RT Journal Article T1 Physical delithiation of epitaxial LiCoO2 battery cathodes as a platform for surface electronic structure Investigation A1 Salagre, Elena A1 Segovia, Pilar A1 González Barrio, Miguel Ángel A1 Jugovac, Matteo A1 Moras, Paolo A1 Pis, Igor A1 Bondino, Federica A1 Pearson, Justin A1 Shiwei Wang, Richmond A1 Takeuchi, Ichiro A1 Fuller, Elliot J. A1 Talin, Alec A. A1 Mascaraque Susunaga, Arantzazu A1 Michel, Enrique G. AB We report a novel delithiation process for epitaxial thin films of LiCoO2(001) cathodes using only physical methods, based on ion sputtering and annealing cycles. Preferential Li sputtering followed by annealing produces a surface layer with a Li molar fraction in the range 0.5 < x < 1, characterized by good crystalline quality. This delithiation procedure allows the unambiguous identification of the effects of Li extraction without chemical byproducts and experimental complications caused by electrolyte interaction with the LiCoO2 surface. An analysis by X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) provides a detailed description of the delithiation process and the role of O and Co atoms in charge compensation. We observe the simultaneous formation of Co4+ ions and of holes localized near O atoms upon Li removal, while the surface shows a (2 × 1) reconstruction. The delithiation method described here can be applied to other crystalline battery elements and provide information on their properties that is otherwise difficult to obtain. PB American Chemical Society SN 1944-8244 YR 2023 FD 2023-07-19 LK https://hdl.handle.net/20.500.14352/115776 UL https://hdl.handle.net/20.500.14352/115776 LA eng NO Salagre, E.; Segovia, P.; González-Barrio, M. Á.; Jugovac, M.; Moras, P.; Pis, I.; Bondino, F.; Pearson, J.; Wang, R. S.; Takeuchi, I.; Fuller, E. J.; Talin, A. A.; Mascaraque, A.; Michel, E. G. Physical Delithiation of Epitaxial LiCoO2 Battery Cathodes as a Platform for Surface Electronic Structure Investigation. ACS Appl. Mater. Interfaces 2023, 15 (30), 36224–36232. https://doi.org/10.1021/acsami.3c06147. NO Ministerio de Ciencia e Innovación (España) NO European Commission NO Agencia Estatal de Investigación (España) NO Universidad Autónoma de Madrid NO Comunidad de Madrid NO University of Maryland NO United States Department of Energy DS Docta Complutense RD 20 abr 2025