Self-Organization of 1-Propanol at H-ZSM-5 Brønsted Acid Sites.

Autor:	Kim S; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Lee MS; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Camaioni DM; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Gutiérrez OY; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Glezakou VA; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Govind N; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Huthwelker T; Swiss Light Source, Paul Scherrer Institut (PSI), 5232 Villigen, Switzerland., Zhao R; Department of Chemistry and Catalysis Research Institute, TU München, Lichtenbergstrasse 4, 85748 Garching, Germany., Rousseau R; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Fulton JL; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Lercher JA; Institute for Integrated Catalysis and Physical Science Division, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.; Department of Chemistry and Catalysis Research Institute, TU München, Lichtenbergstrasse 4, 85748 Garching, Germany.
Jazyk:	angličtina
Zdroj:	JACS Au [JACS Au] 2023 Aug 30; Vol. 3 (9), pp. 2487-2497. Date of Electronic Publication: 2023 Aug 30 (Print Publication: 2023).
DOI:	10.1021/jacsau.3c00259
Abstrakt:	In situ Al K-edge X-ray absorption near edge structure (XANES) and Extended X-ray absorption fine structure (EXAFS) spectroscopy in conjunction with ab initio molecular dynamics (AIMD) simulations show that adsorption of 1-propanol alters the structure of the Brønsted acid site through changes in the associated aluminum-oxygen tetrahedron in zeolite H-MFI. The decreasing intensity of the pre-edge signal of the in situ Al K-edge XANES spectra with increasing 1-propanol coverage shows that Al T-sites become more symmetric as the sorbed alcohol molecules form monomers, dimers, and trimers. The adsorption of monomeric 1-propanol on Brønsted acid sites reduces the distortion of the associated Al T-site, shortens the Al-O distance, and causes the formation of a Zundel-like structure. With dimeric and trimeric alcohol clusters, the zeolite proton is fully transferred to the alcohols and the aluminum-oxygen tetrahedron becomes fully symmetric. The subtle changes in Al-K-edge XANES in the presence of sorbate structures, with the use of theory, are used to probe the local zeolite structures and provide a basis to predict the population and chemical state of the sorbed species. Competing Interests: The authors declare no competing financial interest. (© 2023 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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