Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex

Matheu, Roc; Ertem, Mehmed Z.; Benet-Buchholz, Jordi; Coronado, Eugenio; Batista, Victor S.; Sala, Xavier; Llobet, Antoni

doi:10.1021/jacs.5b06541

Title: Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex

Authors:

Matheu, Roc ^[1]; Ertem, Mehmed Z. ^[2]; Benet-Buchholz, Jordi ^[1]; Coronado, Eugenio ^[3]; Batista, Victor S. ^[4]; Sala, Xavier ^[5]; Llobet, Antoni ^[6]

Institute of Chemical Research of Catalonia (ICIQ), Avinguda Països Catalans 16, 43007 Tarragona, Spain
Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, United States
Instituto de Ciencia Molecular (ICMol), Universidad de Valencia, 46980 Paterna, Spain
Department of Chemistry, Yale University, P.O. Box 208107, New Haven, Connecticut 06520-8107, United States
Departament de Química, Universitat Autònoma de Barcelona, Cerdanyola del Vallès, 08193 Barcelona, Spain
Institute of Chemical Research of Catalonia (ICIQ), Avinguda Països Catalans 16, 43007 Tarragona, Spain; Departament de Química, Universitat Autònoma de Barcelona, Cerdanyola del Vallès, 08193 Barcelona, Spain

Publication Date:: Wed Aug 12 00:00:00 EDT 2015

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)

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

OSTI Identifier:: 1386273

DOE Contract Number:: SC0001059

Resource Type:: Journal Article

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 137; Journal Issue: 33; Related Information: ANSER partners with Northwestern University (lead); Argonne National Laboratory; University of Chicago; University of Illinois, Urbana-Champaign; Yale University; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, defects, charge transport, spin dynamics, membrane, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly)

Citation Formats


                    Matheu, Roc, Ertem, Mehmed Z., Benet-Buchholz, Jordi, Coronado, Eugenio, Batista, Victor S., Sala, Xavier, and Llobet, Antoni. Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex.  United States: N. p., 2015. 
        Web.  doi:10.1021/jacs.5b06541.

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                    Matheu, Roc, Ertem, Mehmed Z., Benet-Buchholz, Jordi, Coronado, Eugenio, Batista, Victor S., Sala, Xavier, & Llobet, Antoni. Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex.  United States.  https://doi.org/10.1021/jacs.5b06541

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                    Matheu, Roc, Ertem, Mehmed Z., Benet-Buchholz, Jordi, Coronado, Eugenio, Batista, Victor S., Sala, Xavier, and Llobet, Antoni. 2015.  
        "Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex".  United States.  https://doi.org/10.1021/jacs.5b06541.

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@article{osti_1386273,

  title        = {Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex},

  author       = {Matheu, Roc and Ertem, Mehmed Z. and Benet-Buchholz, Jordi and Coronado, Eugenio and Batista, Victor S. and Sala, Xavier and Llobet, Antoni},

  abstractNote = {},

  doi          = {10.1021/jacs.5b06541},

  url          = {https://www.osti.gov/biblio/1386273},
  journal      = {Journal of the American Chemical Society},

  issn         = {0002-7863},

  number       = 33,

  volume       = 137,

  place        = {United States},

  year         = {Wed Aug 12 00:00:00 EDT 2015},

  month        = {Wed Aug 12 00:00:00 EDT 2015}

}

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An Overview of Significant Achievements in Ruthenium-Based Molecular Water Oxidation Catalysis
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Kamdar, Jayneil; Grotjahn, Douglas
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https://doi.org/10.3390/molecules24030494

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Title: Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex

Citation Formats

Molecular artificial photosynthesis journal, January 2014

Role of ligands in catalytic water oxidation by mononuclear ruthenium complexes journal, December 2015

Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction journal, October 2013

Benchmarking Hydrogen Evolving Reaction and Oxygen Evolving Reaction Electrocatalysts for Solar Water Splitting Devices journal, March 2015

Solution-Cast Metal Oxide Thin Film Electrocatalysts for Oxygen Evolution journal, October 2012

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Wireless Solar Water Splitting Using Silicon-Based Semiconductors and Earth-Abundant Catalysts journal, September 2011

A hole-conductor-free, fully printable mesoscopic perovskite solar cell with high stability journal, July 2014

Molecular Catalysts that Oxidize Water to Dioxygen journal, January 2009

Oxygen−Oxygen Bond Formation Pathways Promoted by Ruthenium Complexes journal, December 2009

