Rates of levoglucosanol hydrogenolysis over Brønsted and Lewis acid sites on platinum silica-alumina catalysts synthesized by atomic layer deposition

Krishna, Siddarth H.; Zhang, Lifeng; Hermans, Ive; Huber, George W.; Kuech, Thomas F.; Dumesic, James A.

doi:10.1016/j.jcat.2020.05.025

Title: Rates of levoglucosanol hydrogenolysis over Brønsted and Lewis acid sites on platinum silica-alumina catalysts synthesized by atomic layer deposition

Journal Article · Tue May 26 00:00:00 EDT 2020 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2020.05.025· OSTI ID:1778255

^[1]; Zhang, Lifeng ^[1]; Hermans, Ive ^[1]; Huber, George W. ^[1]; Kuech, Thomas F. ^[1];

^[1]

Univ. of Wisconsin, Madison, WI (United States)

Nanoscale coatings of AlO_x were deposited onto SiO₂ using atomic layer deposition (ALD) to synthesize amorphous silica-alumina (SiAl) catalysts, and these catalysts were investigated for levoglucosanol (Lgol) hydrogenolysis. With decreasing Al₂O₃ loading, the ratio of Brønsted to Lewis acid sites, measured by NH₃-TPD and pyridine-FTIR, systematically increases, while the Al coordination, measured by solid state ²⁷Al NMR, decreases. These structural changes correspond to an increasing mass-normalized rate of Lgol hydrogenolysis. We model the mass-normalized reaction rate as the sum of independent contributions from Brønsted and Lewis sites, showing that Brønsted acid sites on ALD-AlO_x/SiO₂ catalysts have a 6-times higher turnover frequency (TOF) than Lewis acid sites on these catalysts. Additionally, Lewis acid sites on ALD-AlO_x/SiO₂ catalysts (potentially related to Al(V) species) have a 4-times higher TOF than Lewis acid sites on bulk γ-Al₂O₃. The overall mass-normalized reactivity of ALD-AlO_x/SiO₂ catalysts is due to Lewis acid sites at the highest Al₂O₃ loading, while it is predominantly due to Brønsted acid sites at the lowest Al₂O₃ loadings. In conclusion, this work provides a new approach to synthesize amorphous SiAls with tunable Brønsted/Lewis acid site ratio and reveals differences in the reactivity of Brønsted and Lewis acid sites on these materials.

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Research Organization:: Univ. of Wisconsin, Madison, WI (United States)

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

Grant/Contract Number:: SC0014058; DGE-1256259

OSTI ID:: 1778255

Alternate ID(s):: OSTI ID: 1775865

Journal Information:: Journal of Catalysis, Vol. 389; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
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Title: Rates of levoglucosanol hydrogenolysis over Brønsted and Lewis acid sites on platinum silica-alumina catalysts synthesized by atomic layer deposition

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