A Mean-Field Model for Oxygen Reduction Electrocatalytic Activity on High-Entropy Alloys
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A Mean-Field Model for Oxygen Reduction Electrocatalytic Activity on High-Entropy Alloys. / Pedersen, Jack K.; Clausen, Christian M.; Skjegstad, Lars Erik J.; Rossmeisl, Jan.
I: ChemCatChem, Bind 14, Nr. 18, 202200699, 11.08.2022.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - A Mean-Field Model for Oxygen Reduction Electrocatalytic Activity on High-Entropy Alloys
AU - Pedersen, Jack K.
AU - Clausen, Christian M.
AU - Skjegstad, Lars Erik J.
AU - Rossmeisl, Jan
PY - 2022/8/11
Y1 - 2022/8/11
N2 - High-entropy alloys (HEAs) represent near-equimolar points in the middle of a vast composition space of multi-metallic catalysts. Successful modeling of the catalytic activity of these complex materials allows to search this composition space for optimal catalysts. This study shows the effect of approximating the ligand effect of the surrounding atoms around an adsorption site with a mean-field perturbation. Modeling the electrocatalytic activity of the oxygen reduction reaction on the quinary AgIrPdPtRu HEA, it is shown that the extent of such a mean-field approximation is valid up to and including equimolar ternary alloys, corresponding to 60.3 % of the quinary composition space, by comparing to models that consider the ligand effect locally. When extrapolating to make predictions far from near-equimolar compositions, such as for binary alloys, the mean field has been sufficiently perturbed to cause large discrepancies. Here, the local ligand models thus prove more useful for discovering optimal catalysts.
AB - High-entropy alloys (HEAs) represent near-equimolar points in the middle of a vast composition space of multi-metallic catalysts. Successful modeling of the catalytic activity of these complex materials allows to search this composition space for optimal catalysts. This study shows the effect of approximating the ligand effect of the surrounding atoms around an adsorption site with a mean-field perturbation. Modeling the electrocatalytic activity of the oxygen reduction reaction on the quinary AgIrPdPtRu HEA, it is shown that the extent of such a mean-field approximation is valid up to and including equimolar ternary alloys, corresponding to 60.3 % of the quinary composition space, by comparing to models that consider the ligand effect locally. When extrapolating to make predictions far from near-equimolar compositions, such as for binary alloys, the mean field has been sufficiently perturbed to cause large discrepancies. Here, the local ligand models thus prove more useful for discovering optimal catalysts.
KW - ab initio calculations
KW - alloys
KW - electrocatalysis
KW - high-entropy alloys
KW - CATALYSTS
KW - PLATINUM
U2 - 10.1002/cctc.202200699
DO - 10.1002/cctc.202200699
M3 - Journal article
VL - 14
JO - ChemCatChem
JF - ChemCatChem
SN - 1867-3880
IS - 18
M1 - 202200699
ER -
ID: 317438896