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J Am Chem Soc. 2019 Nov 6;141(44):17498-17502. doi: 10.1021/jacs.9b09575. Epub 2019 Oct 28.

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

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Department of Chemistry , University of Cambridge , Lensfield Road , Cambridge CB2 1EW , U.K.
Instituto de Tecnologia Química e Biológica António Xavier (ITQB) , Universidade NOVA de Lisboa , Av. da República , 2780-157 Oeiras , Portugal.
Medical Research Council Mitochondrial Biology Unit , University of Cambridge , The Keith Peters Building, Cambridge Biomedical Campus, Hills Road , Cambridge CB2 0XY , U.K.


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.

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