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Title: Balancing electron transfer rate and driving force for efficient photocatalytic hydrogen production in CdSe/CdS nanorod–[NiFe] hydrogenase assemblies

Abstract

We describe a hybrid photocatalytic system for hydrogen production consisting of nanocrystalline CdSe/CdS dot-in-rod (DIR) structures coupled to [NiFe] soluble hydrogenase I (SHI) fromPyrococcus furiosus.

Authors:
 [1];  [2];  [1];  [3];  [1]; ORCiD logo [1]
  1. Department of Chemistry; Emory University; Atlanta; USA
  2. Department of Chemistry and Biochemistry; University of Georgia; Athens; USA
  3. Department of Biochemistry and Molecular Biology; University of Georgia; Athens; USA
Publication Date:
Research Org.:
Emory Univ., Atlanta, GA (United States); Univ. of Georgia, Athens, GA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1539923
DOE Contract Number:  
SC0008798; FG05-95ER20175
Resource Type:
Journal Article
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 10; Journal Issue: 10; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology

Citation Formats

Chica, Bryant, Wu, Chang-Hao, Liu, Yuhgene, Adams, Michael W. W., Lian, Tianquan, and Dyer, R. Brian. Balancing electron transfer rate and driving force for efficient photocatalytic hydrogen production in CdSe/CdS nanorod–[NiFe] hydrogenase assemblies. United States: N. p., 2017. Web. doi:10.1039/c7ee01738c.
Chica, Bryant, Wu, Chang-Hao, Liu, Yuhgene, Adams, Michael W. W., Lian, Tianquan, & Dyer, R. Brian. Balancing electron transfer rate and driving force for efficient photocatalytic hydrogen production in CdSe/CdS nanorod–[NiFe] hydrogenase assemblies. United States. doi:10.1039/c7ee01738c.
Chica, Bryant, Wu, Chang-Hao, Liu, Yuhgene, Adams, Michael W. W., Lian, Tianquan, and Dyer, R. Brian. Sun . "Balancing electron transfer rate and driving force for efficient photocatalytic hydrogen production in CdSe/CdS nanorod–[NiFe] hydrogenase assemblies". United States. doi:10.1039/c7ee01738c.
@article{osti_1539923,
title = {Balancing electron transfer rate and driving force for efficient photocatalytic hydrogen production in CdSe/CdS nanorod–[NiFe] hydrogenase assemblies},
author = {Chica, Bryant and Wu, Chang-Hao and Liu, Yuhgene and Adams, Michael W. W. and Lian, Tianquan and Dyer, R. Brian},
abstractNote = {We describe a hybrid photocatalytic system for hydrogen production consisting of nanocrystalline CdSe/CdS dot-in-rod (DIR) structures coupled to [NiFe] soluble hydrogenase I (SHI) fromPyrococcus furiosus.},
doi = {10.1039/c7ee01738c},
journal = {Energy & Environmental Science},
issn = {1754-5692},
number = 10,
volume = 10,
place = {United States},
year = {2017},
month = {1}
}

Works referenced in this record:

The Scientific Consensus on Climate Change
journal, December 2004


Hydrogen:  An Overview
journal, October 2007

  • Lubitz, Wolfgang; Tumas, William
  • Chemical Reviews, Vol. 107, Issue 10
  • DOI: 10.1021/cr050200z

Direct Evidence of Active-Site Reduction and Photodriven Catalysis in Sensitized Hydrogenase Assemblies
journal, June 2012

  • Greene, Brandon L.; Joseph, Crisjoe A.; Maroney, Michael J.
  • Journal of the American Chemical Society, Vol. 134, Issue 27
  • DOI: 10.1021/ja3042367

Characterization of Photochemical Processes for H 2 Production by CdS Nanorod–[FeFe] Hydrogenase Complexes
journal, March 2012

  • Brown, Katherine A.; Wilker, Molly B.; Boehm, Marko
  • Journal of the American Chemical Society, Vol. 134, Issue 12
  • DOI: 10.1021/ja2116348

Perfect Photon-to-Hydrogen Conversion Efficiency
journal, February 2016


Hydrogenases
journal, March 2014

  • Lubitz, Wolfgang; Ogata, Hideaki; Rüdiger, Olaf
  • Chemical Reviews, Vol. 114, Issue 8
  • DOI: 10.1021/cr4005814

Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybrid
journal, April 2016


Photocatalytic Regeneration of Nicotinamide Cofactors by Quantum Dot–Enzyme Biohybrid Complexes
journal, February 2016


Proton Reduction Using a Hydrogenase-Modified Nanoporous Black Silicon Photoelectrode
journal, June 2016

  • Zhao, Yixin; Anderson, Nicholas C.; Ratzloff, Michael W.
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 23
  • DOI: 10.1021/acsami.6b00189

How Light-Harvesting Semiconductors Can Alter the Bias of Reversible Electrocatalysts in Favor of H 2 Production and CO 2 Reduction
journal, September 2013

  • Bachmeier, Andreas; Wang, Vincent C. C.; Woolerton, Thomas W.
  • Journal of the American Chemical Society, Vol. 135, Issue 40
  • DOI: 10.1021/ja4042675

Controlled Assembly of Hydrogenase-CdTe Nanocrystal Hybrids for Solar Hydrogen Production
journal, July 2010

  • Brown, Katherine A.; Dayal, Smita; Ai, Xin
  • Journal of the American Chemical Society, Vol. 132, Issue 28
  • DOI: 10.1021/ja101031r

Synthesis and enzymatic photo-activity of an O 2 tolerant hydrogenase–CdSe@CdS quantum rod bioconjugate
journal, January 2014

  • Hamon, C.; Ciaccafava, A.; Infossi, P.
  • Chem. Commun., Vol. 50, Issue 39
  • DOI: 10.1039/C3CC49368G

The Crystal Structure of the [NiFe] Hydrogenase from the Photosynthetic Bacterium Allochromatium vinosum: Characterization of the Oxidized Enzyme (Ni-A State)
journal, September 2010

  • Ogata, Hideaki; Kellers, Petra; Lubitz, Wolfgang
  • Journal of Molecular Biology, Vol. 402, Issue 2
  • DOI: 10.1016/j.jmb.2010.07.041

Carbon Dots as Versatile Photosensitizers for Solar-Driven Catalysis with Redox Enzymes
journal, December 2016

  • Hutton, Georgina A. M.; Reuillard, Bertrand; Martindale, Benjamin C. M.
  • Journal of the American Chemical Society, Vol. 138, Issue 51
  • DOI: 10.1021/jacs.6b10146

Carbon nitride–TiO 2 hybrid modified with hydrogenase for visible light driven hydrogen production
journal, January 2015

  • Caputo, Christine A.; Wang, Lidong; Beranek, Radim
  • Chemical Science, Vol. 6, Issue 10
  • DOI: 10.1039/C5SC02017D

Inorganic/whole-cell biohybrid photocatalyst for highly efficient hydrogen production from water
journal, August 2017


Self-photosensitization of nonphotosynthetic bacteria for solar-to-chemical production
journal, December 2015


Water splitting–biosynthetic system with CO 2 reduction efficiencies exceeding photosynthesis
journal, June 2016


Electron Transfer Kinetics in CdS Nanorod–[FeFe]-Hydrogenase Complexes and Implications for Photochemical H 2 Generation
journal, March 2014

  • Wilker, Molly B.; Shinopoulos, Katherine E.; Brown, Katherine A.
  • Journal of the American Chemical Society, Vol. 136, Issue 11
  • DOI: 10.1021/ja413001p

Engineering Hyperthermophilic Archaeon Pyrococcus furiosus to Overproduce Its Cytoplasmic [NiFe]-Hydrogenase
journal, December 2011

  • Chandrayan, Sanjeev K.; McTernan, Patrick M.; Hopkins, R. Christopher
  • Journal of Biological Chemistry, Vol. 287, Issue 5, p. 3257-3264
  • DOI: 10.1074/jbc.M111.290916

Near Unity Quantum Yield of Light-Driven Redox Mediator Reduction and Efficient H 2 Generation Using Colloidal Nanorod Heterostructures
journal, July 2012

  • Zhu, Haiming; Song, Nianhui; Lv, Hongjin
  • Journal of the American Chemical Society, Vol. 134, Issue 28
  • DOI: 10.1021/ja303698e

