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Title: Seven Coordinated Molecular Ruthenium–Water Oxidation Catalysts: A Coordination Chemistry Journey: Focus Review

Abstract

Molecular water oxidation catalysis is a field that has experienced an impressive development over the past decade mainly fueled by the promise of generation of a sustainable carbon neutral fuel society, based on water splitting. Most of these advancements have been possible thanks to the detailed understanding of the reactions and intermediates involved in the catalytic cycles. Today’s best molecular water oxidation catalysts reach turnover frequencies that are orders of magnitude higher than that of the natural oxygen evolving center in photosystem II. These catalysts are based on Ru complexes where at some stage, the first coordination sphere of the metal center becomes seven coordinated. The key for this achievement is largely based on the use of adaptative ligands that adjust their coordination mode depending on the structural and electronic demands of the metal center at different oxidation states accessed within the catalytic cycle. Here, this Review covers the latest and most significant developments on Ru complexes that behave as powerful water oxidation catalysts and where at some stage the Ru metal attains coordination number 7. Further it provides a comprehensive and rational understanding of the different structural and electronic factors that govern the behavior of these catalysts.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]
  1. Barcelona Institute of Science and Technology (BIST), Tarragona (Spain); Univ. Rovira i Virgili, Tarragona (Spain)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Barcelona Institute of Science and Technology (BIST), Tarragona (Spain)
  4. Univ. Autonoma de Barcelona, Barcelona (Spain)
  5. Barcelona Institute of Science and Technology (BIST), Tarragona (Spain); Univ. Autonoma de Barcelona, Barcelona (Spain)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1497379
Report Number(s):
BNL-211301-2019-JAAM
Journal ID: ISSN 0009-2665
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Reviews
Additional Journal Information:
Journal Volume: 119; Journal Issue: 6; Journal ID: ISSN 0009-2665
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; water oxidation; water splitting; molecular catalysis; redox properties; transition metal complexes; energy conversion

Citation Formats

Matheu, Roc, Ertem, Mehmed Z., Gimbert-Suriñach, Carolina, Sala, Xavier, and Llobet, Antoni. Seven Coordinated Molecular Ruthenium–Water Oxidation Catalysts: A Coordination Chemistry Journey: Focus Review. United States: N. p., 2019. Web. doi:10.1021/acs.chemrev.8b00537.
Matheu, Roc, Ertem, Mehmed Z., Gimbert-Suriñach, Carolina, Sala, Xavier, & Llobet, Antoni. Seven Coordinated Molecular Ruthenium–Water Oxidation Catalysts: A Coordination Chemistry Journey: Focus Review. United States. doi:10.1021/acs.chemrev.8b00537.
Matheu, Roc, Ertem, Mehmed Z., Gimbert-Suriñach, Carolina, Sala, Xavier, and Llobet, Antoni. Thu . "Seven Coordinated Molecular Ruthenium–Water Oxidation Catalysts: A Coordination Chemistry Journey: Focus Review". United States. doi:10.1021/acs.chemrev.8b00537.
@article{osti_1497379,
title = {Seven Coordinated Molecular Ruthenium–Water Oxidation Catalysts: A Coordination Chemistry Journey: Focus Review},
author = {Matheu, Roc and Ertem, Mehmed Z. and Gimbert-Suriñach, Carolina and Sala, Xavier and Llobet, Antoni},
abstractNote = {Molecular water oxidation catalysis is a field that has experienced an impressive development over the past decade mainly fueled by the promise of generation of a sustainable carbon neutral fuel society, based on water splitting. Most of these advancements have been possible thanks to the detailed understanding of the reactions and intermediates involved in the catalytic cycles. Today’s best molecular water oxidation catalysts reach turnover frequencies that are orders of magnitude higher than that of the natural oxygen evolving center in photosystem II. These catalysts are based on Ru complexes where at some stage, the first coordination sphere of the metal center becomes seven coordinated. The key for this achievement is largely based on the use of adaptative ligands that adjust their coordination mode depending on the structural and electronic demands of the metal center at different oxidation states accessed within the catalytic cycle. Here, this Review covers the latest and most significant developments on Ru complexes that behave as powerful water oxidation catalysts and where at some stage the Ru metal attains coordination number 7. Further it provides a comprehensive and rational understanding of the different structural and electronic factors that govern the behavior of these catalysts.},
doi = {10.1021/acs.chemrev.8b00537},
journal = {Chemical Reviews},
number = 6,
volume = 119,
place = {United States},
year = {2019},
month = {2}
}

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This content will become publicly available on February 28, 2020
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