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Hydride-induced reconstruction of Pd electrode surfaces: a combined computational and experimental study
Ngoipala, Apinya; Schott,, Christian; Briega-Martos, Valentin; Qamar, Minaam; Mrovec, Matous; Javan Nikkhah, Sousa; Schmidt, Thorsten O.; Deville, Lewin; Capogrosso, Andrea; Moumaneix, Lilian; Kallio, Tanja; Viola, Arnaud; Maillard, Frédéric; Drautz, Ralf; Bandarenka, Aliaksandr S.; Cherevko, Serhiy; Vandichel, Matthias; Gubanova, Elena L.
Date
2024
Abstract
Designing electrocatalysts with optimal activity and selectivity relies on a thorough understanding of the surface structure under reaction conditions. In this study, experimental and computational approaches are combined to elucidate reconstruction processes on low-index Pd surfaces during H-insertion following proton electroreduction. While electrochemical scanning tunneling microscopy clearly reveals pronounced surface roughening and morphological changes on Pd(111), Pd(110), and Pd(100) surfaces during cyclic voltammetry, a complementary analysis using inductively coupled plasma mass spectrometry excludes Pd dissolution as the primary cause of the observed restructuring. Large-scale molecular dynamics simulations further show that these surface alterations are related to the creation and propagation of structural defects as well as phase transformations that take place during hydride formation.
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Description
Publisher
Wiley and Sons Ltd
Citation
Advanced Materials, 2025, 37 (4), 2410951
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Funding Information
A.N., C.S., V.B.-M., and M.Q. contributed equally to this work. This project has received funding from the European Union’s Horizon 2020 research and innovation program under Grant Agreement HERMES No. 952184. A.N. and M.V. acknowledge funding from the Irish Research Council for a Government of Ireland Postgraduate Scholarship, Project ID. GOIPG/2021/867. A.N., S.J.N., and M.V. thank the Irish Centre for High-End Computing (ICHEC) for the provision of computational facilities and support. S.J.N. is grateful for the support by Enterprise Ireland and the European Union’s Horizon 2020 research and innovation programme under Marie Skłodowska-Curie (grant agreement no. 847402, project ID: MF20210297). A.S.B. thanks SFB1625 DFG for the funding. V.B.-M. acknowledges Maja Milosevic (Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IET-2), Forschungszentrum Jülich GmbH) for the discussions and assistance with the on-line dissolution measurements for the Pd nanoparticles.