Catalytic oxidation of water by an oxo-bridged ruthenium dimer journal, July 1982

A New Ru Complex Capable of Catalytically Oxidizing Water to Molecular Dioxygen journal, June 2004

Water Oxidation by a Mononuclear Ruthenium Catalyst: Characterization of the Intermediates journal, September 2011

One Site is Enough. Catalytic Water Oxidation by [Ru(tpy)(bpm)(OH 2 )] 2+ and [Ru(tpy)(bpz)(OH 2 )] 2+ journal, December 2008

Water Oxidation Catalysis with Nonheme Iron Complexes under Acidic and Basic Conditions: Homogeneous or Heterogeneous? journal, August 2013

Water Oxidation by a Nickel-Glycine Catalyst journal, July 2014

Efficient Chemical and Visible-Light-Driven Water Oxidation using Nickel Complexes and Salts as Precatalysts journal, October 2013

Electrocatalytic Water Oxidation with a Copper(II) Polypeptide Complex journal, January 2013

Redox Non-innocent Ligand Controls Water Oxidation Overpotential in a New Family of Mononuclear Cu-Based Efficient Catalysts journal, May 2015

The cis-[RuII(bpy)2(H2O)2]2+ Water-Oxidation Catalyst Revisited journal, September 2010

Structural Modifications of Mononuclear Ruthenium Complexes: A Combined Experimental and Theoretical Study on the Kinetics of Ruthenium-Catalyzed Water Oxidation journal, December 2010

A Self-Improved Water-Oxidation Catalyst: Is One Site Really Enough? journal, November 2013

Molecular Water Oxidation Mechanisms Followed by Transition Metals: State of the Art journal, December 2013

Experimental and quantum chemical characterization of the water oxidation cycle catalysed by [RuII(damp)(bpy)(H2O)]2+ journal, January 2012

The Ru−Hbpp Water Oxidation Catalyst journal, October 2009

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Mechanism of Water Oxidation by Single-Site Ruthenium Complex Catalysts journal, February 2010

Isolated Seven-Coordinate Ru(IV) Dimer Complex with [HOHOH] − Bridging Ligand as an Intermediate for Catalytic Water Oxidation journal, August 2009

Supramolecular Water Oxidation with Ru-bda-Based Catalysts journal, November 2014

Highly efficient and robust molecular water oxidation catalysts based on ruthenium complexes journal, January 2014

Mononuclear Ruthenium–Water Oxidation Catalysts: Discerning between Electronic and Hydrogen-Bonding Effects journal, June 2012

The OO Bonding in Water Oxidation: the Electronic Structure Portrayal of a Concerted Oxygen Atom-Proton Transfer Pathway journal, June 2011

How Do Proximal Hydroxy or Methoxy Groups on the Bidentate Ligand Affect [(2,2′;6′,2"-Terpyridine)Ru(N,N)X] Water-Oxidation Catalysts? Synthesis, Characterization, and Reactivity at Acidic and Near-Neutral pH: Water-Oxidation Catalysts journal, October 2013

Concerted O atom-proton transfer in the O--O bond forming step in water oxidation journal, April 2010

Base-enhanced catalytic water oxidation by a carboxylate–bipyridine Ru(II) complex journal, April 2015

Direct Access to Terpyridine-Containing Polyazamacrocycles as Photosensitizing Ligands for Eu(III) Luminescence in Aqueous Media journal, March 2005

Substitution Reactions in Dinuclear Ru-Hbpp Complexes: an Evaluation of Through-Space Interactions journal, January 2012

Through-Space Ligand Interactions in Enantiomeric Dinuclear Ru Complexes journal, June 2010

Highly Efficient Binuclear Ruthenium Catalyst for Water Oxidation journal, February 2015

Understanding the eighteen-electron rule journal, October 2006

A new local density functional for main-group thermochemistry, transition metal bonding, thermochemical kinetics, and noncovalent interactions journal, November 2006

M11-L: A Local Density Functional That Provides Improved Accuracy for Electronic Structure Calculations in Chemistry and Physics journal, December 2011

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Hard and Soft Acids and Bases journal, November 1963

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Competitive oxygen-18 kinetic isotope effects expose O–O bond formation in water oxidation catalysis by monomeric and dimeric ruthenium complexes journal, January 2014

A Synthetic Nickel Electrocatalyst with a Turnover Frequency Above 100,000 s-1 for H2 Production journal, August 2011

