Single-Step Conversion of Methyl Ethyl Ketone to Olefins over ZnxZryOz Catalysts in Water

Susan Habas, Frederick Baddour, Richard Elander, Vanessa Dagle, Robert Dagle, Libor Kovarik

Research output: Contribution to journalArticlepeer-review

5 Scopus Citations

Abstract

In this study we investigated the conversion of aqueous methyl-ethyl-ketone (MEK) to olefin fuel precursors over ZnxZryOz mixed oxide catalysts. Experiments were carried out in water as MEK is intended to be produced from the dehydration of 2,3-butanediol in fermentation broth which is highly diluted in water. We demonstrated that ZnxZryOz catalysts are highly effective for converting aqueous MEK to C4-C5 olefins. High selectivity to olefins equal to 85% was reached at 92% per pass conversion when under H2 atmosphere. Catalyst stability was demonstrated for 60 hours' time on stream, highlighting the potential for upgrading 2,3-butanediol contained in fermentation broth without the need for energy-intensive water separation. Increased concentration of MEK in the aqueous feed results in increased activity towards olefin production. However, water inhibits catalyst deactivation from coking. A mechanistic investigation revealed the impact of the reaction environment (inert or reducing atmosphere) on the reaction pathways. In an inert environment, the mechanism involves consecutive aldol condensation of MEK and 3-pentanone intermediate. Under reducing conditions two reaction pathways compete with each other as MEK hydrogenation to butenes occurs concurrently with the aldol condensation/decomposition.
Original languageAmerican English
Pages (from-to)3393-3400
Number of pages8
JournalChemCatChem
Volume11
Issue number15
DOIs
StatePublished - 7 Aug 2019

Bibliographical note

Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

NREL Publication Number

  • NREL/JA-5100-73271

Keywords

  • 2,3-butanediol
  • aqueous
  • bio-fuels
  • methyl-ethyl-ketone
  • olefins

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