Cationic and Anionic Redox of Battery Cathodes Investigated by Advanced Synchrotron‐Based Mapping of Resonant Inelastic X‐ray Scattering

Cheng, Chen; Zhuo, Zengqing; Chen, Shuyuan; Zhou, Xi; Yuan, Cheng; Zeng, Pan; Guo, Jinghua; Zhang, Liang

doi:10.1002/adfm.202403442

Title: Cationic and Anionic Redox of Battery Cathodes Investigated by Advanced Synchrotron‐Based Mapping of Resonant Inelastic X‐ray Scattering

Journal Article · 17 April 2024 · Advanced Functional Materials

DOI: https://doi.org/10.1002/adfm.202403442 · OSTI ID:2338232

Cheng, Chen ^[1]; Zhuo, Zengqing ^[2]; Chen, Shuyuan ^[1]; Zhou, Xi ^[1]; Yuan, Cheng ^[1]; Zeng, Pan ^[3];

^[2]; Zhang, Liang ^[1]

Institute of Functional Nano &, Soft Materials (FUNSOM) Soochow University 199 Ren'ai Road Suzhou 215123 China, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University 199 Ren'ai Road Suzhou 215123 China
Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
Institute for Advanced Study School of Mechanical Engineering Chengdu University Chengdu 610106 China

Abstract Redox reaction builds the foundation stone for the energy density of rechargeable battery cathodes. Probing and understanding the redox reaction behavior is crucial, but also extremely formidable, which requires individual and reliable detection of cationic and anionic redox states. Fortunately, the recently developed ultra‐high‐efficiency mapping of resonant inelastic X‐ray scattering (mRIXS) has emerged as a powerful tool to probe the battery chemistry states. Here, the latest advances of employing advanced mRIXS is summarized to investigate the cationic and anionic redox mechanism of battery cathodes during electrochemical operation. Owing to the new dimension of information along the emission energy and high sensitivity to valence 3d states, 3d transition‐metal L ‐edge (TM‐ L ) mRIXS can eliminate the lineshape distortion in conventional 3d TM‐ L fluorescence X‐ray absorption spectra and investigate the cationic redox quantitatively. Moreover, O‐ K mRIXS could fingerprint the intrinsic oxidized lattice oxygen states and quantify the oxygen redox (OR) reversibility, thus demystifying the controversy in traditional wisdom. In addition, different modification strategies coupled with underlying mechanisms for regulating the activity and reversibility of OR utilizing mRIXS are also summarized. This review provides valuable guidance for further exploration of underlying reaction mechanisms of battery cathodes by mRIXS, along with both technological and scientific improvements.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2338232

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials; ISSN 1616-301X

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

Country of Publication:: Germany

Language:: English

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