WOx supported on γ-Al2O3 with different morphologies as model catalysts for alkanol dehydration

Shi, Dachuan; Wang, Huamin; Kovarik, Libor; Gao, Feng; Wan, Chuan; Hu, Jian Zhi; Wang, Yong

doi:10.1016/j.jcat.2018.04.004

WO_x supported on γ-Al₂O₃ with different morphologies as model catalysts for alkanol dehydration

Journal Article · Sat Apr 21 00:00:00 EDT 2018 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2018.04.004· OSTI ID:1770170

Shi, Dachuan ^[1]; Wang, Huamin ^[1]; Kovarik, Libor ^[1]; ^[1]; Wan, Chuan ^[1]; ^[1]; Wang, Yong ^[2]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis; Washington State Univ., Pullman, WA (United States)

The distinctive morphological and surface characteristics of platelet-like γ-Al₂O₃ were compared to a regular γ-Al₂O₃. Additionally, γ-Al₂O₃ platelets display dominant (1 1 0) surface facets and higher densities of coordinative unsaturated penta-coordinate Al³⁺ (Al³⁺_penta) sites than regular γ-Al₂O₃, as measured by solid-state magic-angle spinning nuclear magnetic resonance spectroscopy (MAS NMR). Such Al³⁺_penta sites are also the preferred surface anchoring sites for tungsten oxide (WO_x) species consistent with NMR analysis indicating that these sites are consumed upon WO_x adsorption. The higher Al³⁺_penta density on γ-Al₂O₃ platelets leads to greater WO_x dispersion (or smaller WO_x clusters), as demonstrated by scanning transmission electron microscopy and ultraviolet–visible spectroscopy, and WO_x species at intermediate WO_x surface concentration are the most active for the probe reaction of 2-butanol dehydration. WO_x on γ-Al₂O₃ platelets approaches the highest turnover rates at higher surface densities than WO_x on regular γ-Al₂O₃, yet with similar highest rate values for both series of catalysts. This indicates that different Al₂O₃ supports mainly affect the dispersion of supported WO_x rather than the intrinsic reactivity of individual WO_x clusters with similar size.

View Accepted Manuscript (DOE)

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

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1770170

Alternate ID(s):: OSTI ID: 1435890

Report Number(s):: PNNL-SA--132764

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 363; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

2-butanol
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
dehydration
morphology
supported WOx catalyst