Highly dispersed SiOx/Al2O3 catalysts illuminate the reactivity of isolated silanol sites
Abstract
The reaction of γ-alumina with tetraethylorthosilicate (TEOS) vapor at low temperatures selectively yields monomeric SiOx 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 SiOx sites exhibit up to 3.5-fold higher specific activity than the parent alumina with identical selectivity.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Iowa State Univ., Ames, IA (United States)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1227425
- Report Number(s):
- IS-J-8828
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- CHE1213235; CHE0923236; AC02-06CH11357; FG02-03ER15457; DMR1121262; EEC0118025/003; SC0001329; AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 54; Journal Issue: 45; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Mouat, Aidan R., George, Cassandra, Kobayashi, Takeshi, Pruski, Marek, van Duyne, Richard P., Marks, Tobin J., and Stair, Peter C. Highly dispersed SiOx/Al2O3 catalysts illuminate the reactivity of isolated silanol sites. United States: N. p., 2015.
Web. doi:10.1002/anie.201505452.
Mouat, Aidan R., George, Cassandra, Kobayashi, Takeshi, Pruski, Marek, van Duyne, Richard P., Marks, Tobin J., & Stair, Peter C. Highly dispersed SiOx/Al2O3 catalysts illuminate the reactivity of isolated silanol sites. United States. https://doi.org/10.1002/anie.201505452
Mouat, Aidan R., George, Cassandra, Kobayashi, Takeshi, Pruski, Marek, van Duyne, Richard P., Marks, Tobin J., and Stair, Peter C. Wed .
"Highly dispersed SiOx/Al2O3 catalysts illuminate the reactivity of isolated silanol sites". United States. https://doi.org/10.1002/anie.201505452. https://www.osti.gov/servlets/purl/1227425.
@article{osti_1227425,
title = {Highly dispersed SiOx/Al2O3 catalysts illuminate the reactivity of isolated silanol sites},
author = {Mouat, Aidan R. and George, Cassandra and Kobayashi, Takeshi and Pruski, Marek and van Duyne, Richard P. and Marks, Tobin J. and Stair, Peter C.},
abstractNote = {The reaction of γ-alumina with tetraethylorthosilicate (TEOS) vapor at low temperatures selectively yields monomeric SiOx 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 SiOx sites exhibit up to 3.5-fold higher specific activity than the parent alumina with identical selectivity.},
doi = {10.1002/anie.201505452},
journal = {Angewandte Chemie (International Edition)},
number = 45,
volume = 54,
place = {United States},
year = {Wed Sep 23 00:00:00 EDT 2015},
month = {Wed Sep 23 00:00:00 EDT 2015}
}
Web of Science
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