Ruthenium water oxidation catalysts containing the non-planar tetradentate ligand, biisoquinoline dicarboxylic acid (biqaH 2 ) journal, January 2016

Iridium Water Oxidation Catalysts Based on Pyridine‐Carbene Alkyl‐Substituted Ligands journal, March 2019

Structural evolution of the Ru-bms complex to the real water oxidation catalyst of Ru-bda: the bite angle matters journal, January 2020

Catalytic Oxidation of Water to Dioxygen by Mononuclear Ru Complexes Bearing a 2,6‐Pyridinedicarboxylato Ligand journal, November 2018

Ir- and Ru-doped layered double hydroxides as affordable heterogeneous catalysts for electrochemical water oxidation journal, January 2020

Recent Advances in the Development of Molecular Catalyst‐Based Anodes for Water Oxidation toward Artificial Photosynthesis journal, November 2018

The development of molecular water oxidation catalysts journal, April 2019

Fe, Ru, and Os complexes with the same molecular framework: comparison of structures, properties and catalytic activities journal, January 2017

Collaboration between experiment and theory in solar fuels research journal, January 2019

Modeling the Catalyst Activation Step in a Metal–Ligand Radical Mechanism Based Water Oxidation System journal, May 2019

Ruthenium Water Oxidation Catalysts based on Pentapyridyl Ligands journal, November 2017

Universal scaling relations for the rational design of molecular water oxidation catalysts with near-zero overpotential journal, November 2019

Energetic Effects of a Closed System Approach Including Explicit Proton and Electron Acceptors as Demonstrated by a Mononuclear Ruthenium Water Oxidation Catalyst journal, August 2018

A Bio-inspired Cu 4 O 4 Cubane: Effective Molecular Catalysts for Electrocatalytic Water Oxidation in Aqueous Solution journal, May 2018

Intramolecular hydrogen-bonding in a cobalt aqua complex and electrochemical water oxidation activity journal, January 2018

A Charge‐Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface journal, November 2018

A Charge-Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface journal, October 2018

Water Oxidation Catalysts for Artificial Photosynthesis journal, July 2019

Kinetics and mechanisms of catalytic water oxidation journal, January 2019

Early photophysical events of a ruthenium( ii ) molecular dyad capable of performing photochemical water oxidation and of its model compounds journal, January 2019

Control over Electrochemical Water Oxidation Catalysis by Preorganization of Molecular Ruthenium Catalysts in Self-Assembled Nanospheres journal, August 2018

Synthesis, Structure, and Water Oxidation Activity of Ruthenium(II) Complexes: Influence of Intramolecular Redox Process on O 2 Evolution : Synthesis, Structure, and Water Oxidation Activity of Ruthenium(II) Complexes: Influence of Intramolecular Redox Process on O journal, June 2018

Molecular artificial photosynthesis
journal, January 2014

Role of ligands in catalytic water oxidation by mononuclear ruthenium complexes
journal, December 2015

Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction
journal, October 2013

Benchmarking Hydrogen Evolving Reaction and Oxygen Evolving Reaction Electrocatalysts for Solar Water Splitting Devices
journal, March 2015

Solution-Cast Metal Oxide Thin Film Electrocatalysts for Oxygen Evolution
journal, October 2012

Photochemical Route for Accessing Amorphous Metal Oxide Materials for Water Oxidation Catalysis
journal, March 2013

Behavior of the Ru-bda Water Oxidation Catalyst Covalently Anchored on Glassy Carbon Electrodes
journal, May 2015

Water Oxidation by Mononuclear Ruthenium Complexes with TPA-Based Ligands
journal, November 2011

Wireless Solar Water Splitting Using Silicon-Based Semiconductors and Earth-Abundant Catalysts
journal, September 2011

A hole-conductor-free, fully printable mesoscopic perovskite solar cell with high stability
journal, July 2014

Molecular Catalysts that Oxidize Water to Dioxygen
journal, January 2009

Oxygen−Oxygen Bond Formation Pathways Promoted by Ruthenium Complexes
journal, December 2009

Catalytic oxidation of water by an oxo-bridged ruthenium dimer
journal, July 1982

A New Ru Complex Capable of Catalytically Oxidizing Water to Molecular Dioxygen
journal, June 2004

Water Oxidation by a Mononuclear Ruthenium Catalyst: Characterization of the Intermediates
journal, September 2011

