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Deciphering Interfacial Chemical and Electrochemical Reactions of Sulfide-Based All-Solid-State Batteries

Journal Article · · Advanced Energy Materials
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  1. Univ. of Western Ontario, London, ON (Canada). Dept. of Mechanical and Materials Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Univ. of Western Ontario, London, ON (Canada). Dept. of Materials Science and Engineering
  4. Glabat Solid‐State Battery Inc., London, ON (Canada)
  5. China Automotive Battery Research Institute Co., Ltd., Beijing (China)
+ Show Author Affiliations

Large interfacial resistance resulting from interfacial reactions is widely acknowledged as one of the main challenges in sulfide electrolytes (SEs)-based all-solid-state lithium batteries (ASSLBs). However, the root cause of the large interfacial resistance between the SEs and typical layered oxide cathodes is not fully understood yet. Here we deciphered that interfacial oxygen loss from single-crystal LiNi0.5Mn0.3Co0.2O2 (SC-NMC532) chemically oxidizes Li10GeP2S12, generating oxygen-containing interfacial species. Meanwhile, the interfacial oxygen loss also induces a structural change of oxide cathodes (layered-to-rocksalt). Besides, the high operation voltage can electrochemically oxidize SEs to form non-oxygen species (e.g. polysulfides). These chemically and electrochemically oxidized species, together with the interfacial structural change, are responsible for the large interfacial resistance at the cathode interface. More importantly, the widely adopted interfacial coating strategy is effective in suppressing chemically oxidized oxygen-containing species and mitigating the coincident interfacial structural change but is unable to prevent electrochemically induced non-oxygen species. These findings provide a deeper insight into the large interfacial resistance between the typical SE and layered oxide cathodes, which may be of assistance for the rational interface design of SE-based ASSLBs in future.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Natural Sciences and Engineering Research Council of Canada; Canada Research Chair Program; Canada Foundation for Innovation; Ontario Research Fund
Grant/Contract Number:
SC0012704
OSTI ID:
1784477
Alternate ID(s):
OSTI ID: 1781990
Report Number(s):
BNL--221398-2021-JAAM
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 24 Vol. 11; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
Li10GeP2S12
all-solid-state lithium batteries
interfacial coating
interfacial oxygen loss
single-crystal LiNi0.5Mn0.3Co0.2O2