O–O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O–O radical coupling

Shaffer, David W.; Xie, Yan; Concepcion, Javier J.

doi:10.1039/C7CS00542C

Title: O–O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O–O radical coupling

Journal Article · Fri Sep 01 00:00:00 EDT 2017 · Chemical Society Reviews

DOI:https://doi.org/10.1039/C7CS00542C· OSTI ID:1405932

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Brookhaven National Lab. (BNL), Upton, NY (United States)

In this review we discuss at the mechanistic level the different steps involved in water oxidation catalysis with ruthenium-based molecular catalysts. We have chosen to focus on ruthenium-based catalysts to provide a more coherent discussion and because of the availability of detailed mechanistic studies for these systems but many of the aspects presented in this review are applicable to other systems as well. The water oxidation cycle has been divided in four major steps: water oxidative activation, O–O bond formation, oxidative activation of peroxide intermediates, and O₂ evolution. A significant portion of the review is dedicated to the O–O bond formation step as the key step in water oxidation catalysis. As a result, the two main pathways to accomplish this step, single-site water nucleophilic attack and O–O radical coupling, are discussed in detail and compared in terms of their potential use in photoelectrochemical cells for solar fuels generation.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1405932

Report Number(s):: BNL-114429-2017-JA; CSRVBR; R&D Project: CO026; KC0304030

Journal Information:: Chemical Society Reviews, Vol. 46, Issue 20; ISSN 0306-0012

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 176 works

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Chemical and Light-Driven Oxidation of Water Catalyzed by an Efficient Dinuclear Ruthenium Complex Xu, Yunhua; Fischer, Andreas; Duan, Lele Angewandte Chemie, Vol. 122, Issue 47 https://doi.org/10.1002/ange.201004278	journal	October 2010
Promoting the Activity of Catalysts for the Oxidation of Water with Bridged Dinuclear Ruthenium Complexes Jiang, Yi; Li, Fei; Zhang, Biaobiao Angewandte Chemie, Vol. 125, Issue 12 https://doi.org/10.1002/ange.201209045	journal	February 2013
Electro-assembly of a Chromophore-Catalyst Bilayer for Water Oxidation and Photocatalytic Water Splitting Ashford, Dennis L.; Sherman, Benjamin D.; Binstead, Robert A. Angewandte Chemie, Vol. 127, Issue 16 https://doi.org/10.1002/ange.201410944	journal	February 2015
Proton-Coupled Electron Transfer J., Meyer, Thomas; V., Huynh, My Hang The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/cywa-5d70	text	January 2007
Crossing the divide between homogeneous and heterogeneous catalysis in water oxidation K., Vannucci, A.; N., Parsons, G.; J., Meyer, T. The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/mx47-fj97	text	January 2013
Experimental demonstration of radicaloid character in a RuV=O intermediate in catalytic water oxidation J., Meyer, T.; J., Concepcion, J.; I., Alperovich, The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/sd6b-fv42	text	January 2013
Proton-coupled electron transfer at modified electrodes by multiple pathways Z., Chen,; W., Jurss, J.; K., Vannucci, A. The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/wfbk-qd18	text	January 2011
Ru‐Hbpp‐Based Water‐Oxidation Catalysts Anchored on Conducting Solid Supports Mola, Joaquim; Mas‐Marza, Elena; Sala, Xavier Angewandte Chemie, Vol. 120, Issue 31 https://doi.org/10.1002/ange.200704912	journal	July 2008
The Possible Role of Proton-Coupled Electron Transfer (PCET) in Water Oxidation by Photosystem II Meyer, Thomas J.; Huynh, My Hang V.; Thorp, H. Holden ChemInform, Vol. 38, Issue 38 https://doi.org/10.1002/chin.200738270	journal	September 2007

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Heterogeneous catalytic water oxidation controlled by coordination geometries of copper( ii ) centers with thiolato donors Kuwamura, Naoto; Kurioka, Yoshinari; Yoshinari, Nobuto Chemical Communications, Vol. 54, Issue 76 https://doi.org/10.1039/c8cc06238b	journal	January 2018
Structural evolution of the Ru-bms complex to the real water oxidation catalyst of Ru-bda: the bite angle matters Yang, Jing; Liu, Bin; Duan, Lele Dalton Transactions, Vol. 49, Issue 14 https://doi.org/10.1039/c9dt04693c	journal	January 2020
Homogeneous photochemical water oxidation with metal salophen complexes in neutral media Asraf, Md. Ali; Ezugwu, Chizoba I.; Zakaria, C. M. Photochemical & Photobiological Sciences, Vol. 18, Issue 11 https://doi.org/10.1039/c9pp00254e	journal	January 2019
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A Charge-Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface Sampaio, Renato N.; Troian-Gautier, Ludovic; Meyer, Gerald J. Angewandte Chemie International Edition, Vol. 57, Issue 47 https://doi.org/10.1002/anie.201807627	journal	October 2018
Cobalt Carbonate as an Electrocatalyst for Water Oxidation Patra, Shanti G.; Illés, Erzsébet; Mizrahi, Amir Chemistry – A European Journal, Vol. 26, Issue 3 https://doi.org/10.1002/chem.201904051	journal	December 2019
Spectroelectrochemical studies of a ruthenium complex containing the pH sensitive 4,4′-dihydroxy-2,2′-bipyridine ligand Viere, Erin J.; Kuhn, Ashley E.; Roeder, Margaret H. Dalton Transactions, Vol. 47, Issue 12 https://doi.org/10.1039/c7dt04554a	journal	January 2018
Computational Modeling of Cobalt-Based Water Oxidation: Current Status and Future Challenges Schilling, Mauro; Luber, Sandra Frontiers in Chemistry, Vol. 6 https://doi.org/10.3389/fchem.2018.00100	journal	April 2018
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Control over Electrochemical Water Oxidation Catalysis by Preorganization of Molecular Ruthenium Catalysts in Self-Assembled Nanospheres Yu, Fengshou; Poole, David; Mathew, Simon Angewandte Chemie International Edition, Vol. 57, Issue 35 https://doi.org/10.1002/anie.201805244	journal	August 2018
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