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

Journal Article · · Energy & Environmental Science
DOI:https://doi.org/10.1039/d2ee01067d· OSTI ID:1963045
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  1. Xiamen Univ. (China)
  2. Xiamen Univ. (China); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  4. Guilin Electrical Equipment Scientific Research Institute Co., Ltd, Guilin (China)
  5. 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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
AC02-05CH11231; 21875196; 21935009; 22021001; 2021YFB2401800; 2019H0003
OSTI ID:
1963045
Journal Information:
Energy & Environmental Science, Vol. 15, Issue 8; ISSN 1754-5692
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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