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Photocatalytic Aqueous CO2 Reduction to CO and CH4 Sensitized by Ullazine Supramolecular Polymers

  • Oliver Dumele
    Oliver Dumele
    Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
  • Luka Đorđević
    Luka Đorđević
    Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
    Center for Bio-Inspired Energy Science, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
    Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, Illinois 60611, United States
  • Hiroaki Sai
    Hiroaki Sai
    Center for Bio-Inspired Energy Science, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States
    More by Hiroaki Sai
  • Thomas J. Cotey
    Thomas J. Cotey
    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States
  • M. Hussain Sangji
    M. Hussain Sangji
    Center for Bio-Inspired Energy Science, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
    Department of Biomedical Engineering, Northwestern University, Evanston, Illinois 60208, United States
  • Kohei Sato
    Kohei Sato
    Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, Illinois 60611, United States
    More by Kohei Sato
  • Adam J. Dannenhoffer
    Adam J. Dannenhoffer
    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States
  • , and 
  • Samuel I. Stupp*
    Samuel I. Stupp
    Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
    Center for Bio-Inspired Energy Science, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
    Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, Illinois 60611, United States
    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States
    Department of Biomedical Engineering, Northwestern University, Evanston, Illinois 60208, United States
    Department of Medicine, Northwestern University, Chicago, Illinois 60611, United States
    *[email protected]
Cite this: J. Am. Chem. Soc. 2022, 144, 7, 3127–3136
Publication Date (Web):February 10, 2022
https://doi.org/10.1021/jacs.1c12155
Copyright © 2022 American Chemical Society

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    Abstract

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    There has been rapid progress on the chemistry of supramolecular scaffolds that harness sunlight for aqueous photocatalytic production of hydrogen. However, great efforts are still needed to develop similar photosynthetic systems for the great challenge of CO2 reduction especially if they avoid the use of nonabundant metals. This work investigates the synthesis of supramolecular polymers capable of sensitizing catalysts that require more negative potentials than proton reduction. The monomers are chromophore amphiphiles based on a diareno-fused ullazine core that undergo supramolecular polymerization in water to create entangled nanoscale fibers. Under 450 nm visible light these fibers sensitize a dinuclear cobalt catalyst for CO2 photoreduction to generate carbon monoxide and methane using a sacrificial electron donor. The supramolecular photocatalytic system can generate amounts of CH4 comparable to those obtained with a precious metal-based [Ru(phen)3](PF6)2 sensitizer and, in contrast to Ru-based catalysts, retains photocatalytic activity in all aqueous media over 6 days. The present study demonstrates the potential of tailored supramolecular polymers as renewable energy and sustainability materials.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.1c12155.

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    CCDC 18786081878609, 1878614, and 1878616 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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