Selective conversion of acetone to isobutene and acetic acid on aluminosilicates: Kinetic coupling between acid-catalyzed and radical-mediated pathways

Selective conversion of acetone to isobutene and acetic acid on aluminosilicates: Kinetic... Journal of Catalysis 360 (2018) 66–80 Contents lists available at ScienceDirect Journal of Catalysis journal homepage: www.elsevier.com/locate/jcat Selective conversion of acetone to isobutene and acetic acid on aluminosilicates: Kinetic coupling between acid-catalyzed and radical- mediated pathways Stanley Herrmann, Enrique Iglesia Department of Chemical and Biomolecular Engineering, University of California, Berkeley, United States ar ti c l e i nf o ab stra ct Article history: Solid Brønsted acids catalyze aldol condensations that form CAC bonds and remove O-atoms from oxy- Received 1 December 2017 genate reactants, but sequential b-scission reactions also cleave CAC bonds, leading to isobutene and Revised 25 January 2018 acetic acid products for acetone reactants. The elementary steps and site requirements that cause these Accepted 29 January 2018 selectivities to depend sensitively on Al content and framework type in aluminosilicate solid acids remain Available online 22 February 2018 speculative. Acetone reactions on microporous and mesoporous aluminosilicates (FER, TON, MFI, BEA, MCM-41) showed highest b-scission selectivities on MFI and BEA; they increased as the Al content and Keywords: the intracrystalline density of active protons decreased. The effects of acetone and H O pressure on turn- Solid Brønsted acids over rates and selectivities indicate that an equilibrated pool http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Journal of Catalysis Elsevier

Selective conversion of acetone to isobutene and acetic acid on aluminosilicates: Kinetic coupling between acid-catalyzed and radical-mediated pathways

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Publisher
Elsevier
Copyright
Copyright © 2018 Elsevier Ltd
ISSN
0021-9517
D.O.I.
10.1016/j.jcat.2018.01.032
Publisher site
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Abstract

Journal of Catalysis 360 (2018) 66–80 Contents lists available at ScienceDirect Journal of Catalysis journal homepage: www.elsevier.com/locate/jcat Selective conversion of acetone to isobutene and acetic acid on aluminosilicates: Kinetic coupling between acid-catalyzed and radical- mediated pathways Stanley Herrmann, Enrique Iglesia Department of Chemical and Biomolecular Engineering, University of California, Berkeley, United States ar ti c l e i nf o ab stra ct Article history: Solid Brønsted acids catalyze aldol condensations that form CAC bonds and remove O-atoms from oxy- Received 1 December 2017 genate reactants, but sequential b-scission reactions also cleave CAC bonds, leading to isobutene and Revised 25 January 2018 acetic acid products for acetone reactants. The elementary steps and site requirements that cause these Accepted 29 January 2018 selectivities to depend sensitively on Al content and framework type in aluminosilicate solid acids remain Available online 22 February 2018 speculative. Acetone reactions on microporous and mesoporous aluminosilicates (FER, TON, MFI, BEA, MCM-41) showed highest b-scission selectivities on MFI and BEA; they increased as the Al content and Keywords: the intracrystalline density of active protons decreased. The effects of acetone and H O pressure on turn- Solid Brønsted acids over rates and selectivities indicate that an equilibrated pool

Journal

Journal of CatalysisElsevier

Published: Apr 1, 2018

References

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