Hydrogen Production by Molecular Photocatalysis
journal, October 2007

  • Esswein, Arthur J.; Nocera, Daniel G.
  • Chemical Reviews, Vol. 107, Issue 10
  • DOI: 10.1021/cr050193e

Improved Hydrogen Production with Tetramethyl-and Hexamethylviologen as Electron-Transfer Agents in the System H 2 O-Ru(bpy) 2+ 3 -edta-Pt
journal, January 1982

  • Launikonis, Anton; Loder, John W.; Mau, Albert W. -H.
  • Israel Journal of Chemistry, Vol. 22, Issue 2
  • DOI: 10.1002/ijch.198200030

Excited-state electron-transfer quenching by a series of water photoreduction mediators
journal, September 1980


On the Effect of Electron Relay Redox Potential on Electron Transfer Reactions in a Water Photoreduction Model System
journal, January 1982


Photochemical production of hydrogen from water
journal, May 1985


Mechanisms for Adsorption of Methyl Viologen on CdS Quantum Dots
journal, February 2014

  • Peterson, Mark D.; Jensen, Stephen C.; Weinberg, David J.
  • ACS Nano, Vol. 8, Issue 3
  • DOI: 10.1021/nn406651a

Hole Removal Rate Limits Photodriven H 2 Generation Efficiency in CdS-Pt and CdSe/CdS-Pt Semiconductor Nanorod–Metal Tip Heterostructures
journal, May 2014

  • Wu, Kaifeng; Chen, Zheyuan; Lv, Hongjin
  • Journal of the American Chemical Society, Vol. 136, Issue 21
  • DOI: 10.1021/ja5023893

Direct Determination of Thiol p K a by Isothermal Titration Microcalorimetry
journal, September 2004

  • Tajc, Stephen G.; Tolbert, Blanton S.; Basavappa, Ravi
  • Journal of the American Chemical Society, Vol. 126, Issue 34
  • DOI: 10.1021/ja047929u

Kinetic Characterization of the Endogenous Glutathione Transferase Activity of Octopus Lens S-Crystallin
journal, June 1996


Kinetics of reduction of eight viologens by dithionite ion
journal, May 1985

  • Tsukahara, K.; Wilkins, R. G.
  • Journal of the American Chemical Society, Vol. 107, Issue 9
  • DOI: 10.1021/ja00295a013

Robust Photogeneration of H2 in Water Using Semiconductor Nanocrystals and a Nickel Catalyst
journal, November 2012


Wave Function Engineering for Ultrafast Charge Separation and Slow Charge Recombination in Type II Core/Shell Quantum Dots
journal, June 2011

  • Zhu, Haiming; Song, Nianhui; Lian, Tianquan
  • Journal of the American Chemical Society, Vol. 133, Issue 22
  • DOI: 10.1021/ja202752s

Beyond Band Alignment: Hole Localization Driven Formation of Three Spatially Separated Long-Lived Exciton States in CdSe/CdS Nanorods
journal, July 2013

  • Wu, Kaifeng; Rodríguez-Córdoba, William E.; Liu, Zheng
  • ACS Nano, Vol. 7, Issue 8
  • DOI: 10.1021/nn402597p

Observation of trapped-hole diffusion on the surfaces of CdS nanorods
journal, July 2016

  • Utterback, James K.; Grennell, Amanda N.; Wilker, Molly B.
  • Nature Chemistry, Vol. 8, Issue 11
  • DOI: 10.1038/nchem.2566

Alternating layer addition approach to CdSe/CdS core/shell quantum dots with near-unity quantum yield and high on-time fractions
journal, January 2012

  • Greytak, Andrew B.; Allen, Peter M.; Liu, Wenhao
  • Chemical Science, Vol. 3, Issue 6
  • DOI: 10.1039/c2sc00561a

Competition of branch-to-core exciton localization and interfacial electron transfer in CdSe tetrapods
journal, June 2016


Wavelength dependent efficient photoreduction of redox mediators using type II ZnSe/CdS nanorod heterostructures
journal, January 2014

  • Zhu, Haiming; Chen, Zheyuan; Wu, Kaifeng
  • Chem. Sci., Vol. 5, Issue 10
  • DOI: 10.1039/C4SC01549E

