Catalysts transform while molecules react: An atomic-scale view

Zhenxing Feng, Junling Lu, Hao Feng, Peter C. Stair, Jeffrey W. Elam, Michael J. Bedzyk

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

We explore how the atomic-scale structural and chemical properties of an oxide-supported monolayer (ML) catalyst are related to catalytic behavior. This case study is for vanadium oxide deposited on a rutile α-TiO 2(110) single-crystal surface by atomic layer deposition (ALD) undergoing a redox reaction cycle in the oxidative dehydrogenation (ODH) of cyclohexane. For measurements that require a greater effective surface area, we include a comparative set of ALD-processed rutile powder samples. In situ single-crystal X-ray standing wave (XSW) analysis shows a reversible vanadium oxide structural change through the redox cycle. Ex situ X-ray photoelectron spectroscopy (XPS) shows that V cations are 5+ in the oxidized state and primarily 4+ in the reduced state for both the (110) single-crystal surface and the multifaceted surfaces of the powder sample. In situ diffuse reflectance infrared Fourier transform spectroscopy, which could only achieve a measurable signal level from the powder sample, indicates that these structural and chemical state changes are associated with the change of the VO vanadyl group. Catalytic tests on the powder-supported VOx revealed benzene as the major product. This study not only provides atomic-scale models for cyclohexane molecules interacting with V sites on the rutile surface but also demonstrates a general strategy for linking the processing, structure, properties, and performance of oxide-supported catalysts.

Original languageEnglish
Pages (from-to)285-291
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume4
Issue number2
DOIs
Publication statusPublished - Jan 17 2013

Keywords

  • Catalysis
  • Interfaces
  • Porous Materials
  • Surfaces

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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