Continuous Furfuryl Alcohol Production via Coupled Dehydrogenation-Hydrogenation over Supported Cu and Au Catalysts: A Consideration of Hydrogen Generation and Transfer

Chiara Pischetola, Laura Collado, Roque Aguado-Molina, Samuel Martín-Treceño, Mark A. Keane, Fernando Cardenas-Lizana

Research output: Contribution to journalArticle

Abstract

We have investigated the continuous (P = 1 atm, T = 453 K) coupled dehydrogenation/hydrogenation of 2-butanol/furfural for the simultaneous production of 2-butanone and furfuryl alcohol. A series of oxides (Al 2O 3, ZrO 2, SiO 2, TiO 2 and CeO 2) were used to support nano-scale Cu (mean size 2.2–2.8 nm from STEM) and tested in the dehydrogenation of 2-butanol. All the supported Cu catalysts promoted exclusive formation of the target 2-butanone. Hydrogen production was shown to correlate with the Lewis basicity of the oxide support and the highest rate was recorded for Cu/CeO 2. Conventional furfural hydrogenation (using an external supply of hydrogen) over ceria supported Au (mean size =3.5 nm) was fully selective to furfuryl alcohol where less than 1 % of the hydrogen supplied was utilised. Under the same reaction conditions, exclusive formation of 2-butanone and furfuryl alcohol and higher hydrogenation rate was achieved in the coupled process over physical mixtures of Au/CeO 2+Cu/Oxide (in N 2) where Cu → Au hydrogen transfer was favored by coke (from TGA). The combination Au/CeO 2+Cu/CeO 2 delivered a 70-fold higher hydrogenation rate, full H 2 utilisation and 215 times lower E-factor. Our results demonstrate in situ hydrogen generation via dehydrogenation as a sustainable alternative hydrogenation route to valuable products.

Original languageEnglish
Article number110912
JournalMolecular Catalysis
Volume492
Early online date2 Jun 2020
DOIs
Publication statusPublished - Aug 2020

Keywords

  • 2-butanone
  • Au+Cu physical mixture
  • Coupling
  • Dehydrogenation-hydrogenation
  • Furfuryl alcohol

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology
  • Physical and Theoretical Chemistry

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