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

机译:Bulk Oxygen Stabilization via Electrode-Electrolyte Interphase Tailored Surface Activities of Li-Rich Cathodes

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摘要

The O3-type Li-rich layered oxides (LLOs) are approaching industrial applicationsas 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, especiallythe electrochemical behaviors of oxygen anions, remains elusive. Here, byregulating the surface of an O3-type LLO (Li_(1.13)Mn_(0.517)Ni_(0.256)Co_(0.097)O_2) using anall-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) within300 cycles are realized. The performance enhancement is attributed to the thin,uniform, robust, and compact F-rich cathode-electrolyte interphase (CEI), whichsuppresses various types of oxygen-related surface degradation and, moreimportantly, stabilizes the bulk oxygen reactions. Through the combined experimentaland theoretical studies, this work directly reveals the intriguing associationbetween the surface and bulk oxygen activities and demonstrates thatoptimizing the interphase is an effective approach for improving the stability ofhigh-energy battery cathodes involving oxygen redox reactions.

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