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Mouat AR, George C, Kobayashi T, et al. Highly Dispersed SiO(x)/Al2O3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites. Angew Chem Int Ed Engl. 2015;54(45):13346-51doi: 10.1002/anie.201505452.
Mouat, A. R., George, C., Kobayashi, T., Pruski, M., van Duyne, R. P., Marks, T. J., & Stair, P. C. (2015). Highly Dispersed SiO(x)/Al2O3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites. Angewandte Chemie (International ed. in English), 54(45), 13346-51. https://doi.org/10.1002/anie.201505452
Mouat, Aidan R, et al. "Highly Dispersed SiO(x)/Al2O3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites." Angewandte Chemie (International ed. in English) vol. 54,45 (2015): 13346-51. doi: https://doi.org/10.1002/anie.201505452
Mouat AR, George C, Kobayashi T, Pruski M, van Duyne RP, Marks TJ, Stair PC. Highly Dispersed SiO(x)/Al2O3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites. Angew Chem Int Ed Engl. 2015 Nov 02;54(45):13346-51. doi: 10.1002/anie.201505452. Epub 2015 Sep 23. PMID: 26398359.
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Angew Chem Int Ed Engl. 2015 Nov 02;54(45):13346-51. doi: 10.1002/anie.201505452. Epub 2015 Sep 23.

Highly Dispersed SiO(x)/Al2O3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites.

Angewandte Chemie (International ed. in English)

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

Affiliations

  1. Chemistry Department and the Center for Catalysis and Surface Science, Northwestern University, 2145 Sheridan Rd., Evanston, IL 60208 (USA).
  2. U.S. DOE Ames Laboratory, and Department of Chemistry, Iowa State University, Ames, IA 50011 (USA).
  3. Chemistry Department and the Center for Catalysis and Surface Science, Northwestern University, 2145 Sheridan Rd., Evanston, IL 60208 (USA). [email protected].
  4. Chemistry Department and the Center for Catalysis and Surface Science, Northwestern University, 2145 Sheridan Rd., Evanston, IL 60208 (USA). [email protected].

PMID: 26398359 DOI: 10.1002/anie.201505452

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 NH3, 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-Al2O3 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.

© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Keywords: alcohol dehydration; atomic layer deposition; heterogeneous catalysis; silica-alumina; solid acid

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