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Direct Conversion of Syngas to Higher Alcohols via Tandem Integration of Fischer–Tropsch Synthesis and Reductive Hydroformylation

Angewandte Chemie, vol. 134

Abstract

Abstract The selective conversion of syngas to higher alcohols is an attractive albeit elusive route in the quest for effective production of chemicals from alternative carbon resources. We report the tandem integration of solid cobalt Fischer–Tropsch and molecular hydroformylation catalysts in a one‐pot slurry‐phase process. Unprecedented selectivities (>50 wt %) to C2+ alcohols are achieved at CO conversion levels >70 %, alongside negligible CO2 side‐production. The efficient overall transformation is enabled by catalyst engineering, bridging gaps in operation temperature and intrinsic selectivity which have classically precluded integration of these reactions in a single conversion step. Swift capture of 1‐olefin Fischer–Tropsch primary products by the molecular hydroformylation catalyst, presumably within the pores of the solid catalyst is key for high alcohol selectivity. The results underscore that controlled cooperation between solid aggregate and soluble molecular metal catalysts, which pertain to traditionally dichotomic realms of heterogeneous and homogeneous catalysis, is a promising blueprint toward selective conversion processes.

Authors 9

  1. Max-Planck-Institut für Kohlenforschung

    Affiliation as printed

    Department for Heterogeneous Catalysis Max-Planck-Institut für Kohlenforschung Kaiser-Wilhelm-Platz 1 45470 Mülheim an der Ruhr Germany

    These authors contributed equally to this work

  2. Max Planck Institute for Chemical Energy Conversion

    Affiliation as printed

    Max Planck Institute for Chemical Energy Conversion Stiftstraße 34–36 45470 Mülheim an der Ruhr Germany

    These authors contributed equally to this work

  3. Max Planck Institute for Chemical Energy Conversion

    Affiliation as printed

    Max Planck Institute for Chemical Energy Conversion Stiftstraße 34–36 45470 Mülheim an der Ruhr Germany

  4. Consejo Superior de Investigaciones Científicas · Universitat Politècnica de València · Instituto de Tecnología Química

    Affiliation as printed

    ITQ Instituto de Tecnología Química Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) Avenida de los Naranjos s/n 46022 Valencia Spain

  5. University of Cape Town

    Affiliation as printed

    Catalysis Institute and DSI-NRF Centre of Excellence in Catalysis c✶change Department of Chemical Engineering University of Cape Town Cape Town, Rondebosch 7701 South Africa

  6. University of Cape Town

    Affiliation as printed

    Catalysis Institute and DSI-NRF Centre of Excellence in Catalysis c✶change Department of Chemical Engineering University of Cape Town Cape Town, Rondebosch 7701 South Africa

  7. RWTH Aachen University · Max Planck Institute for Chemical Energy Conversion

    Affiliation as printed

    Institut für Technische und Makromolekulare Chemie RWTH Aachen Worringerweg 2 52074 Aachen Germany

    Max Planck Institute for Chemical Energy Conversion Stiftstraße 34–36 45470 Mülheim an der Ruhr Germany

  8. Andreas J. Vorholt corresponding

    Max Planck Institute for Chemical Energy Conversion

    Affiliation as printed

    Max Planck Institute for Chemical Energy Conversion Stiftstraße 34–36 45470 Mülheim an der Ruhr Germany

  9. Gonzalo Prieto corresponding

    Consejo Superior de Investigaciones Científicas · Universitat Politècnica de València · Max-Planck-Institut für Kohlenforschung · Instituto de Tecnología Química

    Affiliation as printed

    Department for Heterogeneous Catalysis Max-Planck-Institut für Kohlenforschung Kaiser-Wilhelm-Platz 1 45470 Mülheim an der Ruhr Germany

    ITQ Instituto de Tecnología Química Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) Avenida de los Naranjos s/n 46022 Valencia Spain

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References 57