title: Aqueous light driven hydrogen production by a Ru-ferredoxin-Co biohybrid.
abstract: Herein we report the creation of a novel solar fuel biohybrid for light-driven H2 production utilizing the native electron transfer protein ferredoxin (Fd) as a scaffold for binding of a ruthenium photosensitizer (PS) and a molecular cobaloxime catalyst (Co). EPR and transient optical experiments provide direct evidence of a long-lived (>1.5 ms) Ru(III)-Fd-Co(I) charge separated state formed via an electron relay through the Fd [2Fe-2S] cluster, initiating the catalytic cycle for 2H(+) + 2e(-) → H2.
authors.affiliation: Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, IL 60439, USA. utschig@anl.gov.
authors.forename: S R
authors.initials: SR
authors.lastname: Soltau
authors.forename: J
authors.initials: J
authors.lastname: Niklas
authors.forename: P D
authors.initials: PD
authors.lastname: Dahlberg
authors.forename: O G
authors.initials: OG
authors.lastname: Poluektov
authors.forename: D M
authors.initials: DM
authors.lastname: Tiede
authors.forename: K L
authors.initials: KL
authors.lastname: Mulfort
authors.forename: L M
authors.initials: LM
authors.lastname: Utschig
mesh_terms: D001205:Ascorbic Acid / Q000737:chemistry; D002384:Catalysis; D004579:Electron Transport; D005288:Ferredoxins / Q000737:chemistry*; D006859:Hydrogen / Q000737:chemistry* / Q000378:metabolism; D008027:Light; D009942:Organometallic Compounds / Q000737:chemistry*; D056951:Photoelectron Spectroscopy; D017319:Photosensitizing Agents / Q000737:chemistry*; D012428:Ruthenium / Q000737:chemistry*
chemical_list: D005288:Ferredoxins; D009942:Organometallic Compounds; D017319:Photosensitizing Agents; C556179:cobaloxime; D012428:Ruthenium; D006859:Hydrogen; D001205:Ascorbic Acid