Chemical Grafting of Highly Dispersed VOx/CeO2 for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation
Abstract
Vanadia supported on well-defned ceria nanocubes are synthesized at various loadings using a liquid-phase chemical grafting technique and are compared to those prepared using traditional incipient wetness impregnation. Raman and IR characterization reveal that, as vanadia loading is increased to near monolayer coverage, vanadia deposited using grafting shows greatly enhanced dispersion (i.e., improved VOx monomer/dimer distribution). Methanol is used as a probe molecule to explore the redox behavior of the catalysts. IR and temperature programmed desorption of methanol show increased CO2 formation occurs on the bare ceria support and increasing the dispersion of vanadia promotes dehydrogenation to formaldehyde due to the inhibited oxygen vacancy formation on VOx/CeO2. Hydrogen temperature programmed reduction demonstrates that the catalyst reducibility and formation of surface oxygen vacancy are directly related to the degree of vanadia oligomerization. In conclusion, the samples prepared using grafting exhibit superior catalytic performance for methanol oxidative dehydrogenation to formaldehyde compared to the impregnated samples, due to the presence of highly dispersed VOx species (i.e., monomers and dimers).
- Authors:
-
- Washington State Univ., Pullman, WA (United States)
- Washington State Univ., Pullman, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Institute for Integrated Catalysis
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
- OSTI Identifier:
- 2283978
- Report Number(s):
- PNNL-SA-183700
Journal ID: ISSN 1011-372X
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Catalysis Letters
- Additional Journal Information:
- Journal Volume: 152; Journal Issue: 10; Journal ID: ISSN 1011-372X
- Publisher:
- Springer
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ceria; Supported VOx catalysts; Chemical grafting; Methanol; Oxidative dehydrogenation
Citation Formats
Sudduth, Berlin, Sun, Junming, and Wang, Yong. Chemical Grafting of Highly Dispersed VOx/CeO2 for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation. United States: N. p., 2022.
Web. doi:10.1007/s10562-021-03862-8.
Sudduth, Berlin, Sun, Junming, & Wang, Yong. Chemical Grafting of Highly Dispersed VOx/CeO2 for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation. United States. https://doi.org/10.1007/s10562-021-03862-8
Sudduth, Berlin, Sun, Junming, and Wang, Yong. Tue .
"Chemical Grafting of Highly Dispersed VOx/CeO2 for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation". United States. https://doi.org/10.1007/s10562-021-03862-8. https://www.osti.gov/servlets/purl/2283978.
@article{osti_2283978,
title = {Chemical Grafting of Highly Dispersed VOx/CeO2 for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation},
author = {Sudduth, Berlin and Sun, Junming and Wang, Yong},
abstractNote = {Vanadia supported on well-defned ceria nanocubes are synthesized at various loadings using a liquid-phase chemical grafting technique and are compared to those prepared using traditional incipient wetness impregnation. Raman and IR characterization reveal that, as vanadia loading is increased to near monolayer coverage, vanadia deposited using grafting shows greatly enhanced dispersion (i.e., improved VOx monomer/dimer distribution). Methanol is used as a probe molecule to explore the redox behavior of the catalysts. IR and temperature programmed desorption of methanol show increased CO2 formation occurs on the bare ceria support and increasing the dispersion of vanadia promotes dehydrogenation to formaldehyde due to the inhibited oxygen vacancy formation on VOx/CeO2. Hydrogen temperature programmed reduction demonstrates that the catalyst reducibility and formation of surface oxygen vacancy are directly related to the degree of vanadia oligomerization. In conclusion, the samples prepared using grafting exhibit superior catalytic performance for methanol oxidative dehydrogenation to formaldehyde compared to the impregnated samples, due to the presence of highly dispersed VOx species (i.e., monomers and dimers).},
doi = {10.1007/s10562-021-03862-8},
journal = {Catalysis Letters},
number = 10,
volume = 152,
place = {United States},
year = {Tue Jan 04 00:00:00 EST 2022},
month = {Tue Jan 04 00:00:00 EST 2022}
}
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