Structural Identification of ZnxZryOz Catalysts for Cascade Aldolization and Self-Deoxygenation Reactions

Baylon, Rebecca A. L.; Sun, Junming; Kovarik, Libor; Engelhard, Mark; Li, Houqian; Winkelman, Austin D.; Martin, Kevin J.; Wang, Yong

doi:10.1016/j.apcatb.2018.04.051

Title: Structural Identification of Zn_xZr_yO_z Catalysts for Cascade Aldolization and Self-Deoxygenation Reactions

Journal Article · Sun Apr 22 00:00:00 EDT 2018 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2018.04.051· OSTI ID:1434662

Baylon, Rebecca A. L. ^[1]; Sun, Junming ^[1]; Kovarik, Libor ^[2]; Engelhard, Mark ^[2]; Li, Houqian ^[1]; Winkelman, Austin D. ^[1]; Martin, Kevin J. ^[3]; Wang, Yong ^[4]

Washington State Univ., Pullman, WA (United States). The Gene and Linda Voiland School of Chemical Engineering and Bioengineering
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis and Environmental Molecular Sciences Lab.
Archer Daniels Midland Company, Chicago, IL (United States)
Washington State Univ., Pullman, WA (United States). The Gene and Linda Voiland School of Chemical Engineering and Bioengineering; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis

Here, complementary characterizations, such as nitrogen sorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), visible Raman, scanning transmission electron microscopy (STEM) coupled with elemental mapping, NH₃/CO₂ temperature programmed desorption (NH₃/CO₂-TPD), infrared spectroscopic analysis of adsorbed pyridine (Py-IR), and CO_2-IR, have been employed to identify the structure and surface chemistry (i.e., acid-base) of mixed Zn_xZr_yO_z oxide catalysts of varied ratios of Zn/Zr. Atomically dispersed Zn²⁺ species are present in the framework within a thin surface shell (1.5-2.0 nm) of ZrO₂ particles when the Zn/Zr ratio is smaller than 1/10; when the ratio is above this, both atomically dispersed Zn²⁺ and ZnO clusters coexist in mixed Zn_xZr_yO_z oxide catalysts. The presence of ZnO clusters shows no significant side effect but only a slight increase of selectivity to CO₂, caused by steam reforming. The incorporation of atomic Zn²⁺ into the ZrO₂ framework was found to not only passivate strong Lewis acid sites (i.e., Zr-O-Zr) on ZrO₂, but to also generate new Lewis acid-base site pairs with enhanced Lewis basicity on the bridged O (i.e., _{Zr—o$$\curvearrowleft\atop{e\atop—}$$Zn}). In the mixed ketone (i.e., acetone and methyl ethyl ketone (MEK)) reactions, while the passivation of strong acid sites can be correlated to the inhibition of side reactions, such as ketone decomposition and coking, the new Lewis acid-base pairs introduced enhance the cascade aldolization and self-deoxygenation reactions involved in olefin (C₃⁼-C₆⁼) production. More importantly, the surface acid-base properties change with varying Zn/Zr ratios, which in turn affect the cross- and self-condensation reactivity and subsequent distribution of olefins.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; FWP-47319; WSU002206; AC05-RL01830

OSTI ID:: 1434662

Alternate ID(s):: OSTI ID: 1591649

Report Number(s):: PNNL-SA-134337; PII: S0926337318303801; TRN: US1802344

Journal Information:: Applied Catalysis. B, Environmental, Vol. 234; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
09 BIOMASS FUELS
10 SYNTHETIC FUELS
36 MATERIALS SCIENCE
Lewis acid-base pairs
aldolization
ketonization
mixed-metal oxide
oxygenates
olefins

Title: Structural Identification of ZnxZryOz Catalysts for Cascade Aldolization and Self-Deoxygenation Reactions

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Title: Structural Identification of Zn_xZr_yO_z Catalysts for Cascade Aldolization and Self-Deoxygenation Reactions