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

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

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
Journal	Advanced Materials
DOIs	https://doi.org/10.1002/adma.202410951
Publication status	Accepted/In press - 2024

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.202410951

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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. (Accepted/In press). Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study. Advanced Materials. https://doi.org/10.1002/adma.202410951

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title = "Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study",

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.}",

note = "Publisher Copyright: {\textcopyright} 2024 The Author(s). Advanced Materials published by Wiley-VCH GmbH.",

year = "2024",

doi = "10.1002/adma.202410951",

language = "English",

journal = "Advanced Materials",

issn = "0935-9648",

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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 2024, 'Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study', Advanced Materials. https://doi.org/10.1002/adma.202410951

TY - JOUR

T1 - Hydride-Induced Reconstruction of Pd Electrode Surfaces

T2 - A Combined Computational and Experimental Study

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.

PY - 2024

Y1 - 2024

N2 - 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.

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

KW - palladium hydride formation

KW - proton electroreduction

KW - strain relaxation

KW - surface reconstruction

UR - http://www.scopus.com/inward/record.url?scp=85210996401&partnerID=8YFLogxK

U2 - 10.1002/adma.202410951

DO - 10.1002/adma.202410951

M3 - Article

AN - SCOPUS:85210996401

SN - 0935-9648

JO - Advanced Materials

JF - Advanced Materials

ER -

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

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Keywords

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