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Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic

Journal Article


Abstract


  • The biological formate hydrogenlyase (FHL) complex links a formate dehydrogenase (FDH) to a hydrogenase (H2ase) and produces H2 and CO2 from formate via mixed-acid fermentation in Escherichia coli. Here, we describe an electrochemical and a colloidal semiartificial FHL system that consists of an FDH and a H2ase immobilized on conductive indium tin oxide (ITO) as an electron relay. These in vitro systems benefit from the efficient wiring of a highly active enzyme pair and allow for the reversible conversion of formate to H2 and CO2 under ambient temperature and pressure. The hybrid systems provide a template for the design of synthetic catalysts and surpass the FHL complex in vivo by storing and releasing H2 on demand by interconverting CO2/H2 and formate with minimal bias in either direction.

Publication Date


  • 2019

Citation


  • Sokol, K. P., Robinson, W. E., Oliveira, A. R., Zacarias, S., Lee, C. Y., Madden, C., . . . Reisner, E. (2019). Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic. Journal of the American Chemical Society, 141(44), 17498-17502. doi:10.1021/jacs.9b09575

Scopus Eid


  • 2-s2.0-85074387265

Start Page


  • 17498

End Page


  • 17502

Volume


  • 141

Issue


  • 44

Abstract


  • The biological formate hydrogenlyase (FHL) complex links a formate dehydrogenase (FDH) to a hydrogenase (H2ase) and produces H2 and CO2 from formate via mixed-acid fermentation in Escherichia coli. Here, we describe an electrochemical and a colloidal semiartificial FHL system that consists of an FDH and a H2ase immobilized on conductive indium tin oxide (ITO) as an electron relay. These in vitro systems benefit from the efficient wiring of a highly active enzyme pair and allow for the reversible conversion of formate to H2 and CO2 under ambient temperature and pressure. The hybrid systems provide a template for the design of synthetic catalysts and surpass the FHL complex in vivo by storing and releasing H2 on demand by interconverting CO2/H2 and formate with minimal bias in either direction.

Publication Date


  • 2019

Citation


  • Sokol, K. P., Robinson, W. E., Oliveira, A. R., Zacarias, S., Lee, C. Y., Madden, C., . . . Reisner, E. (2019). Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic. Journal of the American Chemical Society, 141(44), 17498-17502. doi:10.1021/jacs.9b09575

Scopus Eid


  • 2-s2.0-85074387265

Start Page


  • 17498

End Page


  • 17502

Volume


  • 141

Issue


  • 44