Phosphonate‐Modified UiO‐66 Brønsted Acid Catalyst and Its Use in Dehydra‐Decyclization of 2‐Methyltetrahydrofuran to Pentadienes
[1];
[4]
- Department of Chemical Engineering and Materials Science University of Minnesota 421 Washington Ave SE Minneapolis MN 55455 USA
- Department of Chemical Engineering University of California 10 Mesa Road Santa Barbara CA 93106 USA
- Department of Chemical &, Biomolecular Engineering University of Delaware 221 Academy Street Newark DE 19716 USA
- Department of Chemical Engineering and Materials Science University of Minnesota 421 Washington Ave SE Minneapolis MN 55455 USA, Department of Chemical and Biomolecular Engineering Johns Hopkins University 3400 N. Charles Street Baltimore MD 21218 USA, Applied Physics Laboratory Johns Hopkins University 11100 Johns Hopkins Road Laurel MD 20723 USA
Abstract Phosphorus‐modified all‐silica zeolites exhibit activity and selectivity in certain Brønsted acid catalyzed reactions for biomass conversion. In an effort to achieve similar performance with catalysts having well‐defined sites, we report the incorporation of Brønsted acidity to metal–organic frameworks with the UiO‐66 topology, achieved by attaching phosphonic acid to the 1,4‐benzenedicarboxylate ligand and using it to form UiO‐66‐PO 3 H 2 by post‐synthesis modification. Characterization reveals that UiO‐66‐PO 3 H 2 retains stability similar to UiO‐66, and exhibits weak Brønsted acidity, as demonstrated by titrations, alcohol dehydration, and dehydra‐decyclization of 2‐methyltetrahydrofuran (2‐MTHF). For the later reaction, the reported catalyst exhibits site‐time yields and selectivity approaching that of phosphoric acid on all‐silica zeolites. Using solid‐state NMR and deprotonation energy calculations, the chemical environments of P and the corresponding acidities are determined.
- Sponsoring Organization:
- USDOE
- OSTI ID:
- 1631786
- Journal Information:
- Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Vol. 59 Journal Issue: 32; ISSN 1433-7851
- Publisher:
- Wiley Blackwell (John Wiley & Sons)Copyright Statement
- Country of Publication:
- Germany
- Language:
- English
Web of Science
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