@article{32443, author = {Zachary W Lebens-Higgins and Hyeseung Chung and Mateusz J Zuba and Jatinkumar Rana and Yixuan Li and Nicholas V Faenza and Nathalie Pereira and Bryan D McCloskey and Fanny Rodolakis and Wanli Yang and M. M Stanley Whittingham and Glenn G Amatucci and Ying Shirley Meng and Tien-Lin Lee and Louis F. J Piper}, title = {How Bulk Sensitive is Hard X-ray Photoelectron Spectroscopy: Accounting for the Cathode{\textendash}Electrolyte Interface when Addressing Oxygen Redox}, abstract = {
Sensitivity to the {\textquotedblleft}bulk{\textquotedblright} oxygen core orbital makes hard X-ray photoelectron spectroscopy (HAXPES) an appealing technique for studying oxygen redox candidates. Various studies have reported an additional O 1s peak (530{\textendash}531 eV) at high voltages, which has been considered a direct signature of the bulk oxygen redox process. Here, we find the emergence of a 530.4 eV O 1s HAXPES peak for three model cathodes{\textemdash}Li2MnO3, Li-rich NMC, and NMC 442{\textemdash}that shows no clear link to oxygen redox. Instead, the 530.4 eV peak for these three systems is attributed to transition metal reduction and electrolyte decomposition in the near-surface region. Claims of oxygen redox relying on photoelectron spectroscopy must explicitly account for the surface sensitivity of this technique and the extent of the cathode degradation layer.
}, year = {2020}, booktitle = {The Journal of Physical Chemistry Letters}, journal = {The Journal of Physical Chemistry Letters}, series = {The Journal of Physical Chemistry Letters}, volume = {11}, pages = {2106 - 2112}, month = {02/2020}, issn = {1948-7185}, doi = {10.1021/acs.jpclett.0c00229}, language = {eng}, }