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

Yijing Chen, Peng Li, Jiawang Zhou, Cassandra T. Buru, Luka Aorević, Penghao Li, Xuan Zhang, M. Mustafa Cetin, J. Fraser Stoddart, Samuel I. Stupp, Michael R. Wasielewski, Omar K. Farha

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

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.

Original languageEnglish
Pages (from-to)1768-1773
Number of pages6
JournalJournal of the American Chemical Society
Volume142
Issue number4
DOIs
Publication statusPublished - Jan 29 2020

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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