Work Function and High-Coverage Adsorption Energy as Hydrogen-Evolution Descriptors on Ag-Au-Pd-Pt Alloys
Abstract
Hydrogen-evolution activity is commonly rationalized through hydrogen adsorption energies and the Sabatier principle, yet this descriptor picture becomes ambiguous on multimetallic surfaces, where each composition exposes a distribution of local adsorption environments. Here we investigate whether the bare-surface work function, previously shown to add predictive information for monometallic surfaces, remains an activity descriptor for compositionally complex surfaces. We test this on three combinatorial Ag-Au-Pd-Pt thin-film materials libraries screened for acidic hydrogen evolution by scanning electrochemical cell microscopy. Graph neural networks provide adsorption-energy distributions and work functions for each measured composition. A work-function-only model explained most of the activity variation (mean R2log = 0.903), as did a coverage-corrected adsorption model (mean R2log = 0.955), outperforming dilute adsorption (mean R2log = 0.758). Combining work function and coverage-corrected adsorption yielded the highest fit quality (mean R2log = 0.969), but only a small gain over coverage-corrected adsorption alone. For these four metals the coverage-corrected adsorption energy and work function follow a similar trend, producing similar activity rankings, hence including both adds little beyond either one individually, although both are strong predictors.
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BibTeX
@misc{liasi2026work,
title = {{Work Function and High-Coverage Adsorption Energy as Hydrogen-Evolution Descriptors on Ag-Au-Pd-Pt Alloys}},
author = {Zacharias Liasi and Ridha Zerdoumi and Felix Thelen and Geovane Arruda de Oliveira and Rico Zehl and Natalia Pukhareva and Leonardo H. Morais and Henrik H. Kristoffersen and Alfred Ludwig and Wolfgang Schuhmann and Jan Rossmeisl},
howpublished = {arXiv},
year = {2026},
month = aug,
doi = {10.48550/arxiv.2608.28347},
eprint = {2608.28347},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2608.28347},
}
RIS
TY - UNPB
TI - Work Function and High-Coverage Adsorption Energy as Hydrogen-Evolution Descriptors on Ag-Au-Pd-Pt Alloys
AU - Zacharias Liasi
AU - Ridha Zerdoumi
AU - Felix Thelen
AU - Geovane Arruda de Oliveira
AU - Rico Zehl
AU - Natalia Pukhareva
AU - Leonardo H. Morais
AU - Henrik H. Kristoffersen
AU - Alfred Ludwig
AU - Wolfgang Schuhmann
AU - Jan Rossmeisl
PY - 2026
DA - 2026/08/28
PB - arXiv
DO - 10.48550/arxiv.2608.28347
UR - https://arxiv.org/abs/2608.28347
AB - Hydrogen-evolution activity is commonly rationalized through hydrogen adsorption energies and the Sabatier principle, yet this descriptor picture becomes ambiguous on multimetallic surfaces, where each composition exposes a distribution of local adsorption environments. Here we investigate whether the bare-surface work function, previously shown to add predictive information for monometallic surfaces, remains an activity descriptor for compositionally complex surfaces. We test this on three combinatorial Ag-Au-Pd-Pt thin-film materials libraries screened for acidic hydrogen evolution by scanning electrochemical cell microscopy. Graph neural networks provide adsorption-energy distributions and work functions for each measured composition. A work-function-only model explained most of the activity variation (mean R^2_log = 0.903), as did a coverage-corrected adsorption model (mean R^2_log = 0.955), outperforming dilute adsorption (mean R^2_log = 0.758). Combining work function and coverage-corrected adsorption yielded the highest fit quality (mean R^2_log = 0.969), but only a small gain over coverage-corrected adsorption alone. For these four metals the coverage-corrected adsorption energy and work function follow a similar trend, producing similar activity rankings, hence including both adds little beyond either one individually, although both are strong predictors.
ER -