Highly Dispersed SiO x /Al 2 O 3 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/ange.201505452

Highly Dispersed SiO _x /Al ₂ O ₃ Catalysts Illuminate the Reactivity of Isolated Silanol Sites (in German)

Journal Article · Wed Sep 23 00:00:00 EDT 2015 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.201505452· OSTI ID:2279222

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

Abstract

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) ₃ Si(OH) sites are characterized by PXRD, XPS, DRIFTS of adsorbed NH ₃ , CO, and pyridine, and ²⁹ Si and ²⁷ Al DNP‐enhanced solid‐state NMR spectroscopy. The formation of isolated sites suggests that TEOS reacts preferentially at strong Lewis acid sites on the γ‐Al ₂ O ₃ surface, functionalizing the surface with “mild” Brønsted acid sites. 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 (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0001329; FG02-03ER15457; AC02-07CH11358; AC02-06CH11357

OSTI ID:: 2279222

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 45 Vol. 127; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: German

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