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Unveiling the High‐valence Oxygen Degradation Across the Delithiated Cathode Surface

Qinghao Li, Qinghao Li, Qi Liang, Hui Zhang, Sichen Jiao, Zengqing Zhuo, Junyang Wang, Qiang Li, Qiang Li, Jienan Zhang, Xiqian Yu

2022Angewandte Chemie International Edition32 citationsDOIOpen Access PDF

Abstract

Abstract Charge compensation on anionic redox reaction (ARR) has been promising to realize extra capacity beyond transition metal redox in battery cathodes. The practical development of ARR capacity has been hindered by high‐valence oxygen instability, particularly at cathode surfaces. However, the direct probe of surface oxygen behavior has been challenging. Here, the electronic states of surface oxygen are investigated by combining mapping of resonant Auger electronic spectroscopy (mRAS) and ambient pressure X‐ray photoelectron spectroscopy (APXPS) on a model LiCoO 2 cathode. The mRAS verified that no high‐valence oxygen can sustain at cathode surfaces, while APXPS proves that cathode electrolyte interphase (CEI) layer evolves and oxidizes upon oxygen gas contact. This work provides valuable insights into the high‐valence oxygen degradation mode across the interface. Oxygen stabilization from surface architecture is proven a prerequisite to the practical development of ARR active cathodes.

Topics & Concepts

CathodeX-ray photoelectron spectroscopyOxygenValence (chemistry)ElectrolyteChemistryChemical physicsRedoxAuger electron spectroscopyMaterials scienceAnalytical Chemistry (journal)Chemical engineeringElectrodeInorganic chemistryPhysical chemistryPhysicsOrganic chemistryNuclear physicsChromatographyEngineeringAdvancements in Battery MaterialsAdvanced battery technologies researchElectrocatalysts for Energy Conversion