Unravelling the pH-dependence of a molecular photocatalytic system for hydrogen production
journal, January 2015

  • Reynal, Anna; Pastor, Ernest; Gross, Manuela A.
  • Chemical Science, Vol. 6, Issue 8
  • DOI: 10.1039/C5SC01349F

Mechanistic Insights into the Interface-Directed Transformation of Thiols into Disulfides and Molecular Hydrogen by Visible-Light Irradiation of Quantum Dots
journal, January 2014

  • Li, Xu-Bing; Li, Zhi-Jun; Gao, Yu-Ji
  • Angewandte Chemie International Edition, Vol. 53, Issue 8
  • DOI: 10.1002/anie.201310249

Proton-Coupled Electron Transfer Dynamics in the Catalytic Mechanism of a [NiFe]-Hydrogenase
journal, March 2015

  • Greene, Brandon L.; Wu, Chang-Hao; McTernan, Patrick M.
  • Journal of the American Chemical Society, Vol. 137, Issue 13
  • DOI: 10.1021/jacs.5b01791

Redox regulation by glutathione needs enzymes
journal, July 2014

  • Berndt, Carsten; Lillig, Christopher H.; Flohé, Leopold
  • Frontiers in Pharmacology, Vol. 5
  • DOI: 10.3389/fphar.2014.00168

Reversible Biological Birch Reduction at an Extremely Low Redox Potential
journal, July 2010

  • Kung, Johannes W.; Baumann, Sven; von Bergen, Martin
  • Journal of the American Chemical Society, Vol. 132, Issue 28
  • DOI: 10.1021/ja103448u

Clean Donor Oxidation Enhances the H 2 Evolution Activity of a Carbon Quantum Dot-Molecular Catalyst Photosystem
journal, June 2016

  • Martindale, Benjamin C. M.; Joliat, Evelyne; Bachmann, Cyril
  • Angewandte Chemie International Edition, Vol. 55, Issue 32
  • DOI: 10.1002/anie.201604355

Ascorbate as an electron relay between an irreversible electron donor and Ru( ii ) or Re( i ) photosensitizers
journal, January 2014

  • Bachmann, Cyril; Probst, Benjamin; Guttentag, Miguel
  • Chem. Commun., Vol. 50, Issue 51
  • DOI: 10.1039/C4CC01500B

A unified model for surface electrocatalysis based on observations with enzymes
journal, January 2014

  • Hexter, Suzannah V.; Esterle, Thomas F.; Armstrong, Fraser A.
  • Physical Chemistry Chemical Physics, Vol. 16, Issue 24
  • DOI: 10.1039/c3cp55230f

Nitrogenase bioelectrocatalysis: heterogeneous ammonia and hydrogen production by MoFe protein
journal, January 2016

  • Milton, Ross D.; Abdellaoui, Sofiene; Khadka, Nimesh
  • Energy & Environmental Science, Vol. 9, Issue 8
  • DOI: 10.1039/C6EE01432A

Revisiting the IspH Catalytic System in the Deoxyxylulose Phosphate Pathway: Achieving High Activity
journal, July 2009

  • Xiao, Youli; Chu, Lisa; Sanakis, Yiannis
  • Journal of the American Chemical Society, Vol. 131, Issue 29
  • DOI: 10.1021/ja903778d

504. The stereochemistry of the bridged quaternary salts of 2,2′-bipyridyl
journal, January 1960


Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach
journal, October 2007

  • Carbone, Luigi; Nobile, Concetta; De Giorgi, Milena
  • Nano Letters, Vol. 7, Issue 10
  • DOI: 10.1021/nl0717661

A Modular Phase Transfer and Ligand Exchange Protocol for Quantum Dots
journal, April 2011

  • Zylstra, Joshua; Amey, Jennifer; Miska, Nathaniel J.
  • Langmuir, Vol. 27, Issue 8
  • DOI: 10.1021/la104542n

High yield purification of a tagged cytoplasmic [NiFe]-hydrogenase and a catalytically-active nickel-free intermediate form
journal, March 2015

  • Chandrayan, Sanjeev K.; Wu, Chang-Hao; McTernan, Patrick M.
  • Protein Expression and Purification, Vol. 107
  • DOI: 10.1016/j.pep.2014.10.018