Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic.
Sokol, Katarzyna P
Robinson, William E
Journal of the American Chemical Society
American Chemical Society
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Sokol, K. P., Robinson, W. E., Oliveira, A. R., Zacarias, S., Lee, C., Madden, C., Bassegoda, A., et al. (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. https://doi.org/10.1021/jacs.9b09575
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 semi-artificial 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.
ERC Consolidator Grant “MatEnSAP” (682833), BBSRC (BB/J000124/1, BB/I026367/1), EPSRC (EP/L015978/1, EP/G037221/1, nanoDTC and a DTA studentship to K.P.S.), Marie Curie IntraEuropean Fellowship (PIEFGA- 2013-625034), Fundação para a Ciência e Tecnologia (Portugal) fellowship SFRH/BD/116515/2016, grants PTDC/BIAMIC/ 2723/2014,
ECH2020 EUROPEAN RESEARCH COUNCIL (ERC) (682833)
European Commission (625034)
External DOI: https://doi.org/10.1021/jacs.9b09575
This record's URL: https://www.repository.cam.ac.uk/handle/1810/298222
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