Selectivity control in hydrogenation through adaptive catalysis using ruthenium nanoparticles on a CO2-responsive support
Nature Chemistry, vol. 13, pp. 916–922
Abstract
Abstract With the advent of renewable carbon resources, multifunctional catalysts are becoming essential to hydrogenate selectively biomass-derived substrates and intermediates. However, the development of adaptive catalytic systems, that is, with reversibly adjustable reactivity, able to cope with the intermittence of renewable resources remains a challenge. Here, we report the preparation of a catalytic system designed to respond adaptively to feed gas composition in hydrogenation reactions. Ruthenium nanoparticles immobilized on amine-functionalized polymer-grafted silica act as active and stable catalysts for the hydrogenation of biomass-derived furfural acetone and related substrates. Hydrogenation of the carbonyl group is selectively switched on or off if pure H2 or a H2/CO2 mixture is used, respectively. The formation of alkylammonium formate species by the catalytic reaction of CO2 and H2 at the amine-functionalized support has been identified as the most likely molecular trigger for the selectivity switch. As this reaction is fully reversible, the catalyst performance responds almost in real time to the feed gas composition.
Authors 8
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Max Planck Institute for Chemical Energy Conversion
Affiliation as printed
Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr, Germany
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Affiliation as printed
Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Aachen, Germany
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Affiliation as printed
Department of Chemistry, Queen's University, Kingston, Ontario, Canada
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Affiliation as printed
Department of Chemistry, Queen's University, Kingston, Ontario, Canada
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Max Planck Institute for Chemical Energy Conversion
Affiliation as printed
Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr, Germany
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Affiliation as printed
Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Aachen, Germany
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Affiliation as printed
Department of Chemistry, Queen's University, Kingston, Ontario, Canada
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Max Planck Institute for Chemical Energy Conversion · RWTH Aachen University
Affiliation as printed
Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Aachen, Germany. walter.leitner@cec.mpg.de
Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr, Germany. walter.leitner@cec.mpg.de
Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Aachen, Germany
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