Chemical Grafting of Highly Dispersed VOx/CeO2 for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation

Sudduth, Berlin; Sun, Junming; Wang, Yong

doi:10.1007/s10562-021-03862-8

Title: Chemical Grafting of Highly Dispersed VO_x/CeO₂ for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation

Journal Article · 04 January 2022 · Catalysis Letters

DOI: https://doi.org/10.1007/s10562-021-03862-8 · OSTI ID:2283978

Sudduth, Berlin ^[1]; Sun, Junming ^[1]; Wang, Yong ^[2]

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

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 VO_x 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 VO_x/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 VO_x species (i.e., monomers and dimers).

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2283978

Report Number(s):: PNNL-SA--183700

Journal Information:: Catalysis Letters, Journal Name: Catalysis Letters Journal Issue: 10 Vol. 152; ISSN 1011-372X

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Chemical Grafting of Highly Dispersed VOx/CeO2 for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation

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Title: Chemical Grafting of Highly Dispersed VO_x/CeO₂ for Increased Catalytic Activity in Methanol Oxidative Dehydrogenation