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

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [1];  [2];  [2];  [1];  [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Iowa State Univ., Ames, IA (United States)
+ Show Author Affiliations

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.

Research Organization:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
CHE1213235; CHE0923236; AC02-06CH11357; FG02-03ER15457; DMR1121262; EEC0118025/003; SC0001329; AC02-07CH11358
OSTI ID:
1227425
Report Number(s):
IS-J-8828
Journal Information:
Angewandte Chemie (International Edition), Vol. 54, Issue 45; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 61 works
Citation information provided by
Web of Science

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Cited By (10)

NMR Spectroscopic Characterization of Flame‐Made Amorphous Silica‐Alumina for Cyclohexanol and Glyceraldehyde Conversion journal October 2019
Shedding light on the atomic-scale structure of amorphous silica–alumina and its Brønsted acid sites journal January 2019
Probing acid sites in solid catalysts with pyridine UV-Vis spectroscopy journal January 2018
Strong electrostatic adsorption of Pt onto SiO 2 partially overcoated Al 2 O 3 —Towards single atom catalysts journal December 2019
Acidity enhancement through synergy of penta- and tetra-coordinated aluminum species in amorphous silica networks journal January 2020
Atomic Layer Deposition (ALD) as a Way to Prepare New Mixed-Oxide Catalyst Supports: The Case of Alumina Addition to Silica-Supported Platinum for the Selective Hydrogenation of Cinnamaldehyde journal March 2019
Shedding light on the atomic-scale structure of amorphous silica-alumina and its Brønsted acid sites text January 2019
Acidity enhancement through synergy of penta- and tetra-coordinated aluminum species in amorphous silica networks text January 2020
Determining the Surface Structure of Silicated Alumina Catalysts via Isotopic Enrichment and Dynamic Nuclear Polarization Surface-Enhanced NMR Spectroscopy journal October 2017
Three-Dimensional Structure Determination of Surface Sites journal January 2017

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY