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Catalysts Transform While Molecules React: An Atomic-Scale View.

Zhenxing Feng¹, Junling Lu², Hao Feng²

¹‡Electrochemical Energy Laboratory, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.

The Journal of Physical Chemistry Letters

|August 19, 2015

Summary

This summary is machine-generated.

This study links atomic structure and chemistry of vanadium oxide catalysts on titanium dioxide to their performance in cyclohexane oxidation. Understanding these relationships is key for designing efficient oxide-supported catalysts.

Keywords:

X-ray standing wave atomic-layer deposition infrared spectroscopy oxidative dehydrogenation redox activity titanium dioxide vanadium oxide

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Area of Science:

Surface Science
Catalysis
Materials Chemistry

Background:

Oxide-supported catalysts are crucial for industrial chemical transformations.
Understanding the structure-property-performance relationship at the atomic scale is essential for catalyst design.
Vanadium oxide on titanium dioxide is a model system for studying redox reactions.

Purpose of the Study:

To investigate the atomic-scale structural and chemical properties of vanadium oxide monolayer catalysts on rutile TiO2.
To correlate these properties with catalytic behavior in the oxidative dehydrogenation of cyclohexane.
To establish a general strategy for linking catalyst processing, structure, properties, and performance.

Main Methods:

Atomic layer deposition (ALD) of vanadium oxide on rutile α-TiO2(110) single crystals and powders.
In situ single-crystal X-ray standing wave (XSW) analysis to probe structural changes.
Ex situ X-ray photoelectron spectroscopy (XPS) to determine vanadium oxidation states.
In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to analyze surface species.
Catalytic testing of powder-supported VOx for cyclohexane oxidative dehydrogenation.

Main Results:

Reversible structural changes of vanadium oxide were observed during the redox cycle using XSW.
XPS confirmed V5+ in the oxidized state and predominantly V4+ in the reduced state.
DRIFTS indicated that structural and chemical state changes are linked to the vanadyl group (V═O).
Benzene was identified as the major product in the catalytic oxidation of cyclohexane over VOx/TiO2.

Conclusions:

Atomic-scale insights into vanadium oxide structural and chemical changes during redox cycling on TiO2.
Demonstrated a link between catalyst structure, chemical state, and performance in cyclohexane ODH.
Provided a generalizable strategy for the rational design of oxide-supported catalysts.