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Title: Replacing a Cysteine Ligand by Selenocysteine in a [NiFe]-Hydrogenase Unlocks Hydrogen Production Activity and Addresses the Role of Concerted Proton-Coupled Electron Transfer in Electrocatalytic Reversibility

Journal Article · · Journal of the American Chemical Society
 [1]; ORCiD logo [2];  [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]
  1. Department of Chemistry, University of Oxford, Oxford OX1 3TA, United Kingdom
  2. Department of Biochemistry and Molecular Biology, University of Georgia, Athens, Georgia 30602, United States
  3. Department of Molecular Biophysics and Biochemistry, Yale University, New Haven, Connecticut 06511, United States, Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States

Not Available

Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
FG02-98ER20311
OSTI ID:
2350845
Alternate ID(s):
OSTI ID: 2394610
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 25 Vol. 146; ISSN 0002-7863
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (60)

Spectroscopic and Electrochemical Characterization of the [NiFeSe] Hydrogenase from Desulfovibrio vulgaris Miyazaki F: Reversible Redox Behavior and Interactions between Electron Transfer Centers journal September 2013
From Protein Film Electrochemistry to Nanoconfined Enzyme Cascades and the Electrochemical Leaf journal December 2022
Selenium versus sulfur: Reversibility of chemical reactions and resistance to permanent oxidation in proteins and nucleic acids journal November 2018
Proton Transfer in the Catalytic Cycle of [NiFe] Hydrogenases: Insight from Vibrational Spectroscopy journal March 2017
Selenium—More than Just a Fortuitous Sulfur Substitute in Redox Biology journal December 2023
The energetics and evolution of oxidoreductases in deep time journal August 2023
Structural Determinants of the Catalytic Nia-L Intermediate of [NiFe]-Hydrogenase journal June 2023
[NiFeSe]-Hydrogenase Chemistry journal October 2015
Mechanistic Exploitation of a Self-Repairing, Blocked Proton Transfer Pathway in an O 2 -Tolerant [NiFe]-Hydrogenase journal July 2018
Two Pathways for Electrocatalytic Oxidation of Hydrogen by a Nickel Bis(diphosphine) Complex with Pendant Amines in the Second Coordination Sphere journal June 2013
The value of enzymes in solar fuels research – efficient electrocatalysts through evolution journal January 2019
Proton-Coupled Electron Transfer in Solution, Proteins, and Electrochemistry journal November 2008
Volcano Activity Relationships for Proton-Coupled Electron Transfer Reactions in Electrocatalysis journal September 2015
Understanding and Design of Bidirectional and Reversible Catalysts of Multielectron, Multistep Reactions journal June 2019
Selenium and Sulfur in Exchange Reactions: A Comparative Study journal August 2010
Free Energies of Proton-Coupled Electron Transfer Reagents and Their Applications journal December 2021
The catalytic cycle of [FeFe] hydrogenase: A tale of two sites journal December 2021
Guiding Principles of Hydrogenase Catalysis Instigated and Clarified by Protein Film Electrochemistry journal April 2016
Discovery of Dark pH-Dependent H+ Migration in a [NiFe]-Hydrogenase and Its Mechanistic Relevance: Mobilizing the Hydrido Ligand of the Ni-C Intermediate journal June 2015
Introducing Selenocysteine into Recombinant Proteins in Escherichia coli journal February 2021
Glutamic Acid 204 is the Terminal Proton Release Group at the Extracellular Surface of Bacteriorhodopsin journal November 1995
How Escherichia coli Is Equipped to Oxidize Hydrogen under Different Redox Conditions journal November 2009
Mechanism of hydrogen activation by [NiFe] hydrogenases journal November 2015
Proton Transfer Mechanisms in Bimetallic Hydrogenases journal December 2020
Theoretical Modeling of Electrochemical Proton-Coupled Electron Transfer journal March 2022
Theory of Coupled Electron and Proton Transfer Reactions journal December 2010
