Li Qingtian, Lebens-Higgins Zachary W, Li Yixuan, Meng Ying Shirley, Chuang Yi-de, Piper Louis F J, Liu Zhi, Yang Wanli
State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
J Phys Chem Lett. 2021 Feb 4;12(4):1138-1143. doi: 10.1021/acs.jpclett.0c03639. Epub 2021 Jan 21.
The characterization of oxidized oxygen states through high-efficiency mapping of resonant inelastic X-ray scattering (mRIXS) has become a crucial approach for studying the oxygen redox activities in high-energy battery cathodes. However, this approach has been recently challenged due to the concern of irradiation damage. Here we revisited a typical Li-rich electrode, LiNiMnCoO, in both lithiated and delithiated states and evaluated the X-ray irradiation effect in the lengthy mRIXS experiments. Our results show that irradiation cannot introduce any oxidized oxygen feature, and the features of oxidized oxygen are weakened with a high X-ray dose. The results confirm again that mRIXS detects the intrinsic oxidized oxygen state in battery electrodes. However, the distinct irradiation effects in different systems imply that irradiation could selectively target the least stable elemental or chemical states, which should be analyzed with caution in the study of active chemical states.
通过共振非弹性X射线散射(mRIXS)的高效映射来表征氧化态氧,已成为研究高能电池阴极中氧氧化还原活性的关键方法。然而,由于对辐照损伤的担忧,这种方法最近受到了挑战。在这里,我们重新研究了一种典型的富锂电极LiNiMnCoO,分别处于锂化和脱锂状态,并在长时间的mRIXS实验中评估了X射线辐照效应。我们的结果表明,辐照不会引入任何氧化态氧特征,并且随着高X射线剂量,氧化态氧的特征会减弱。结果再次证实,mRIXS检测到的是电池电极中固有的氧化态氧。然而,不同系统中明显的辐照效应表明,辐照可能会选择性地针对最不稳定的元素或化学状态,在研究活性化学状态时应谨慎分析。