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Integration of Enzymes and Photosensitizers in a Hierarchical Mesoporous Metal–Organic Framework for Light-Driven CO2 Reduction

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    Integration of Enzymes and Photosensitizers in a Hierarchical Mesoporous Metal–Organic Framework for Light-Driven CO2 Reduction
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    • Yijing Chen
      Yijing Chen
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      International Institute for Nanotechnology (IIN), Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
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      Orcidhttp://orcid.org/0000-0002-3545-4622
    • Peng Li*
      Peng Li
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      International Institute for Nanotechnology (IIN), Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      *[email protected]
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    • Jiawang Zhou
      Jiawang Zhou
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
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      Orcidhttp://orcid.org/0000-0002-2399-0030
    • Cassandra T. Buru
      Cassandra T. Buru
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
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      Orcidhttp://orcid.org/0000-0001-6142-8252
    • Luka Đorđević
      Luka Đorđević
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      Simpson Querrey Institute, Northwestern University, Chicago, Illinois 60611, United States
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    • Penghao Li
      Penghao Li
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
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      Orcidhttp://orcid.org/0000-0002-1517-5845
    • Xuan Zhang
      Xuan Zhang
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
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      Orcidhttp://orcid.org/0000-0001-8214-7265
    • M. Mustafa Cetin
      M. Mustafa Cetin
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
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      Orcidhttp://orcid.org/0000-0002-6443-0232
    • J. Fraser Stoddart
      J. Fraser Stoddart
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      Institute for Molecular Design and Synthesis, Tianjin University, 92 Weijin Road, Tianjin 300072, China
      School of Chemistry, University of New South Wales, Sydney, NSW 2052, Australia
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      Orcidhttp://orcid.org/0000-0003-3161-3697
    • Samuel I. Stupp
      Samuel I. Stupp
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      Simpson Querrey Institute  and  Department of Medicine, Northwestern University, Chicago, Illinois 60611, United States
      Department of Materials Science and Engineering and Department of Biomedical Engineering, Northwestern University, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-5491-7442
    • Michael R. Wasielewski
      Michael R. Wasielewski
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      International Institute for Nanotechnology (IIN), Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      Institute for Sustainability and Energy at Northwestern, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
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      Orcidhttp://orcid.org/0000-0003-2920-5440
    • Omar K. Farha*
      Omar K. Farha
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      Institute for Sustainability and Energy at Northwestern, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      Department of Chemical and Biological Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      International Institute for Nanotechnology (IIN), Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States
      *[email protected]
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      Orcidhttp://orcid.org/0000-0002-9904-9845
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    Cite this: J. Am. Chem. Soc. 2020, 142, 4, 1768–1773
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    https://doi.org/10.1021/jacs.9b12828
    Published January 12, 2020
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    Protection of enzymes with synthetic materials is a viable strategy to stabilize, and hence to retain, the reactivity of these highly active biomolecules in non-native environments. Active synthetic supports, coupled to encapsulated enzymes, can enable efficient cascade reactions which are necessary for processes like light-driven CO2 reduction, providing a promising pathway for alternative energy generation. Herein, a semi-artificial system—containing an immobilized enzyme, formate dehydrogenase, in a light harvesting scaffold—is reported for the conversion of CO2 to formic acid using white light. The electron-mediator Cp*Rh(2,2′-bipyridyl-5,5′-dicarboxylic acid)Cl was anchored to the nodes of the metal–organic framework NU-1006 to facilitate ultrafast photo-induced electron transfer when irradiated, leading to the reduction of the coenzyme nicotinamide adenine dinucleotide at a rate of about 28 mM·h–1. Most importantly, the immobilized enzyme utilizes the reduced coenzyme to generate formic acid selectively from CO2 at a high turnover frequency of about 865 h–1 in 24 h. The outcome of this research is the demonstration of a feasible pathway for solar-driven carbon fixation.

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    This article is cited by 188 publications.

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    Cite this: J. Am. Chem. Soc. 2020, 142, 4, 1768–1773
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