Mapping Proton Wires in Proteins: Carbonic Anhydrase and GFP Chromophore Biosynthesis journal April 2009
Thermodynamics and kinetics of proton-coupled electron transfer: stepwise vs. concerted pathways journal April 2004
Atomically defined mechanism for proton transfer to a buried redox centre in a protein journal June 2000
Reversible catalysis journal April 2021
Proton-Coupled Electron Transfer: Moving Together and Charging Forward journal July 2015
A Glutamate Is the Essential Proton Transfer Gate during the Catalytic Cycle of the [NiFe] Hydrogenase journal December 2003
Proton Inventory and Dynamics in the Ni a -S to Ni a -C Transition of a [NiFe] Hydrogenase journal March 2016
Direct comparison of the electrocatalytic oxidation of hydrogen by an enzyme and a platinum catalystElectronic supplementary information (ESI) available: Levich plots at 1% and 10% hydrogen, and a comparison of the effect of carbon monoxide on oxidation currents obtained at platinum and enzyme-modified electrodes. See http://www.rsc.org/suppdata/cc/b2/b201337a/ journal March 2002
Infrared Spectroscopy During Electrocatalytic Turnover Reveals the Ni-L Active Site State During H 2 Oxidation by a NiFe Hydrogenase journal April 2015
The direct role of selenocysteine in [NiFeSe] hydrogenase maturation and catalysis journal March 2017
The structure of hydrogenase-2 from Escherichia coli: implications for H2-driven proton pumping journal April 2018
Glutamate Gated Proton-Coupled Electron Transfer Activity of a [NiFe]-Hydrogenase journal September 2016
The Difference a Se Makes? Oxygen-Tolerant Hydrogen Production by the [NiFeSe]-Hydrogenase from Desulfomicrobium baculatum journal October 2008
Why Nature Chose Selenium journal February 2016
Electrochemical Approach to the Mechanistic Study of Proton-Coupled Electron Transfer journal July 2008
Protonation of glycine, serine and cysteine. Conformations, proton affinities and intrinsic basicities journal March 2001
Assembly of Tat‐dependent [NiFe] hydrogenases: identification of precursor‐binding accessory proteins journal July 2003
Long-Range Electron Tunneling journal February 2014
Reversibility and efficiency in electrocatalytic energy conversion and lessons from enzymes journal August 2011
Kinetic Modeling of the Reversible or Irreversible Electrochemical Responses of FeFe-Hydrogenases journal January 2024
Proton-Coupled Electron Transfer Dynamics in the Catalytic Mechanism of a [NiFe]-Hydrogenase journal March 2015
Proton-Coupled Electron Transfer: The Engine of Energy Conversion and Storage journal January 2022
Intermediates in the Catalytic Cycle of [NiFe] Hydrogenase: Functional Spectroscopy of the Active Site journal April 2010
Transforming an oxygen-tolerant [NiFe] uptake hydrogenase into a proficient, reversible hydrogen producer journal January 2014
Protonation states of intermediates in the reaction mechanism of [NiFe] hydrogenase studied by computational methods journal March 2016
Selenium in chemistry and biochemistry in comparison to sulfur journal January 2007
Proton-Coupled Electron Transfer Guidelines, Fair and Square journal January 2021
Protein film electrochemistry journal October 2023
Cysteine SH and Glutamate COOH Contributions to [NiFe] Hydrogenase Proton Transfer Revealed by Highly Sensitive FTIR Spectroscopy journal September 2019
The roles of long-range proton-coupled electron transfer in the directionality and efficiency of [FeFe]-hydrogenases journal August 2020
Natural expansion of the genetic code journal December 2006
Comprehensive structural, infrared spectroscopic and kinetic investigations of the roles of the active-site arginine in bidirectional hydrogen activation by the [NiFe]-hydrogenase ‘Hyd-2’ from Escherichia coli journal January 2023
A Facile Method for Producing Selenocysteine-Containing Proteins journal May 2018
Selective cysteine-to-selenocysteine changes in a [NiFe]-hydrogenase confirm a special position for catalysis and oxygen tolerance journal March 2021

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