Suppressing Universal Cathode Crossover in High‐Energy Lithium Metal Batteries via a Versatile Interlayer Design**

Xie, Chuyi; Zhao, Chen; Jeong, Heonjae; Li, Tianyi; Li, Luxi; Xu, Wenqian; Yang, Zhenzhen; Lin, Cong; Liu, Qiang; Cheng, Lei; Huang, Xingkang; Xu, Gui‐Liang; Amine, Khalil; Chen, Guohua

doi:10.1002/anie.202217476

Title: Suppressing Universal Cathode Crossover in High‐Energy Lithium Metal Batteries via a Versatile Interlayer Design**

Journal Article · Mon Apr 03 00:00:00 EDT 2023 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202217476· OSTI ID:2274833

Xie, Chuyi ^[1]; Zhao, Chen ^[2]; Jeong, Heonjae ^[3]; Li, Tianyi ^[4]; Li, Luxi ^[4]; Xu, Wenqian ^[4]; Yang, Zhenzhen ^[2]; Lin, Cong ^[1]; Liu, Qiang ^[1]; Cheng, Lei ^[3]; Huang, Xingkang ^[2];

^[2]; Amine, Khalil ^[5]; Chen, Guohua ^[6]

Department of Mechanical Engineering and Research Institute for Smart Energy (RISE) The Hong Kong Polytechnic University 11 Yuk Choi Rd Hung Hom Hong Kong
Chemical Sciences and Engineering Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA
Materials Science Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA
X-ray Sciences Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA
Chemical Sciences and Engineering Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA, Materials Science and Engineering Stanford University Stanford CA 94305 USA, Materials Science and Nanoengineering Mohammed VI Polytechnic University Lot 660 Hay Moulay Rachid Ben Guerir 43150 Morocco, Institute for Research&, Medical Consultations Imam Abdulrahman Bin Faisal University (IAU) Dammam Saudi Arabia
Department of Mechanical Engineering and Research Institute for Smart Energy (RISE) The Hong Kong Polytechnic University 11 Yuk Choi Rd Hung Hom Hong Kong, School of Energy and Environment City University of Hong Kong Kowloon Hong Kong

Abstract The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high‐energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as‐induced dual‐gradient solid‐electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm ⁻² . Moreover, X‐ray photoelectron spectroscopy and synchrotron X‐ray experiments revealed that N‐rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high‐energy cathode materials including LiNi _0.7 Mn _0.2 Co _0.1 O ₂ , Li _1.2 Co _0.1 Mn _0.55 Ni _0.15 O ₂ , and sulfur demonstrate significantly improved cycling stability with high cathode loading.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: 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); Shenzhen Science and Technology Program; Guangdong Basic and Applied Basic Research Foundation; GDSTC-Guangdong-HK-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices

Grant/Contract Number:: AC02-06CH11357; SGDX20190816230615451; 2020A1515110798; 2019B121205001

OSTI ID:: 2274833

Alternate ID(s):: OSTI ID: 1968056; OSTI ID: 2314988

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Vol. 62 Journal Issue: 19; ISSN 1433-7851

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

Country of Publication:: Germany

Language:: English

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