Exploring Low-Temperature Dehydrogenation at Ionic Cu Sites in Beta Zeolite to Enable Alkane Recycle in Dimethyl Ether Homologation

Daniel Ruddy, Carrie Farberow, Seon Ah Kim, Jesse Hensley, Joshua Schaidle, Jeffrey Miller, James Gallagher, Singfoong Cheah

Research output: Contribution to journalArticlepeer-review

12 Scopus Citations

Abstract

Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Brønsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/BEA catalysts activate C-H bonds in isobutane. Computational analysis revealed that isobutane dehydrogenation at a Cu(I) site proceeds through a two-step mechanism with a maximum energy barrier of 159 kJ/mol. These results demonstrate that light alkanes can be reactivated on Cu/BEA, which may enable re-entry of these species into the chain-growth cycle of dimethyl ether homologation, thereby increasing gasoline-range (C5+) hydrocarbon yield. (Chemical Equation Presented).

Original languageAmerican English
Pages (from-to)3662-3667
Number of pages6
JournalACS Catalysis
Volume7
Issue number5
DOIs
StatePublished - 5 May 2017

Bibliographical note

Publisher Copyright:
© 2017 American Chemical Society.

NREL Publication Number

  • NREL/JA-5100-67284

Keywords

  • C-H activation
  • copper
  • dehydrogenation
  • heterogeneous catalysis
  • zeolites

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