Cerium-Based Metal–Organic Layers Catalyze Hydrogen Evolution Reaction through Dual Photoexcitation

  • Yang Song
    Yang Song
    Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States
    More by Yang Song
  • Yunhong Pi
    Yunhong Pi
    Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States
    School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China
    More by Yunhong Pi
  • Xuanyu Feng
    Xuanyu Feng
    Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States
    More by Xuanyu Feng
  • Kaiyuan Ni
    Kaiyuan Ni
    Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States
    More by Kaiyuan Ni
  • Ziwan Xu
    Ziwan Xu
    Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States
    More by Ziwan Xu
  • Justin S. Chen
    Justin S. Chen
    Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States
  • Zhong Li
    Zhong Li
    School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China
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  • , and 
  • Wenbin Lin*
    Wenbin Lin
    Department of Chemistry, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States
    *[email protected]
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Cite this: J. Am. Chem. Soc. 2020, 142, 15, 6866–6871
Publication Date (Web):March 30, 2020
https://doi.org/10.1021/jacs.0c00679
Copyright © 2020 American Chemical Society
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Abstract

Cerium-based materials such as ceria are increasingly used in catalytic reactions. We report here the synthesis of the first Ce-based metal–organic layer (MOL), Ce6-BTB, comprising Ce6 secondary building units (SBUs) and 1,3,5-benzenetribenzoate (BTB) linkers, and its functionalization for photocatalytic hydrogen evolution reaction (HER). Ce6-BTB was postsynthetically modified with photosensitizing [(MBA)Ir(ppy)2]Cl or [(MBA)Ru(bpy)2]Cl2 (MBA = 2-(5′-methyl-[2,2′-bipyridin]-5-yl)acetate, ppy = 2-phenylpyridine, bpy = 2,2′-bipyridine) to afford Ce6-BTB-Ir or Ce6-BTB-Ru MOLs, respectively. The proximity of photosensitizing ligands and Ce6 SBUs in the MOLs facilitates electron transfer to drive photocatalytic HER under visible light with turnover numbers of 1357 and 484 for Ce6-BTB-Ir and Ce6-BTB-Ru, respectively. Photophysical and electrochemical studies revealed a novel dual photoexcitation pathway whereby the excited photosensitizers in the MOL are reductively quenched and then transfer electrons to Ce6 SBUs to generate CeIII centers, which are further photoexcited to CeIII* species for HER.

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  • Synthesis and characterization of Ce-BTB MOL, Ce-BTB-Ir, and Ce-BTB-Ru; reaction procedures and supplementary experiment results of photocatalytic HER; supplementary photophysical and electrochemical data (PDF)

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