Decarboxylation of Lactones over Zn/ZSM-5: Elucidation of the Structure of the Active Site and Molecular Interactions

Lin Ye, Qi Song, Tsz Woon Benedict Lo, Junlin Zheng, Dejing Kong, Claire A. Murray, Chiu C. Tang, S. C.Edman Tsang

Research output: Journal article publicationJournal articleAcademic researchpeer-review

18 Citations (Scopus)

Abstract

KGaA, Weinheim 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.
Original languageEnglish
Pages (from-to)10711-10716
Number of pages6
JournalAngewandte Chemie - International Edition
Volume56
Issue number36
DOIs
Publication statusPublished - 1 Jan 2017
Externally publishedYes

Keywords

  • decarboxylation
  • Rietveld refinement
  • X-ray diffraction
  • Zn/ZSM-5
  • γ-valerolactone

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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