₃/sulfide electrolyte interface contributes to a high reversible capacity of 257 mA h g^–1 of Li₂RuO₃ at 0.05C rate, and unprecedented cycling stability with 90% capacity retention after 1000 cycles at 1C rate. Iin this work, comprehensive experimental characterizations and first-principles calculations disclose that electronically insulating interfacial reaction products forming at the interface between the Li₂RuO₃ cathode and Li₆PS₅Cl facilitate the formation of a stable and passivating interphase and block the continuous side reactions. Importantly, reversible oxygen redox activity of Li₂RuO₃ is well-maintained in this configuration of ASSLBs even after 600 cycles, thus the common voltage decay of the Li-rich material is also significantly reduced. These new discoveries demonstrate the critical role of interface design for achieving prolonged cycling stability of lithium-rich cathode materials.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Key R&D Program of China; National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1963045

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 8 Vol. 15; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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