Highly efficient binuclear ruthenium catalyst for water oxidation

ChemSusChem
Anett C SanderFranc Meyer

Abstract

Water splitting is one of the key steps in the conversion of sunlight into a usable renewable energy carrier such as dihydrogen or more complex chemical fuels. Developing rugged and highly efficient catalysts for the oxidative part of water splitting, the water oxidation reaction generating dioxygen, is a major challenge in the field. Herein, we introduce a new, and rationally designed, pyrazolate-based diruthenium complex with the highest activity in water oxidation catalysis for binuclear systems reported to date. Single-crystal X-ray diffraction showed favorable preorganization of the metal ions, well suited for binding two water molecules at a distance adequate for OO bond formation; redox titrations as well as spectroelectrochemistry allowed characterization of the system in several oxidation states. Low oxidation potentials reflect the trianionic character of the elaborate compartmental pyrazolate ligand furnished with peripheral carboxylate groups. Water oxidation has been mediated both by a chemical oxidant (Ce(IV) )-by means of manometry and a Clark electrode for monitoring the dioxygen production-and electrochemically with impressive activities.

References

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Citations

Sep 24, 2015·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Ileana DragutanAlbert Demonceau
Feb 4, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Alejandro CadranelJosé H Hodak
Aug 1, 2015·Journal of the American Chemical Society·Roc MatheuAntoni Llobet
Jun 30, 2015·Inorganic Chemistry·Joan AguilóXavier Sala
Jun 7, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Biswanath DasBjörn Åkermark
Nov 18, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Andrey ShatskiyBjörn Åkermark
Dec 25, 2016·Chemistry : a European Journal·Santanu PattanayakSayam Sen Gupta
Feb 24, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Erin J ViereJared J Paul
Oct 24, 2019·Chemistry : a European Journal·Shanti G PatraDan Meyerstein
Oct 27, 2017·ChemSusChem·Marcos Gil-SepulcreAntoni Llobet
Nov 20, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Abolfazl GhaderianCarolina Gimbert-Suriñach

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