Revealing Nanoscale Solid–Solid Interfacial Phenomena for Long-Life and High-Energy All-Solid-State Batteries

Journal Article · 23 October 2019 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.9b13955 · OSTI ID:1606549

Banerjee, Abhik ^[1]; Tang, Hanmei  ^[1]; Wang, Xuefeng  ^[1]; Cheng, Ju-Hsiang ^[1]; Nguyen, Han ^[1]; Zhang, Minghao ^[1]; Tan, Darren H. S. ^[1]; Wynn, Thomas A. ^[1]; Wu, Erik A. ^[1]; Doux, Jean-Marie ^[1]; Wu, Tianpin ^[2]; Ma, Lu ^[2]; Sterbinsky, George E. ^[2]; D’Souza, Macwin Savio ^[1]; Ong, Shyue Ping  ^[1]; Meng, Ying Shirley  ^[1]

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1. Univ. of California, San Diego, La Jolla, CA (United States)
2. Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)

Enabling long cyclability of high-voltage oxide cathodes is a persistent challenge for all-solid-state batteries, largely because of their poor interfacial stabilities against sulfide solid electrolytes. While protective oxide coating layers such as LiNbO₃ (LNO) have been proposed, its precise working mechanisms are still not fully understood. Existing literature attributes reductions in interfacial impedance growth to the coating's ability to prevent interfacial reactions. However, its true nature is more complex, with cathode interfacial reactions and electrolyte electrochemical decomposition occurring simultaneously, making it difficult to decouple each effect. Herein, we utilized various advanced characterization tools and first-principles calculations to probe the interfacial phenomenon between solid electrolyte Li6PS5Cl (LPSCl) and high-voltage cathode LiNi_0.85Co_0.1Al_0.05O₂ (NCA). We segregated the effects of spontaneous reaction between LPSCl and NCA at the interface and quantified the intrinsic electrochemical decomposition of LPSCl during cell cycling. We report both experimental and computational results demonstrated improved thermodynamic stability between NCA and LPSCl after incorporation of the LNO coating. Additionally, we revealed the in situ passivation effect of LPSCl electrochemical decomposition. When combined, both these phenomena occurring at the first charge cycle result in a stabilized interface, enabling long cyclability of all-solid-state batteries.

• Research Organization: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
• Sponsoring Organization: LG Chem; Shell E&P Co; Sustainable Power and Energy Center (SPEC); National Science Foundation (NSF); USDOE Office of Science (SC)
• Grant/Contract Number: AC02-06CH11357; PT78832; CHE-1338173; ECCS-1542148; AC02-05CH11231; ACI-1548562
• OSTI ID: 1606549
• Alternate ID(s): OSTI ID: 1737586
• Journal Information: ACS Applied Materials and Interfaces, Vol. 11, Issue 46; ISSN 1944-8244
• Publisher: American Chemical Society (ACS)Copyright Statement
• Country of Publication: United States
• Language: English