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Decarboxylation of lactones over ZN/ZSM-5: elucidation of the structure of the active site and molecular interactions

DOI: 10.1002/anie.201704347 DOI Help

Authors: Edman Shik Chi Tsang (University of Oxford) , Lin Ye (University of Oxford) , Ben Lo (University of Oxford) , Qi Song (Sinopec) , Junlin Zheng (Sinopec) , Dejing Kong (Sinopec) , Claire Murray (Diamond Light Source) , Chiu Tang (Diamond Light Source)
Co-authored by industrial partner: Yes

Type: Journal Paper
Journal: Angewandte Chemie International Edition

State: Published (Approved)
Published: June 2017

Abstract: 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.

Journal Keywords: Zn-ZSM-5; lactone; decarboxylation; synchrotron; Rietveld

Diamond Keywords: Biofuel

Subject Areas: Chemistry, Energy, Environment


Instruments: I11-High Resolution Powder Diffraction

Added On: 19/06/2017 13:24

Discipline Tags:

Bioenergy Earth Sciences & Environment Sustainable Energy Systems Energy Climate Change Physical Chemistry Catalysis Chemistry

Technical Tags:

Diffraction X-ray Powder Diffraction