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

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 worki...

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Bibliographic Details
Published in:ACS applied materials & interfaces 2019-11, Vol.11 (46), p.43138-43145
Main Authors: Banerjee, Abhik, Tang, Hanmei, Wang, Xuefeng, Cheng, Ju-Hsiang, Nguyen, Han, Zhang, Minghao, Tan, Darren H. S, Wynn, Thomas A, Wu, Erik A, Doux, Jean-Marie, Wu, Tianpin, Ma, Lu, Sterbinsky, George E, D’Souza, Macwin Savio, Ong, Shyue Ping, Meng, Ying Shirley
Format: Article
Language:English
Subjects:
ab initio molecular dynamics (AIMD)
density functional theory (DFT) calculations
ENERGY STORAGE
interface
interfacial engineering
Li6PS5Cl (LPSCl)
LiNbO3 coating
LiNi0.85Co0.1Al0.05O2 (NCA)
solid electrolyte
solid-state battery
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Summary: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 LiNi0.85Co0.1Al0.05O2 (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. 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.
ISSN:1944-8244
1944-8252
DOI:10.1021/acsami.9b13955