Water oxidation catalysis with ligand substituted Ru-bpp type complexes

Stephan Roeser, Fernando Bozoglian, Craig J. Richmond, Aaron B League, Mehmed Z. Ertem, Laia Francàs, Pere Miró, Jordi Benet-Buchholz, Chris Cramer, Antoni Llobet

Research output: Contribution to journalArticlepeer-review

21 Scopus citations


A series of symmetric and non-symmetric dinuclear Ru complexes of general formula {[Ru(R2-trpy)(H2O)][Ru(R3-trpy)(H2O)](μ-R1-bpp)}3+ where trpy is 2,2′:6′,2′′-terpyridine, bpp- is 3,5-bis(2-pyridyl)-pyrazolate and R1, R2 and R3 are electron donating (ED) and electron withdrawing (EW) groups such as Me, MeO, NH2 and NO2 have been prepared using microwave assisted techniques. These complexes have been thoroughly characterized by means of analytical (elemental analysis), spectroscopic (UV-vis, NMR) and electrochemical (CV, SQWV, CPE) techniques. The single crystal X-ray structures for one acetate- and one chloro-bridged precursor have also been solved. Kinetic analysis monitored by UV-vis spectroscopy reveals the electronic effects exerted by the ED and EW groups on the substitution kinetics and stoichiometric water oxidation reaction. The catalytic water oxidation activity is evaluated by means of chemically (CeIV), electrochemically, and photochemically induced processes. It is found that, in general, ED groups do not strongly affect the catalytic rates whereas EW groups drastically reduce catalytic rates. Finally, DFT calculations provide a general and experimentally consistent view of the different water oxidation pathways that can operate in the water oxidation reactions catalyzed by these complexes.

Original languageEnglish (US)
Pages (from-to)5088-5101
Number of pages14
JournalCatalysis Science and Technology
Issue number13
StatePublished - 2016

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© The Royal Society of Chemistry 2016.


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