A new route for de-carboxylation of lactones over Zn/ZSM-5: elucidation of structure and molecular interactions

Journal article

Here, we report a catalytic process of decarboxylating gamma-valerolactone, GVL (the biomass derived lactone as an example) over Zn/ZSM-5 to butene, followed by aromatization at high yield with co-feed water. Evaluation of catalytic performance at prolonged time shows that water molecule is essential in maintaining the decarboxylation/ aromatization activity without rapid deactivation. Synchrotron X-ray diffraction and Rietveld refinement are then used to elucidate the adsorbed structures of GVL and immobilized Zn-species with the support of EXAFS and NMR. A new route of cooperative hydrolysis of GVL by framework Zn-OH and Brønsted acid sites to butene and then to aromatics is for the first time demonstrated. The structures and fundamental pathways for nucleophilic attack of terminal Zn-OH site are comparable to that of reported Zn-containing enzymes in biological systems.

Authors: Tsang, E; Ye, L; Lo, B; Song, Q; Zheng, J

• Publication status: Published
• Peer review status: Peer reviewed
• Publisher: Wiley
• Journal: Angewandte Chemie International Edition
• Volume: 56
• Issue: 36
• Pages: 10711-10716
• Publication date: 2017-06-15
• Acceptance date: 2017-06-14
• DOI: 10.1002/anie.201704347
• EISSN: 1521-3773
• ISSN: 1433-7851
• Language: English
• Keywords: lactone; Rietveld; decarboxylation; synchrotron; Zn-ZSM-5