One Site is Enough. Catalytic Water Oxidation by [Ru(tpy)(bpm)(OH ₂ )] ²⁺ and [Ru(tpy)(bpz)(OH ₂ )] ²⁺
journal, December 2008

Water Oxidation Catalysis with Nonheme Iron Complexes under Acidic and Basic Conditions: Homogeneous or Heterogeneous?
journal, August 2013

Water Oxidation by a Nickel-Glycine Catalyst
journal, July 2014

Efficient Chemical and Visible-Light-Driven Water Oxidation using Nickel Complexes and Salts as Precatalysts
journal, October 2013

Electrocatalytic Water Oxidation with a Copper(II) Polypeptide Complex
journal, January 2013

Redox Non-innocent Ligand Controls Water Oxidation Overpotential in a New Family of Mononuclear Cu-Based Efficient Catalysts
journal, May 2015

The cis-[RuII(bpy)2(H2O)2]2+ Water-Oxidation Catalyst Revisited
journal, September 2010

Structural Modifications of Mononuclear Ruthenium Complexes: A Combined Experimental and Theoretical Study on the Kinetics of Ruthenium-Catalyzed Water Oxidation
journal, December 2010

A Self-Improved Water-Oxidation Catalyst: Is One Site Really Enough?
journal, November 2013

Molecular Water Oxidation Mechanisms Followed by Transition Metals: State of the Art
journal, December 2013

Experimental and quantum chemical characterization of the water oxidation cycle catalysed by [RuII(damp)(bpy)(H2O)]2+
journal, January 2012

The Ru−Hbpp Water Oxidation Catalyst
journal, October 2009

A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II
journal, March 2012

Mechanism of Water Oxidation by Single-Site Ruthenium Complex Catalysts
journal, February 2010

Isolated Seven-Coordinate Ru(IV) Dimer Complex with [HOHOH] ⁻ Bridging Ligand as an Intermediate for Catalytic Water Oxidation
journal, August 2009

Supramolecular Water Oxidation with Ru-bda-Based Catalysts
journal, November 2014

Highly efficient and robust molecular water oxidation catalysts based on ruthenium complexes
journal, January 2014

Mononuclear Ruthenium–Water Oxidation Catalysts: Discerning between Electronic and Hydrogen-Bonding Effects
journal, June 2012

The OO Bonding in Water Oxidation: the Electronic Structure Portrayal of a Concerted Oxygen Atom-Proton Transfer Pathway
journal, June 2011

How Do Proximal Hydroxy or Methoxy Groups on the Bidentate Ligand Affect [(2,2′;6′,2"-Terpyridine)Ru(N,N)X] Water-Oxidation Catalysts? Synthesis, Characterization, and Reactivity at Acidic and Near-Neutral pH: Water-Oxidation Catalysts
journal, October 2013

Concerted O atom-proton transfer in the O--O bond forming step in water oxidation
journal, April 2010

Base-enhanced catalytic water oxidation by a carboxylate–bipyridine Ru(II) complex
journal, April 2015

Direct Access to Terpyridine-Containing Polyazamacrocycles as Photosensitizing Ligands for Eu(III) Luminescence in Aqueous Media
journal, March 2005

Substitution Reactions in Dinuclear Ru-Hbpp Complexes: an Evaluation of Through-Space Interactions
journal, January 2012

Through-Space Ligand Interactions in Enantiomeric Dinuclear Ru Complexes
journal, June 2010

Highly Efficient Binuclear Ruthenium Catalyst for Water Oxidation
journal, February 2015

Understanding the eighteen-electron rule
journal, October 2006

A new local density functional for main-group thermochemistry, transition metal bonding, thermochemical kinetics, and noncovalent interactions
journal, November 2006

M11-L: A Local Density Functional That Provides Improved Accuracy for Electronic Structure Calculations in Chemistry and Physics
journal, December 2011

Cover Picture: Chemical, Electrochemical, and Photochemical Catalytic Oxidation of Water to Dioxygen with Mononuclear Ruthenium Complexes (ChemSusChem 2/2011)
journal, February 2011

Synthesis, Characterization, and Reactivity of Dyad Ruthenium-Based Molecules for Light-Driven Oxidation Catalysis
journal, March 2013

Hard and Soft Acids and Bases
journal, November 1963

Synthesis, Structure, and Spectroscopic, Photochemical, Redox, and Catalytic Properties of Ruthenium(II) Isomeric Complexes Containing Dimethyl Sulfoxide, Chloro, and the Dinucleating Bis(2-pyridyl)pyrazole Ligands
journal, March 2003

