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

11 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

Fingerprint

Powders
Oxides
rutile
Single crystal surfaces
catalysts
Vanadium
Catalysts
Molecules
vanadium oxides
Atomic layer deposition
Cyclohexane
atomic layer epitaxy
crystal surfaces
cyclohexane
molecules
single crystals
cycles
Vanadates
oxides
Redox reactions

Keywords

  • Catalysis
  • Interfaces
  • Porous Materials
  • Surfaces

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

Catalysts transform while molecules react : An atomic-scale view. / Feng, Zhenxing; Lu, Junling; Feng, Hao; Stair, Peter C; Elam, Jeffrey W.; Bedzyk, Michael J.

In: Journal of Physical Chemistry Letters, Vol. 4, No. 2, 17.01.2013, p. 285-291.

Research output: Contribution to journalArticle

Feng, Zhenxing ; Lu, Junling ; Feng, Hao ; Stair, Peter C ; Elam, Jeffrey W. ; Bedzyk, Michael J. / Catalysts transform while molecules react : An atomic-scale view. In: Journal of Physical Chemistry Letters. 2013 ; Vol. 4, No. 2. pp. 285-291.
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