Electronic structure engineering in heterogeneous catalysis: Identifying novel alloy catalysts based on rapid screening for materials with desired electronic properties

Hongliang Xin, Adam Holewinski, Neil Schweitzer, Eranda Nikolla, Suljo Linic*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

56 Scopus citations

Abstract

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.

Original languageEnglish (US)
Pages (from-to)376-390
Number of pages15
JournalTopics in Catalysis
Volume55
Issue number5-6
DOIs
StatePublished - Jun 1 2012

Keywords

  • Alloy
  • Density functional theory
  • Oxygen reduction reaction
  • Platinum
  • Rapid screening
  • Structure-reactivity relationships
  • X-ray absorption spectroscopy

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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