Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 117, Issue 51, Pages 26988-26997Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp409601h
Keywords
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Funding
- German Federal Ministry of Education and Research (BMBF) as part of the ReAlSelOx project [033R028B]
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A systematic gas phase-dependence of the electron work function, electron affinity, band bending and the high frequency electrical conductivity of the prospective oxidation catalyst MoVTeNbOx with orthorhombic M1 structure was identified under selective alkane oxidation conditions. The conductivity measured in a fixed bed flow reactor at 1 bar with a noncontact microwave technique and the surface electronic properties studied by in situ X-ray photoelectron spectroscopy at 0.25 mbar were determined at 400 degrees C in 2:1 mixtures of oxygen and the alkanes ethane, propane, and n-butane, respectively. The observed modulation of the surface electron affinity is explained by a gas phase dependent modification of the dipolar structure of the active surface, while the band alignment is interpreted in terms of the formation and modification of the space charge region due to pinning of the Fermi energy to the surface state energy as defined by the V4+/V5+ oxide surface layer. The thus changed charge carrier density in the space charge region gives rise to the observed conductivity response. Consequently, the catalytic system and its working mode can be described as a semiconductor heterostructure comprising the semiconducting bulk phase, a V4+/V5+ oxide termination layer, and the reactive gas phase modulating the Fermi energy of the whole system.
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