Dinuclear Ruthenium Complexes Containing the Hpbl Ligand: Synthesis, Characterization, Linkage Isomerism, and Epoxidation Catalysis
journal, September 2014

Electronic Modification of the [Ru ^II (tpy)(bpy)(OH ₂ )] ²⁺ Scaffold: Effects on Catalytic Water Oxidation
journal, November 2010

Turnover Numbers, Turnover Frequencies, and Overpotential in Molecular Catalysis of Electrochemical Reactions. Cyclic Voltammetry and Preparative-Scale Electrolysis
journal, June 2012

Multielectron, Multistep Molecular Catalysis of Electrochemical Reactions: Benchmarking of Homogeneous Catalysts
journal, June 2014

Evaluation of Homogeneous Electrocatalysts by Cyclic Voltammetry
journal, September 2014

Mechanisms of Photoisomerization and Water-Oxidation Catalysis of Mononuclear Ruthenium(II) Monoaquo Complexes
journal, May 2013

Competitive oxygen-18 kinetic isotope effects expose O–O bond formation in water oxidation catalysis by monomeric and dimeric ruthenium complexes
journal, January 2014

A Synthetic Nickel Electrocatalyst with a Turnover Frequency Above 100,000 s^-1 for H₂ Production
journal, August 2011

Ruthenium water oxidation catalysts containing the non-planar tetradentate ligand, biisoquinoline dicarboxylic acid (biqaH ₂ )
journal, January 2016

Iridium Water Oxidation Catalysts Based on Pyridine‐Carbene Alkyl‐Substituted Ligands
journal, March 2019

Structural evolution of the Ru-bms complex to the real water oxidation catalyst of Ru-bda: the bite angle matters
journal, January 2020

Catalytic Oxidation of Water to Dioxygen by Mononuclear Ru Complexes Bearing a 2,6‐Pyridinedicarboxylato Ligand
journal, November 2018

Ir- and Ru-doped layered double hydroxides as affordable heterogeneous catalysts for electrochemical water oxidation
journal, January 2020

Recent Advances in the Development of Molecular Catalyst‐Based Anodes for Water Oxidation toward Artificial Photosynthesis
journal, November 2018

The development of molecular water oxidation catalysts
journal, April 2019

Fe, Ru, and Os complexes with the same molecular framework: comparison of structures, properties and catalytic activities
journal, January 2017

Collaboration between experiment and theory in solar fuels research
journal, January 2019

Modeling the Catalyst Activation Step in a Metal–Ligand Radical Mechanism Based Water Oxidation System
journal, May 2019

Ruthenium Water Oxidation Catalysts based on Pentapyridyl Ligands
journal, November 2017

Universal scaling relations for the rational design of molecular water oxidation catalysts with near-zero overpotential
journal, November 2019

Energetic Effects of a Closed System Approach Including Explicit Proton and Electron Acceptors as Demonstrated by a Mononuclear Ruthenium Water Oxidation Catalyst
journal, August 2018

A Bio-inspired Cu ₄ O ₄ Cubane: Effective Molecular Catalysts for Electrocatalytic Water Oxidation in Aqueous Solution
journal, May 2018

Intramolecular hydrogen-bonding in a cobalt aqua complex and electrochemical water oxidation activity
journal, January 2018

A Charge‐Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface
journal, November 2018

A Charge-Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface
journal, October 2018

Water Oxidation Catalysts for Artificial Photosynthesis
journal, July 2019

Kinetics and mechanisms of catalytic water oxidation
journal, January 2019

Early photophysical events of a ruthenium( ii ) molecular dyad capable of performing photochemical water oxidation and of its model compounds
journal, January 2019

Control over Electrochemical Water Oxidation Catalysis by Preorganization of Molecular Ruthenium Catalysts in Self-Assembled Nanospheres
journal, August 2018

Synthesis, Structure, and Water Oxidation Activity of Ruthenium(II) Complexes: Influence of Intramolecular Redox Process on O ₂ Evolution : Synthesis, Structure, and Water Oxidation Activity of Ruthenium(II) Complexes: Influence of Intramolecular Redox Process on O
journal, June 2018

Electrochemically Driven Water Oxidation by a Highly Active Ruthenium‐Based Catalyst
journal, April 2019

Synthesis and characterization of [Ru(NC ^NHC O)(bpy)L] ⁺ complexes and their reactivity towards water oxidation
journal, January 2018