Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study

Apinya Ngoipala; Christian Schott; Valentin Briega-Martos; Minaam Qamar; Matous Mrovec; Sousa Javan Nikkhah; Thorsten O. Schmidt; Lewin Deville; Andrea Capogrosso; Lilian Moumaneix; Tanja Kallio; Arnaud Viola; Frédéric Maillard; Ralf Drautz; Aliaksandr S. Bandarenka; Serhiy Cherevko; Matthias Vandichel; Elena L. Gubanova

doi:10.1002/adma.202410951

Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study

Apinya Ngoipala
, Christian Schott
, Valentin Briega-Martos
, Minaam Qamar
, Matous Mrovec
, Sousa Javan Nikkhah
, Thorsten O. Schmidt
, Lewin Deville
, Andrea Capogrosso
, Lilian Moumaneix
, Tanja Kallio
, Arnaud Viola
, Frédéric Maillard
, Ralf Drautz
, Aliaksandr S. Bandarenka
, Serhiy Cherevko^*
, Matthias Vandichel^*
, Elena L. Gubanova^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › Scientific › peer-review

11 Citations (Scopus)

14 Downloads (Pure)

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.

Original language	English
Article number	2410951
Number of pages	12
Journal	Advanced Materials
Volume	37
Issue number	4
Early online date	4 Dec 2024
DOIs	https://doi.org/10.1002/adma.202410951
Publication status	Published - 29 Jan 2025
MoE publication type	A1 Journal article-refereed

Funding

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. Open access funding enabled and organized by Projekt DEAL.

Keywords

electrochemical scanning tunneling microscopy
molecular dynamics simulations with machine learning potential
online inductively coupled plasma mass spectrometry
palladium hydride formation
proton electroreduction
strain relaxation
surface reconstruction

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10.1002/adma.202410951Licence: CC BY

CHEM_Ngoipala_et_al_Hydride‐Induced_Reconstruction_2025_Advanced_MaterialsFinal published version, 11.6 MBLicence: CC BY

Cite this

Ngoipala, A., Schott, C., Briega-Martos, V., Qamar, M., Mrovec, M., Javan Nikkhah, S., Schmidt, T. O., Deville, L., Capogrosso, A., Moumaneix, L., Kallio, T., Viola, A., Maillard, F., Drautz, R., Bandarenka, A. S., Cherevko, S., Vandichel, M., & Gubanova, E. L. (2025). Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study. Advanced Materials, 37(4), Article 2410951. https://doi.org/10.1002/adma.202410951

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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.",

keywords = "electrochemical scanning tunneling microscopy, molecular dynamics simulations with machine learning potential, online inductively coupled plasma mass spectrometry, palladium hydride formation, proton electroreduction, strain relaxation, surface reconstruction",

author = "Apinya Ngoipala and Christian Schott and Valentin Briega-Martos and Minaam Qamar and Matous Mrovec and \{Javan Nikkhah\}, Sousa and Schmidt, \{Thorsten O.\} and Lewin Deville and Andrea Capogrosso and Lilian Moumaneix and Tanja Kallio and Arnaud Viola and Fr{\'e}d{\'e}ric Maillard and Ralf Drautz and Bandarenka, \{Aliaksandr S.\} and Serhiy Cherevko and Matthias Vandichel and Gubanova, \{Elena L.\}",

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Ngoipala, A, Schott, C, Briega-Martos, V, Qamar, M, Mrovec, M, Javan Nikkhah, S, Schmidt, TO, Deville, L, Capogrosso, A, Moumaneix, L, Kallio, T, Viola, A, Maillard, F, Drautz, R, Bandarenka, AS, Cherevko, S, Vandichel, M & Gubanova, EL 2025, 'Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study', Advanced Materials, vol. 37, no. 4, 2410951. https://doi.org/10.1002/adma.202410951

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AU - Ngoipala, Apinya

AU - Schott, Christian

AU - Briega-Martos, Valentin

AU - Qamar, Minaam

AU - Mrovec, Matous

AU - Javan Nikkhah, Sousa

AU - Schmidt, Thorsten O.

AU - Deville, Lewin

AU - Capogrosso, Andrea

AU - Moumaneix, Lilian

AU - Kallio, Tanja

AU - Viola, Arnaud

AU - Maillard, Frédéric

AU - Drautz, Ralf

AU - Bandarenka, Aliaksandr S.

AU - Cherevko, Serhiy

AU - Vandichel, Matthias

AU - Gubanova, Elena L.

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AB - 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.

KW - electrochemical scanning tunneling microscopy

KW - molecular dynamics simulations with machine learning potential

KW - online inductively coupled plasma mass spectrometry

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ER -

Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study

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HERMES: Breakthrough zero-emissions heat generation with hydrogen-metal systems

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Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study

Abstract

Funding

Keywords

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HERMES: Breakthrough zero-emissions heat generation with hydrogen-metal systems

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