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

Soltau, Sarah R.; Niklas, Jens; Dahlberg, Peter D.; Poluektov, Oleg G.; Tiede, David M.; Mulfort, Karen L.; Utschig, Lisa M.

doi:10.1039/C5CC03006D

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

Abstract

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.

Authors:

Soltau, Sarah R. ^[1]; Niklas, Jens ^[1]; Dahlberg, Peter D. ^[2]; Poluektov, Oleg G. ^[1]; Tiede, David M. ^[1]; Mulfort, Karen L. ^[1]; Utschig, Lisa M. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Univ. of Chicago, IL (United States). Graduate Program in Biophysics

Publication Date:: Mon Jun 08 00:00:00 EDT 2015

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1339164

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: ChemComm

Additional Journal Information:: Journal Volume: 51; Journal Issue: 53; Journal ID: ISSN 1359-7345

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 08 HYDROGEN; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Soltau, Sarah R., Niklas, Jens, Dahlberg, Peter D., Poluektov, Oleg G., Tiede, David M., Mulfort, Karen L., and Utschig, Lisa M. Aqueous light driven hydrogen production by a Ru–ferredoxin–Co biohybrid.  United States: N. p., 2015. 
Web.  doi:10.1039/C5CC03006D.

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                    Soltau, Sarah R., Niklas, Jens, Dahlberg, Peter D., Poluektov, Oleg G., Tiede, David M., Mulfort, Karen L., & Utschig, Lisa M. Aqueous light driven hydrogen production by a Ru–ferredoxin–Co biohybrid.  United States.  https://doi.org/10.1039/C5CC03006D

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                    Soltau, Sarah R., Niklas, Jens, Dahlberg, Peter D., Poluektov, Oleg G., Tiede, David M., Mulfort, Karen L., and Utschig, Lisa M. Mon .  
"Aqueous light driven hydrogen production by a Ru–ferredoxin–Co biohybrid".  United States.  https://doi.org/10.1039/C5CC03006D.  https://www.osti.gov/servlets/purl/1339164.

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@article{osti_1339164,

  title        = {Aqueous light driven hydrogen production by a Ru–ferredoxin–Co biohybrid},

  author       = {Soltau, Sarah R. and Niklas, Jens and Dahlberg, Peter D. and Poluektov, Oleg G. and Tiede, David M. and Mulfort, Karen L. and Utschig, Lisa M.},

  abstractNote = {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.},

  doi          = {10.1039/C5CC03006D},

  journal      = {ChemComm},

  number       = 53,

  volume       = 51,

  place        = {United States},

  year         = {Mon Jun 08 00:00:00 EDT 2015},

  month        = {Mon Jun 08 00:00:00 EDT 2015}

}

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

Abstract

Citation Formats

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

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Photosensitised Multiheme Cytochromes as Light-Driven Molecular Wires and Resistors journal, September 2018

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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
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Photoinduced Hydrogen Evolution Catalyzed by a Synthetic Diiron Dithiolate Complex Embedded within a Protein Matrix
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Protein secondary-shell interactions enhance the photoinduced hydrogen production of cobalt protoporphyrin IX
journal, January 2014

Cobaloxime-Based Artificial Hydrogenases
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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
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Nature-Driven Photochemistry for Catalytic Solar Hydrogen Production: A Photosystem I–Transition Metal Catalyst Hybrid
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Protein Delivery of a Ni Catalyst to Photosystem I for Light-Driven Hydrogen Production
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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
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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

Hybrid Photoelectrochemical Water Splitting Systems: From Interface Design to System Assembly
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Photosensitised Multiheme Cytochromes as Light-Driven Molecular Wires and Resistors
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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
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