Computational Criteria for Hydrogen Evolution Activity on Ligand-Protected Au25-Based Nanoclusters
López-Estrada, O., Mammen, N., Laverdure, L., Melander, M. M., Häkkinen, H., & Honkala, K. (2023). Computational Criteria for Hydrogen Evolution Activity on Ligand-Protected Au25-Based Nanoclusters. ACS Catalysis, 13(13), 8997-9006. https://doi.org/10.1021/acscatal.3c01065
Julkaistu sarjassa
ACS CatalysisTekijät
Päivämäärä
2023Oppiaine
Nanoscience CenterResurssiviisausyhteisöFysikaalinen kemiaNanoscience CenterSchool of Resource WisdomPhysical ChemistryTekijänoikeudet
© 2023 The Authors. Published by American Chemical Society
The hydrogen evolution reaction (HER) is a critical reaction in addressing climate change; however, it requires catalysts to be generated on an industrial scale. Nanomaterials offer several advantages over conventional HER catalysts, including the possibility of atomic precision in tailoring the intrinsic activity. Ligand-protected metal clusters, such as the thiolate-protected MAu24(SR)18 (where M is Au, Cu, Pd), are of particular interest as not only are they electrocatalytically active toward HER, but the charge state and composition can be precisely tuned. Here, we present a comprehensive computational study examining how the charge state and dopants affect the catalytic activity of [MAu24(SCH3)18]q toward the Volmer step of the HER. Assuming an adsorbed hydrogen atom to be the key intermediate, then, according to the Sabatier principle, the H adsorption energy should be nearly thermoneutral for an ideal HER catalyst. Our results show that adsorption energies alone are an insufficient criterion to identify a promising catalytic material; experimentally relevant redox potentials, the corresponding catalyst’s charge states, and the kinetic barriers should also be considered. Notably, this work explains the relative activity of MAu24(SR)18 (M = Au, Cu, Pd) clusters reported by Kumar et al. (Nanoscale 2020, 12, 9969). Our results validate a more thorough computational approach that includes charge and redox potential to understand and screen electrocatalytically active nanoclusters.
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Julkaisija
American Chemical Society (ACS)ISSN Hae Julkaisufoorumista
2155-5435Asiasanat
Julkaisu tutkimustietojärjestelmässä
https://converis.jyu.fi/converis/portal/detail/Publication/183935381
Metadata
Näytä kaikki kuvailutiedotKokoelmat
Rahoittaja(t)
Suomen AkatemiaRahoitusohjelmat(t)
Akatemiahanke, SA; Muut, SA; Tutkijatohtori, SA; Akatemiatutkija, SALisätietoja rahoituksesta
This work was supported by the Academy of Finland (Grant Nos. 351582, 317739, 351583, 332290, 338228). Computational resources were provided by the CSC-IT Center for Science, Espoo, Finland.Lisenssi
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