Proof of Equivalent Catalytic Functionality upon Photon-Induced and Thermal Activation of Supported Isolated Vanadia Species in Methanol Oxidation
Abstract
Abstract In this study, evidence is provided that isolated surface vanadia (VO 4 ) species on SiO 2 can similarly act as a thermal heterogeneous catalyst and as a heterogeneous photocatalyst. Structurally identical surface VO 4 species catalyze the selective oxidation of methanol both by thermal activation and by UV‐light induction. Selectivity to formaldehyde appears to be unity. For the photocatalytic reaction at room temperature, formaldehyde desorption is rate limiting. With larger agglomerates or V 2 O 5 nanoparticles, on the contrary, only the thermal reaction is feasible. This is tentatively attributed to the different positions of electronic states (HOMO/LUMO, valence/conduction band) on the electrochemical energy scale owing to the quantum size effect. Besides providing new fundamental insight into the mode of action of nanosized photocatalysts, our results demonstrate that tuning the photocatalytic reactivity of supported transition‐metal oxides by adjusting the degree of agglomeration is feasible.
- Authors:
-
- Univ. of Rostock (Germany); Ruhr Univ., Bochum (Germany)
- Lehigh Univ., Bethlehem, PA (United States)
- Max Planck Society, Ruhr (Germany)
- Universität Duisburg-Essen (Germany)
- Ruhr Univ., Bochum (Germany)
- Univ. of Rostock (Germany)
- Publication Date:
- Research Org.:
- Georgia Inst. of Technology, Atlanta, GA (United States) Energy Frontier Research Center (EFRC) Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1470292
- Alternate Identifier(s):
- OSTI ID: 1434221
- Grant/Contract Number:
- SC0012577
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 11; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; oxidation; photocatalysis; quantum size effect; structure–activity relationships; vanadium
Citation Formats
Kortewille, Bianca, Wachs, Israel E., Cibura, Niklas, Pfingsten, Oliver, Bacher, Gerd, Muhler, Martin, and Strunk, Jennifer. Proof of Equivalent Catalytic Functionality upon Photon-Induced and Thermal Activation of Supported Isolated Vanadia Species in Methanol Oxidation. United States: N. p., 2018.
Web. doi:10.1002/cctc.201800311.
Kortewille, Bianca, Wachs, Israel E., Cibura, Niklas, Pfingsten, Oliver, Bacher, Gerd, Muhler, Martin, & Strunk, Jennifer. Proof of Equivalent Catalytic Functionality upon Photon-Induced and Thermal Activation of Supported Isolated Vanadia Species in Methanol Oxidation. United States. https://doi.org/10.1002/cctc.201800311
Kortewille, Bianca, Wachs, Israel E., Cibura, Niklas, Pfingsten, Oliver, Bacher, Gerd, Muhler, Martin, and Strunk, Jennifer. Wed .
"Proof of Equivalent Catalytic Functionality upon Photon-Induced and Thermal Activation of Supported Isolated Vanadia Species in Methanol Oxidation". United States. https://doi.org/10.1002/cctc.201800311. https://www.osti.gov/servlets/purl/1470292.
@article{osti_1470292,
title = {Proof of Equivalent Catalytic Functionality upon Photon-Induced and Thermal Activation of Supported Isolated Vanadia Species in Methanol Oxidation},
author = {Kortewille, Bianca and Wachs, Israel E. and Cibura, Niklas and Pfingsten, Oliver and Bacher, Gerd and Muhler, Martin and Strunk, Jennifer},
abstractNote = {Abstract In this study, evidence is provided that isolated surface vanadia (VO 4 ) species on SiO 2 can similarly act as a thermal heterogeneous catalyst and as a heterogeneous photocatalyst. Structurally identical surface VO 4 species catalyze the selective oxidation of methanol both by thermal activation and by UV‐light induction. Selectivity to formaldehyde appears to be unity. For the photocatalytic reaction at room temperature, formaldehyde desorption is rate limiting. With larger agglomerates or V 2 O 5 nanoparticles, on the contrary, only the thermal reaction is feasible. This is tentatively attributed to the different positions of electronic states (HOMO/LUMO, valence/conduction band) on the electrochemical energy scale owing to the quantum size effect. Besides providing new fundamental insight into the mode of action of nanosized photocatalysts, our results demonstrate that tuning the photocatalytic reactivity of supported transition‐metal oxides by adjusting the degree of agglomeration is feasible.},
doi = {10.1002/cctc.201800311},
journal = {ChemCatChem},
number = 11,
volume = 10,
place = {United States},
year = {Wed Feb 28 00:00:00 EST 2018},
month = {Wed Feb 28 00:00:00 EST 2018}
}
Web of Science
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Works referencing / citing this record:
Photocatalytic Methanol Oxidation by Supported Vanadium Oxide Species: Influence of Support and Degree of Oligomerization: Photocatalytic Methanol Oxidation by Supported Vanadium Oxide Species: Influence of Support and Degree of Oligomerization
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