Highly dispersed SiOx/Al2O3 catalysts illuminate the reactivity of isolated silanol sites

Mouat, Aidan R.; George, Cassandra; Kobayashi, Takeshi; Pruski, Marek; van Duyne, Richard P.; Marks, Tobin J.; Stair, Peter C.

doi:10.1002/anie.201505452

Highly dispersed SiO_x/Al₂O₃ catalysts illuminate the reactivity of isolated silanol sites

Journal Article · Wed Sep 23 00:00:00 EDT 2015 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201505452· OSTI ID:1227425

Mouat, Aidan R. ^[1]; George, Cassandra ^[1]; Kobayashi, Takeshi ^[2]; Pruski, Marek ^[2]; van Duyne, Richard P. ^[1]; Marks, Tobin J. ^[1]; Stair, Peter C. ^[1]

Northwestern Univ., Evanston, IL (United States)
Iowa State Univ., Ames, IA (United States)

The reaction of γ-alumina with tetraethylorthosilicate (TEOS) vapor at low temperatures selectively yields monomeric SiO_x species on the alumina surface. These isolated (-AlO)₃Si(OH) sites are characterized by PXRD, XPS, DRIFTS of adsorbed NH₃, CO, and pyridine, and ²⁹Si and ²⁷Al DNP-enhanced solid-state NMR spectroscopy. The formation of isolated sites suggests that TEOS reacts preferentially at strong Lewis acid sites on the γ-Al₂O₃ surface, functionalizing the surface with “mild” Brønsted acid sites. As a result, for liquid-phase catalytic cyclohexanol dehydration, these SiO_x sites exhibit up to 3.5-fold higher specific activity than the parent alumina with identical selectivity.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357; FG02-03ER15457; SC0001329; AC02-07CH11358

OSTI ID:: 1227425

Report Number(s):: IS-J--8828

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 45 Vol. 54; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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