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A practical concept for catalytic carbonylations using carbon dioxide

Author

Listed:
  • Rui Sang

    (Leibniz-Institut für Katalyse e.V.)

  • Yuya Hu

    (Leibniz-Institut für Katalyse e.V.)

  • Rauf Razzaq

    (Leibniz-Institut für Katalyse e.V.)

  • Guillaume Mollaert

    (University of Antwerp)

  • Hanan Atia

    (Leibniz-Institut für Katalyse e.V.)

  • Ursula Bentrup

    (Leibniz-Institut für Katalyse e.V.)

  • Muhammad Sharif

    (Leibniz-Institut für Katalyse e.V.)

  • Helfried Neumann

    (Leibniz-Institut für Katalyse e.V.)

  • Henrik Junge

    (Leibniz-Institut für Katalyse e.V.)

  • Ralf Jackstell

    (Leibniz-Institut für Katalyse e.V.)

  • Bert U. W. Maes

    (University of Antwerp)

  • Matthias Beller

    (Leibniz-Institut für Katalyse e.V.)

Abstract

The rise of CO2 in atmosphere is considered as the major reason for global warming. Therefore, CO2 utilization has attracted more and more attention. Among those, using CO2 as C1-feedstock for the chemical industry provides a solution. Here we show a two-step cascade process to perform catalytic carbonylations of olefins, alkynes, and aryl halides utilizing CO2 and H2. For the first step, a novel heterogeneous copper 10Cu@SiO2-PHM catalyst exhibits high selectivity (≥98%) and decent conversion (27%) in generating CO from reducing CO2 with H2. The generated CO is directly utilized without further purification in industrially important carbonylation reactions: hydroformylation, alkoxycarbonylation, and aminocarbonylation. Notably, various aldehydes, (unsaturated) esters and amides are obtained in high yields and chemo-/regio-selectivities at low temperature under ambient pressure. Our approach is of interest for continuous syntheses in drug discovery and organic synthesis to produce building blocks on reasonable scale utilizing CO2.

Suggested Citation

  • Rui Sang & Yuya Hu & Rauf Razzaq & Guillaume Mollaert & Hanan Atia & Ursula Bentrup & Muhammad Sharif & Helfried Neumann & Henrik Junge & Ralf Jackstell & Bert U. W. Maes & Matthias Beller, 2022. "A practical concept for catalytic carbonylations using carbon dioxide," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32030-8
    DOI: 10.1038/s41467-022-32030-8
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    References listed on IDEAS

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    1. Lingxiang Wang & Erjia Guan & Yeqing Wang & Liang Wang & Zhongmiao Gong & Yi Cui & Xiangju Meng & Bruce C. Gates & Feng-Shou Xiao, 2020. "Author Correction: Silica accelerates the selective hydrogenation of CO2 to methanol on cobalt catalysts," Nature Communications, Nature, vol. 11(1), pages 1-1, December.
    2. Qiang Liu & Lipeng Wu & Ralf Jackstell & Matthias Beller, 2015. "Using carbon dioxide as a building block in organic synthesis," Nature Communications, Nature, vol. 6(1), pages 1-15, May.
    3. Lingxiang Wang & Erjia Guan & Yeqing Wang & Liang Wang & Zhongmiao Gong & Yi Cui & Xiangju Meng & Bruce C. Gates & Feng-Shou Xiao, 2020. "Silica accelerates the selective hydrogenation of CO2 to methanol on cobalt catalysts," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    4. Roy van den Berg & Gonzalo Prieto & Gerda Korpershoek & Lars I. van der Wal & Arnoldus J. van Bunningen & Susanne Lægsgaard-Jørgensen & Petra E. de Jongh & Krijn P. de Jong, 2016. "Structure sensitivity of Cu and CuZn catalysts relevant to industrial methanol synthesis," Nature Communications, Nature, vol. 7(1), pages 1-7, December.
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    Cited by:

    1. Yuman Qin & Robin Cauwenbergh & Suman Pradhan & Rakesh Maiti & Philippe Franck & Shoubhik Das, 2023. "Straightforward synthesis of functionalized γ-Lactams using impure CO2 stream as the carbon source," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    2. Serena Monticelli & Alex Talbot & Philipp Gotico & Fabien Caillé & Olivier Loreau & Antonio Vecchio & Augustin Malandain & Antoine Sallustrau & Winfried Leibl & Ally Aukauloo & Frédéric Taran & Zakari, 2023. "Unlocking full and fast conversion in photocatalytic carbon dioxide reduction for applications in radio-carbonylation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Hao-Xin Liu & Wei-Wei Wang & Xin-Pu Fu & Jin-Cheng Liu & Chun-Jiang Jia, 2024. "Direct cleavage of C=O double bond in CO2 by the subnano MoOx surface on Mo2N," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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