期刊
TOPICS IN CATALYSIS
卷 55, 期 5-6, 页码 376-390出版社
SPRINGER/PLENUM PUBLISHERS
DOI: 10.1007/s11244-012-9794-2
关键词
Structure-reactivity relationships; Alloy; Density functional theory; X-ray absorption spectroscopy; Oxygen reduction reaction; Platinum; Rapid screening
资金
- US Department of Energy DOE-BES, Division of Chemical Sciences [FG-02-05ER15686]
- National Science Foundation [CBET 1132777]
- DuPont Corporation
- Camille & Henry Dreyfus Foundation
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1132777] Funding Source: National Science Foundation
The immense phase space of multimetallic materials spanned by structural and compositional degrees of freedom precludes thorough screening for efficient alloy catalysts, even with combinatorial high-throughput experiments or quantum-chemical calculations. Based on X-ray absorption spectroscopy measurements and density functional theory calculations, we have identified critical electronic structure descriptors that govern local chemical reactivity of different sites in metal alloys. These descriptors were used to develop a model that allows us to predict variations in the adsorption energy of various adsorbates on alloy surfaces based on easily accessible physical characteristics of the constituent elements in alloys, mainly their electronegativity, atomic radius, and the spatial extent of valence orbitals. We show that this model, which is grounded on validated theories of chemisorption on metal surfaces, can be used to rapidly screen through a large phase space of alloy catalysts and identify optimal alloys for targeted catalytic transformations. We underline the potential of the electronic structure engineering, relating alloy geometry to its catalytic performance using simple electronic structure descriptors, in catalysis.
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