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. 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.
| Original language | English |
|---|---|
| Pages (from-to) | 13346-13351 |
| Number of pages | 6 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 54 |
| Issue number | 45 |
| DOIs | |
| Publication status | Published - Nov 1 2015 |
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Keywords
- alcohol dehydration
- atomic layer deposition
- heterogeneous catalysis
- silica-alumina
- solid acid
ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
Cite this
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.
In: Angewandte Chemie - International Edition, Vol. 54, No. 45, 01.11.2015, p. 13346-13351.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Highly Dispersed SiOx/Al2O3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites
AU - Mouat, Aidan R.
AU - George, Cassandra
AU - Kobayashi, Takeshi
AU - Pruski, Marek
AU - Van Duyne, Richard P.
AU - Marks, Tobin J
AU - Stair, Peter C
PY - 2015/11/1
Y1 - 2015/11/1
N2 - 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. 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.
AB - 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. 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.
KW - alcohol dehydration
KW - atomic layer deposition
KW - heterogeneous catalysis
KW - silica-alumina
KW - solid acid
UR - http://www.scopus.com/inward/record.url?scp=84945434809&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84945434809&partnerID=8YFLogxK
U2 - 10.1002/anie.201505452
DO - 10.1002/anie.201505452
M3 - Article
AN - SCOPUS:84945434809
VL - 54
SP - 13346
EP - 13351
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
SN - 1433-7851
IS - 45
ER -