Insight into three-coordinate aluminum species on ethanol-to-olefin conversion over ZSM-5 zeolites

Zichun Wang, Luke A. O'Dell, Xin Zeng, Can Liu, Shufang Zhao, Wenwen Zhang, Marianne Gaborieau, Yijiao Jiang, Jun Huang*

*Corresponding author for this work

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

Commercial bioethanol can be readily converted into ethylene by a dehydration process using solid acids, such as Brønsted acidic H-ZSM-5 zeolites, and thus, it is an ideal candidate to replace petroleum and coal for the sustainable production of ethylene. Now, strong Lewis acidic extra-framework three-coordinate Al3+ species were introduced into H-ZSM-5 zeolites to improve their catalytic activity. Remarkably, Al3+ species working with Brønsted acid sites can accelerate ethanol dehydration at a much lower reaction temperature and shorten the unsteady-state period within 1–2 h, compared to >9 h for those without Al3+ species, which can significantly enhance the ethanol dehydration efficiency and reduce the cost. The reaction mechanism, studied by solid-state NMR, shows that strong Lewis acidic EFAl-Al3+ species can collaborate with Brønsted acid sites and promote ethanol dehydration either directly or indirectly via an aromatics-based cycle to produce ethylene.

Original languageEnglish
Pages (from-to)18061-18068
Number of pages8
JournalAngewandte Chemie - International Edition
Volume58
Issue number50
Early online date8 Oct 2019
DOIs
Publication statusPublished - 9 Dec 2019

Keywords

  • acidity
  • aluminum
  • ethanol to olefin
  • MFI zeolite
  • solid-state NMR spectroscopy

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