Nitrogenase bioelectrocatalysis: heterogeneous ammonia and hydrogen production by MoFe protein

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dc.contributor.authorMilton, Ross D.en
dc.contributor.authorAbdellaoui, Sofieneen
dc.contributor.authorKhadka, Nimeshen
dc.contributor.authorDean, Dennis R.en
dc.contributor.authorLeech, Dónalen
dc.contributor.authorSeefeldt, Lance C.en
dc.contributor.authorMinteer, Shelley D.en
dc.contributor.departmentBiochemistryen
dc.contributor.departmentBiochemistryen
dc.date.accessioned2017-05-01T06:42:16Zen
dc.date.available2017-05-01T06:42:16Zen
dc.date.issued2016-06-20en
dc.description.abstractNitrogenase is the only enzyme known to catalyze the reduction of N2 to 2NH3. In vivo, the MoFe protein component of nitrogenase is exclusively reduced by the ATP-hydrolyzing Fe protein in a series of transient association/dissociation steps that are linked to the hydrolysis of two ATP for each electron transferred. We report MoFe protein immobilized at an electrode surface, where cobaltocene (as an electron mediator that can be observed in real time at a carbon electrode) is used to reduce the MoFe protein (independent of the Fe protein and of ATP hydrolysis) and support the bioelectrocatalytic reduction of protons to dihydrogen, azide to ammonia, and nitrite to ammonia. Bulk bioelectrosynthetic N3− or NO2− reduction (50 mM) for 30 minutes yielded 70 ± 9 nmol NH3 and 234 ± 62 nmol NH3, with NO2− reduction operating at high faradaic efficiency.en
dc.format.extent2550-2554en
dc.format.mimetypeapplication/pdfen
dc.identifierc6ee01432a.pdfen
dc.identifierc6ee01432a1.pdfen
dc.identifier.doihttps://doi.org/10.1039/c6ee01432aen
dc.identifier.eissn1754-5706en
dc.identifier.issn1754-5692en
dc.identifier.issue8en
dc.identifier.urihttp://hdl.handle.net/10919/77550en
dc.identifier.volume9en
dc.language.isoenen
dc.publisherRoyal Society of Chemistryen
dc.relation.ispartofRoyal Society of Chemistry Gold Open Access - 2016en
dc.rightsCreative Commons Attribution-NonCommercial 3.0 Unporteden
dc.rights.holderMilton, Ross D.en
dc.rights.holderAbdellaoui, Sofieneen
dc.rights.holderKhadka, Nimeshen
dc.rights.holderDean, Dennis R.en
dc.rights.holderLeech, Dónalen
dc.rights.holderSeefeldt, Lance C.en
dc.rights.holderMinteer, Shelley D.en
dc.rights.urihttp://creativecommons.org/licenses/by-nc/3.0/en
dc.titleNitrogenase bioelectrocatalysis: heterogeneous ammonia and hydrogen production by MoFe proteinen
dc.title.serialEnergy & Environmental Scienceen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.dcmitypeDataseten

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