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

Journal Article · · Advanced Energy Materials
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  1. Beijing University of Technology (China)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

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 (Li1.13Mn0.517Ni0.256Co0.097O2) 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. Finally, 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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
2422652
Alternate ID(s):
OSTI ID: 1899715
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 2 Vol. 13; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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