What Atomic Positions Determines Reactivity of a Surface? Long‐Range, Directional Ligand Effects in Metallic Alloys
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What Atomic Positions Determines Reactivity of a Surface? Long‐Range, Directional Ligand Effects in Metallic Alloys. / Clausen, Christian M. ; Batchelor, Thomas A. A.; Pedersen, Jack K.; Rossmeisl, Jan.
I: Advanced Science, Bind 8, Nr. 9, 2003357, 2021.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Formidling
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TY - JOUR
T1 - What Atomic Positions Determines Reactivity of a Surface? Long‐Range, Directional Ligand Effects in Metallic Alloys
AU - Clausen, Christian M.
AU - Batchelor, Thomas A. A.
AU - Pedersen, Jack K.
AU - Rossmeisl, Jan
PY - 2021
Y1 - 2021
N2 - Ligand and strain effects can tune the adsorption energy of key reaction intermediates on a catalyst surface to speed up rate‐limiting steps of the reaction. As novel fields like high‐entropy alloys emerge, understanding these effects on the atomic structure level is paramount: What atoms near the binding site determine the reactivity of the alloy surface? By statistical analysis of 2000 density functional theory calculations and subsequent host/guest calculations, it is shown that three atomic positions in the third layer of an fcc(111) metallic structure fourth‐nearest to the adsorption site display significantly increased influence on reactivity over any second or third nearest atomic positions. Subsequently observed in multiple facets and host metals, the effect cannot be explained simply through the d‐band model or a valence configuration model but rather by favorable directions of interaction determined by lattice geometry and the valence difference between host and guest elements. These results advance the general understanding of how the electronic interaction of different elements affect adsorbate–surface interactions and will contribute to design principles for rational catalyst discovery of better, more stable and energy efficient catalysts to be employed in energy conversion, fuel cell technologies, and industrial processes.
AB - Ligand and strain effects can tune the adsorption energy of key reaction intermediates on a catalyst surface to speed up rate‐limiting steps of the reaction. As novel fields like high‐entropy alloys emerge, understanding these effects on the atomic structure level is paramount: What atoms near the binding site determine the reactivity of the alloy surface? By statistical analysis of 2000 density functional theory calculations and subsequent host/guest calculations, it is shown that three atomic positions in the third layer of an fcc(111) metallic structure fourth‐nearest to the adsorption site display significantly increased influence on reactivity over any second or third nearest atomic positions. Subsequently observed in multiple facets and host metals, the effect cannot be explained simply through the d‐band model or a valence configuration model but rather by favorable directions of interaction determined by lattice geometry and the valence difference between host and guest elements. These results advance the general understanding of how the electronic interaction of different elements affect adsorbate–surface interactions and will contribute to design principles for rational catalyst discovery of better, more stable and energy efficient catalysts to be employed in energy conversion, fuel cell technologies, and industrial processes.
U2 - 10.1002/advs.202003357
DO - 10.1002/advs.202003357
M3 - Journal article
C2 - 33977047
VL - 8
JO - Advanced Science
JF - Advanced Science
SN - 2198-3844
IS - 9
M1 - 2003357
ER -
ID: 261046418