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Abstract:
Massiveeffortsare investedin developinginnovativeCO2-sequestrationstrategiesto counterclimatechangeandtransformCO2intohigher-valueproducts.CO2-captureby reductionis a chemicalchallenge,andattentionis turnedtowardbiologicalsystemsthatselectivelyandefficientlycatalysethisreactionundermildconditionsandin aqueoussolvents.Whilea fewreportshaveevaluatedthe effectivenessof isolatedbacterialformatedehydrogenasesas catalystsforthereversibleelectrochemicalreductionof CO2, it is imperativeto exploreotherenzymesamongthenaturalreservoirof potentialmodelsthatmightexhibithigherturnoverratesor preferentialdirectionalityfor thereductivereaction.Here,we presentelectroenzymaticcatalysisof formylmethanofurandehydrogenase,a CO2-reducing-and-fixingbiomachineryisolatedfroma thermophilicmethanogen,whichwasdepositedon a graphiterodelectrodeto enabledirectelectrontransferfor electroenzymaticCO2reduction.Thegas is reducedwitha highFaradaicefficiency(109�1%),wherea lowaffinityfor formatepreventsits electrochemicalreoxidationandfavoursformateaccumulation.Thesepropertiesmakethe enzymean excellenttoolfor electroenzymaticCO2-fixationandinspirationfor proteinengineeringthatwouldbe beneficialfor biotechnologicalpurposesto convertthegreenhousegasintostableformatethatcansubsequentlybe safelystored,transported,andusedfor powergenerationwithoutenergyloss.
