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Title: Aqueous light driven hydrogen production by a Ru–ferredoxin–Co biohybrid

Journal Article · · ChemComm
DOI:https://doi.org/10.1039/C5CC03006D· OSTI ID:1339164
 [1];  [1];  [2];  [1];  [1];  [1];  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Univ. of Chicago, IL (United States). Graduate Program in Biophysics

In this paper, 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). Finally, 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.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1339164
Journal Information:
ChemComm, Vol. 51, Issue 53; ISSN 1359-7345
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 41 works
Citation information provided by
Web of Science

References (35)

Toward Cost-Effective Solar Energy Use journal February 2007
Powering the planet: Chemical challenges in solar energy utilization journal October 2006
Photo-induced hydrogen production in a helical peptide incorporating a [FeFe] hydrogenase active site mimic journal January 2012
A hydrogenase model system based on the sequence of cytochrome c: photochemical hydrogen evolution in aqueous media journal January 2011
Photoinduced Hydrogen Evolution Catalyzed by a Synthetic Diiron Dithiolate Complex Embedded within a Protein Matrix journal July 2014
Protein secondary-shell interactions enhance the photoinduced hydrogen production of cobalt protoporphyrin IX journal January 2014
Cobaloxime-Based Artificial Hydrogenases journal July 2014
Photocatalytic hydrogen evolution by a diiron hydrogenase model based on a peptide fragment of cytochrome c556 with an attached diiron carbonyl cluster and an attached ruthenium photosensitizer journal March 2012
Nature-Driven Photochemistry for Catalytic Solar Hydrogen Production: A Photosystem I–Transition Metal Catalyst Hybrid journal October 2011
Protein Delivery of a Ni Catalyst to Photosystem I for Light-Driven Hydrogen Production journal August 2013
Hydrogen Evolution Catalyzed by Cobaloximes journal December 2009
Selective Reduction of Aqueous Protons to Hydrogen with a Synthetic Cobaloxime Catalyst in the Presence of Atmospheric Oxygen journal August 2012
Structure–function analyses of solar fuelscatalysts using in situ X-ray scattering journal January 2013
Cobaloxime-Based Photocatalytic Devices for Hydrogen Production journal January 2008
Light-driven hydrogen production from Photosystem I-catalyst hybrids journal April 2015
Intermolecular electron transfer in cytochrome P450cam covalently bound with Tris(2,2′-bipyridyl)ruthenium(II): structural changes detected by FTIR spectroscopy journal September 2002
Characterization of the structure, properties, and reactivity of a cobalt(II) macrocyclic complex journal November 1986
The Hydrogen Catalyst Cobaloxime: A Multifrequency EPR and DFT Study of Cobaloxime’s Electronic Structure journal February 2012
Homogeneous catalysis of the photoreduction of water by visible light. 2. Mediation by a tris(2,2'-bipyridine)ruthenium(II)-cobalt(II) bipyridine system journal April 1981
A cobalt–NHC complex as an improved catalyst for photochemical hydrogen evolution from water journal January 2014
(Bipyridine)(terpyridine)(4-iodophenylcyanamide)ruthenium(II) complex: crystallography, electronic absorption spectroscopy, cyclic voltammetry and EPR measurements journal May 2001
ESR and MO studies of some C4v symmetrical ruthenium(III) complexes journal March 1982
Localized states in reduced and excited-state ruthenium(II) terpyridyls journal November 1988
ESR of the reduction products of [Fe(bpy)3]2+ and [Ru(bpy)3]2+ journal May 1981
Solvent-induced EPR anisotropy change of the non-heme chromophore of spinach ferredoxin journal October 1970
Detection of a charge-separated catalyst precursor state in a linked photosensitizer-catalyst assembly journal January 2013
Reductive Quenching of Novel Mixed-Ligand Tris(bipyridyl)ruthenium(II) Complexes in Aqueous Solution and Inert Colloidal Suspensions journal June 1994
Mechanistic Details for Cobalt Catalyzed Photochemical Hydrogen Production in Aqueous Solution: Efficiencies of the Photochemical and Non-Photochemical Steps journal April 2013
Mechanism of Photocatalytic Hydrogen Generation by a Polypyridyl-Based Cobalt Catalyst in Aqueous Solution journal December 2014
Visible Light-Driven Hydrogen Production from Aqueous Protons Catalyzed by Molecular Cobaloxime Catalysts journal June 2009
Chemical Approaches to Artificial Photosynthesis. 2 journal October 2005
Midpoint redox potentials of plant and algal ferredoxins journal November 1977
Electrocatalytic Hydrogen Evolution at Low Overpotentials by Cobalt Macrocyclic Glyoxime and Tetraimine Complexes journal July 2007
Theoretical studies of the mechanism of catalytic hydrogen production by a cobaloxime journal January 2011
Substituent Effects on Cobalt Diglyoxime Catalysts for Hydrogen Evolution journal November 2011

Cited By (5)

Hybrid Photoelectrochemical Water Splitting Systems: From Interface Design to System Assembly journal June 2019
Photosensitised Multiheme Cytochromes as Light-Driven Molecular Wires and Resistors journal September 2018
Designing a modified clostridial 2[4Fe–4S] ferredoxin as a redox coupler to directly link photosystem I with a Pt nanoparticle journal October 2019
From protein engineering to artificial enzymes – biological and biomimetic approaches towards sustainable hydrogen production journal January 2018
The oxygen reactivity of an artificial hydrogenase designed in a reengineered copper storage protein journal January 2020

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