Creating Brønsted acidity at the SiO2-Nb2O5 interface

Wolek, Andrew T. Y.; Ardagh, M. Alexander; Pham, Hien N.; Alayoglu, Selim; Datye, Abhaya K.; Notestein, Justin M.

doi:10.1016/j.jcat.2020.10.027

Creating Brønsted acidity at the SiO₂-Nb₂O₅ interface

Journal Article · Mon Nov 09 00:00:00 EST 2020 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2020.10.027· OSTI ID:1849443

^[1]; Ardagh, M. Alexander ^[2]; Pham, Hien N. ^[3]; Alayoglu, Selim ^[4]; Datye, Abhaya K. ^[3]; ^[2]

Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering; Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering
Univ. of New Mexico, Albuquerque, NM (United States). Center for Micro-Engineered Materials. Dept. of Chemical and Biological Engineering
Northwestern Univ., Evanston, IL (United States). Center for Catalysis and Surface Science

Catalytically active acid sites associated with the silica-niobia interface were probed with a series of overcoated SiO₂ on Nb₂O₅ (SiO₂/Nb₂O₅) mixed oxide materials prepared by deposition of tetraethyl orthosilicate onto niobic acid (Nb₂O₅ nH₂O) or calcined niobia (Nb₂O₅). NH₃ TPD and pyridine DRIFTS studies indicated that the speciation of acid sites in the materials evolved as a function of SiO₂ loading, impacting the quantity and stability of Brønsted sites. Catalyst activity was highly dependent on SiO₂ loading in the liquid phase hydroalkoxylation of dihydropyran with n-octanol. At SiO₂ surface densities corresponding to approximately 1 Si per 2 surface Nb, the activity of these catalysts passed through a maximum approximately 20 times higher than the activity of calcined Nb₂O₅. We found that apparent reaction barriers measured over the most active SiO₂/Nb₂O₅ catalysts were 10 kJ/mol lower than those measured over niobic acid, suggesting that the OH features unique to the SiO₂-Nb₂O₅ interface were slightly more reactive than those on niobic acid.

View Accepted Manuscript (DOE)

Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: FG02-03ER15457

OSTI ID:: 1849443

Alternate ID(s):: OSTI ID: 1775870

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: C Vol. 394; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
42 ENGINEERING
Brønsted Acids
Chemistry
Engineering
Hydroalkoxylation
Mixed Oxides
Niobic Acid
Overcoated Materials
Tetrahydropyranylation

Creating Brønsted acidity at the SiO2-Nb2O5 interface

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References (65)

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Creating Brønsted acidity at the SiO₂-Nb₂O₅ interface