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Selective CO2 Reduction Catalyzed by Single Cobalt Sites on Carbon Nitride under Visible-Light Irradiation

  • Peipei Huang
    Peipei Huang
    Department of Chemistry, University of New Hampshire, Durham, New Hampshire 03857, United States
    More by Peipei Huang
  • Jiahao Huang
    Jiahao Huang
    Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United States
    More by Jiahao Huang
  • Sebastian A. Pantovich
    Sebastian A. Pantovich
    Department of Chemistry, University of New Hampshire, Durham, New Hampshire 03857, United States
  • Alexander D. Carl
    Alexander D. Carl
    Department of Chemistry & Biochemistry, Worcester Polytechnic Institute, Worcester, Massachusetts 01609, United States
  • Thomas G. Fenton
    Thomas G. Fenton
    Department of Chemistry, University of New Hampshire, Durham, New Hampshire 03857, United States
  • Christine A. Caputo
    Christine A. Caputo
    Department of Chemistry, University of New Hampshire, Durham, New Hampshire 03857, United States
  • Ronald L. Grimm
    Ronald L. Grimm
    Department of Chemistry & Biochemistry, Worcester Polytechnic Institute, Worcester, Massachusetts 01609, United States
  • Anatoly I. Frenkel*
    Anatoly I. Frenkel
    Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United States
    Division of Chemistry, Brookhaven National Laboratory, Upton, New York 11973, United States
    *[email protected]
  • , and 
  • Gonghu Li*
    Gonghu Li
    Department of Chemistry, University of New Hampshire, Durham, New Hampshire 03857, United States
    *[email protected]
    More by Gonghu Li
Cite this: J. Am. Chem. Soc. 2018, 140, 47, 16042–16047
Publication Date (Web):November 10, 2018
https://doi.org/10.1021/jacs.8b10380
Copyright © 2018 American Chemical Society

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    Abstract

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    Framework nitrogen atoms of carbon nitride (C3N4) can coordinate with and activate metal sites for catalysis. In this study, C3N4 was employed to harvest visible light and activate Co2+ sites, without the use of additional ligands, in photochemical CO2 reduction. Photocatalysts containing single Co2+ sites on C3N4 were prepared by a simple deposition method and demonstrated excellent activity and product selectivity toward CO formation. A turnover number of more than 200 was obtained for CO production using the synthesized photocatalyst under visible-light irradiation. Inactive cobalt oxides formed at relatively high cobalt loadings but did not alter product selectivity. Further studies with X-ray absorption spectroscopy confirmed the presence of single Co2+ sites on C3N4 and their important role in achieving selective CO2 reduction.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.8b10380.

    • Experimental details on materials, catalyst synthesis, materials characterization, X-ray absorption spectroscopy, photocatalytic testing; estimated quantum yields; and supporting figures (PDF)

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