Unraveling the Stable Cathode Electrolyte Interface in all Solid‐State Thin‐Film Battery Operating at 5 V

Shimizu, Ryosuke; Cheng, Diyi; Weaver, Jamie L.; Zhang, Minghao; Lu, Bingyu; Wynn, Thomas A.; Burger, Randall; Kim, Min‐cheol; Zhu, Guomin; Meng, Ying Shirley

doi:10.1002/aenm.202201119

Title: Unraveling the Stable Cathode Electrolyte Interface in all Solid‐State Thin‐Film Battery Operating at 5 V

Journal Article · Mon Jul 04 00:00:00 EDT 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202201119· OSTI ID:1874841

^[1]; Cheng, Diyi ^[2]; Weaver, Jamie L. ^[3]; Zhang, Minghao ^[1]; Lu, Bingyu ^[1]; Wynn, Thomas A. ^[1]; Burger, Randall ^[1]; Kim, Min‐cheol ^[4]; Zhu, Guomin ^[1];

^[5]

Department of NanoEngineering University of California San Diego La Jolla CA 92093 USA
Materials Science and Engineering Program University of California San Diego La Jolla CA 92093 USA
Material Measurement Laboratory National Institute of Standards and Technology 100, Bureau Drive Gaithersburg MD 20899 USA
Department of NanoEngineering University of California San Diego La Jolla CA 92093 USA, School of Mechanical Engineering Pusan National University Busan 46241 Korea
Department of NanoEngineering University of California San Diego La Jolla CA 92093 USA, Materials Science and Engineering Program University of California San Diego La Jolla CA 92093 USA, Pritzker school of Molecular Engineering University of Chicago Chicago IL 60637 USA

Abstract Spinel‐type LiNi _0.5 Mn _1.5 O ₄ (LNMO) is one of the most promising 5 V‐class cathode materials for Li‐ion batteries that can achieve high energy density and low production costs. However, in liquid electrolyte cells, the high voltage causes continuous cell degradation through the oxidative decomposition of carbonate‐based liquid electrolytes. In contrast, some solid‐state electrolytes have a wide electrochemical stability range and can withstand the required oxidative potential. In this work, a thin‐film battery consisting of an LNMO cathode with a solid lithium phosphorus oxynitride (LiPON) electrolyte is tested and their interface before and after cycling is characterized. With Li metal as the anode, this system can deliver stable performance for 600 cycles with an average Coulombic efficiency >99%. Neutron depth profiling indicates a slight overlithiated layer at the interface prior to cycling, a result that is consistent with the excess charge capacity measured during the first cycle. Cryogenic electron microscopy further reveals intimate contact between LNMO and LiPON without noticeable structure and chemical composition evolution after extended cycling, demonstrating the superior stability of LiPON against a high voltage cathode. Consequently, design guidelines are proposed for interface engineering that can accelerate the commercialization of a high voltage cell with solid or liquid electrolytes.

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Research Organization:: Univ. of California, San Diego, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0002357; ECCS-2025752; ACI-1548562

OSTI ID:: 1874841

Alternate ID(s):: OSTI ID: 1874843; OSTI ID: 1905137

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Vol. 12 Journal Issue: 31; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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cathode electrolyte interphase
cryogenic electron microscopy
high-voltage spinel cathodes
Li metal batteries
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Title: Unraveling the Stable Cathode Electrolyte Interface in all Solid‐State Thin‐Film Battery Operating at 5 V

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