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- Title
Decarboxylation of Lactones over Zn/ZSM-5: Elucidation of the Structure of the Active Site and Molecular Interactions.
- Authors
Ye, Lin; Song, Qi; Lo, Benedict T. W.; Zheng, Junlin; Kong, Dejing; Murray, Claire A.; Tang, Chiu C.; Tsang, S. C. Edman
- Abstract
Herein, we report the catalytic decarboxylation of γ-valerolactone (GVL) over Zn/ZSM-5 to butene, followed by aromatization at high yield with co-feeding of water. An evaluation of the catalytic performance after prolonged periods of time showed that a water molecule is essential to maintain the decarboxylation and aromatization activities and avoid rapid catalyst deactivation. Synchrotron X-ray powder diffraction and Rietveld refinement were then used to elucidate the structures of adsorbed GVL and immobilized Zn species in combination with EXAFS and NMR spectroscopy. A new route for the cooperative hydrolysis of GVL by framework Zn−OH and Brønsted acidic sites to butene and then to aromatic compounds has thus been demonstrated. The structures and fundamental pathways for the nucleophilic attack of terminal Zn−OH sites are comparable to those of Zn-containing enzymes in biological systems.
- Subjects
DECARBOXYLATION; LACTONES; MOLECULAR interactions; AROMATIZATION catalysts; ACTIVATION (Chemistry); X-ray powder diffraction
- Publication
Angewandte Chemie, 2017, Vol 129, Issue 36, p10851
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201704347