Bulk Oxygen Stabilization via Electrode‐Electrolyte Interphase Tailored Surface Activities of Li‐Rich Cathodes

Zhang, Xu; Zhao, Jingteng; Lee, Gi‐Hyeok; Liang, Yuan; Wang, Boya; Liu, Shiqi; Wang, Errui; Yang, Wanli; Yu, Haijun

doi:10.1002/aenm.202202929

Title: Bulk Oxygen Stabilization via Electrode‐Electrolyte Interphase Tailored Surface Activities of Li‐Rich Cathodes

Journal Article · Wed Nov 23 00:00:00 EST 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202202929· OSTI ID:1899715

Zhang, Xu ^[1]; Zhao, Jingteng ^[1]; Lee, Gi‐Hyeok ^[2]; Liang, Yuan ^[1]; Wang, Boya ^[1]; Liu, Shiqi ^[1]; Wang, Errui ^[1]; Yang, Wanli ^[2];

^[1]

Institute of Advanced Battery Materials and Devices Faculty of Materials and Manufacturing Beijing University of Technology Beijing 100124 P. R. China, Key Laboratory of Advanced Functional Materials Ministry of Education Beijing University of Technology Beijing 100124 P. R. China
Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA

Abstract The O3‐type Li‐rich layered oxides (LLOs) are approaching industrial applications as high‐energy cathode materials for Li‐ion batteries (LIBs), however, they suffer from rapid performance decay associated with oxygen activities. The interplay between surface and bulk transformations in LLOs, especially the electrochemical behaviors of oxygen anions, remains elusive. Here, by regulating the surface of an O3‐type LLO (Li _1.13 Mn _0.517 Ni _0.256 Co _0.097 O ₂ ) using an all‐fluorinated electrolyte, an enhanced capacity retention from 57.4% to 85.3% and a suppressed voltage decay from 1.34 mV cycle ⁻¹ to 0.58 mV cycle ⁻¹ within 300 cycles are realized. The performance enhancement is attributed to the thin, uniform, robust, and compact F‐rich cathode‐electrolyte interphase (CEI), which suppresses various types of oxygen‐related surface degradation and, more importantly, stabilizes the bulk oxygen reactions. Through the combined experimental and theoretical studies, this work directly reveals the intriguing association between the surface and bulk oxygen activities and demonstrates that optimizing the interphase is an effective approach for improving the stability of high‐energy battery cathodes involving oxygen redox reactions.

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Sponsoring Organization:: USDOE

OSTI ID:: 1899715

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Vol. 13 Journal Issue: 2; ISSN 1614-6832

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

Country of Publication:: Germany

Language:: English

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