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Title: Highly dispersed SiO x/Al 2O 3 catalysts illuminate the reactivity of isolated silanol sites

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) 3Si(OH) sites are characterized by PXRD, XPS, DRIFTS of adsorbed NH 3, 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-Al 2O 3 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.

Authors:
 [1];  [1];  [2];  [2];  [1];  [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. 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. doi: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. doi: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 = {2015},
month = {9}
}

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Cited by: 21 works
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