Z. Liang1, A. Baubaid1, M. Radtke2, M. Mellin1, C. Maheu1, S. Maiti3, H. Sclar3 I. Píš4, S. Nappini4, E. Magnano4,5, F. Bondino4, R. Winkler1, R. Hausbrand1 L. Alff1, C. Hess2, B. Markovsky6, D. Aurbach6, W. Jaegermann1, G. Cherkashinin1 1 Institute of Materials Science, Technische Universität Darmstadt, Darmstadt, Germany 2 Department of Chemistry, Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technische Universität Darmstadt, Darmstadt, Germany 3 Department of Chemistry, Institute for Nanotechnology and Advanced Materials (BINA), Bar-llan University, Ramat-Gan, Israel 4 CNR - Istituto Officina dei Materiali (IOM), Trieste, Italy 5 Nanotechnology Research Laboratory, Faculty of Engineering, University of Sydney, Australia 6 Department of Chemistry, BINA - BIU Institute of Nanotechnology and Advanced Materials, INIES - Israel National Institute of Energy Storage (supported by Israel Ministry of Energy and Infrastructures), Bar-Ilan University, Ramat-Gan, Israel e-mail: gennady.cherkashinin@tu-darmstadt.de Acknowledgments - German Science Foundation: The research leading to this result has been supported by German Science Foundation (DFG project numbers of HA 6128/6-1, HE 4515/12-1 and CH 566/4-1) - Elettra Sincrotrone Trieste, CNR-IOM: We acknowledge Elettra Sincrotrone Trieste for providing access to its synchrotron radiation facilities - Diamond Light Source: We acknowledge Diamond Light Source for providing access to synchrotron radiation facilities and for financial support (the project No. SI31579) - Helmholtz Zentrum Berlin: We acknowledge Helmholz Zentrum Berlin for providing access to its synchrotron radiation facilities (granting beam time at BESSY II under application 222-11382). Original paper Z. Liang et al., Adv. Sci. 12, 2413054 (2025); DOI: 10.1002/advs.202413054. Fig. 1 Figure 1. Experimentally determined electron energy band diagrams of (a) as-prepared LiCoPO4 and (b) double-gas treated with SO2 and NH3 in HE-NCM cathodes; the occupied and unoccupied electron states are filled and unfilled, respectively. The Li-O-Li bond is due to Li2O formation; M3d means the Co3d, Ni3d and Mn3d states; EU F, VBMU, ΦeU (ET F, VBMT, ΦeT ), Evac, “U” and “T” are the Fermi level, valence band maximum, work function, vacuum level, untreated and treated cathodes, respectively; ∆μ is the difference in the EU F and ET F; the EF shifts down upon delithiation of the cathodes in (c,d) as shown for the charging state of 4.8 V vs. Li+/Li. (e) Voltage profiles of the untreated (black) and the treated (blue) HE-NCM cathodes. Voltage hysteresis is shown by arrows. The charging/discharging potentials, upon which the electronic properties of the cathodes were probed by XPS, SPES, XAS, are labelled by solid filled circles. The 1 and 2 plateau regions correspond to oxidation of the cations and anion, respectively. (f) Cyclic voltammetry of as-prepared LiCoPO4 thin-film and (g) coated with LIPON solid electrolyte. The CV after the first electrochemical cycle is shown in red. Reproduced with permission under a Creative Commons Attribution-NonCommercial 4.0 International Public License CC BY 4.0 Copyright. Surfaces and Interfaces Elettra Highlights 2024–2025 109
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