Adv. Funct. Mater.: Cationic and Anionic Redox of Battery Cathodes Investigated by Advanced Synchrotron-Based Mapping of Resonant Inelastic X-ray Scattering

Title：

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

Authors：

Chen Cheng^1,2, Zengqing Zhuo³, Shuyuan Chen^1,2, Xi Zhou^1,2, Cheng Yuan^1,2, Zeng Pan⁴, Jinghua Guo³*, and Liang Zhang^1,2*

Institutions：

¹Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China

²Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, 215123, China

³Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA

⁴Institute of 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-metalL-edge (TM-L) mRIXS can eliminate the lineshape distortion in conventional 3d TM-Lfluorescence X-ray absorption spectra and investigate the cationic redox quantitatively. Moreover, O-KmRIXS 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.

IF：

19.00

Link：

https://onlinelibrary.wiley.com/doi/10.1002/adfm.202403442