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Photocatalytic CO2 Reduction Using CO2-Binding Enzymes.

Henrik Terholsen1, Hilario Diego Huerta-Zerón2, Christina Möller1

  • 1Institute of Biochemistry, Department of Biotechnology and Enzyme Catalysis, University of Greifswald, Felix-Hausdorff-Straße 4, 17487, Greifswald, Germany.

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PubMed
Summary

Researchers identified enzymes for efficient aqueous carbon dioxide (CO2) reduction. Engineered enzymes achieved high selectivity for carbon monoxide (CO) production, advancing circular carbon economy goals.

Keywords:
CO2 reductionenzymesphotocatalysispromiscuous activityprotein engineering

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Area of Science:

  • Biocatalysis
  • Green Chemistry
  • Enzyme Engineering

Background:

  • Achieving a circular carbon economy necessitates novel carbon dioxide (CO2) utilization strategies.
  • Efficient catalytic systems, particularly in aqueous solutions, are crucial for CO2 conversion.
  • Existing catalytic systems for CO2 reduction in water are limited.

Purpose of the Study:

  • To develop a general strategy for identifying enzymes capable of CO2 reduction.
  • To engineer enzymes for enhanced performance in aqueous photocatalytic CO2 reduction.
  • To investigate the mechanism of CO2 reduction by enzymes.

Main Methods:

  • Structural analysis to identify potential CO2 binding sites in enzymes.
  • Site-directed mutagenesis to engineer enzyme variants.
  • Aqueous photocatalytic CO2 reduction assays using ruthenium photosensitizers and sodium ascorbate.
  • Kinetic studies to determine electron transfer mechanisms.

Main Results:

  • Phenolic acid decarboxylase from Bacillus subtilis (BsPAD) was identified as an enzyme capable of aqueous CO2 reduction to carbon monoxide (CO).
  • Engineered BsPAD variants achieved high turnover numbers (TONs) up to 978 and selectivities up to 93% for CO over H2.
  • Mutations in the active site improved CO generation, revealing that electron transfer is rate-limiting and occurs via multistep tunneling.
  • The approach was validated with eight other enzymes, demonstrating broad applicability for photocatalytic CO2 reduction.

Conclusions:

  • A generalizable strategy for enzyme discovery and engineering for CO2 reduction has been established.
  • Enzymes can be effectively engineered to catalyze aqueous CO2 reduction to CO with high efficiency and selectivity.
  • This work provides a foundation for utilizing biocatalysis in circular carbon economy initiatives.