Synthesis, structure, spectroscopy and reactivity of new heterotrinuclear water oxidation catalysts

Chemical Science
Lorenzo MognonAntoni Llobet

Abstract

Four heterotrinuclear complexes containing the ligands 3,5-bis(2-pyridyl)pyrazolate (bpp-) and 2,2':6',2''-terpyridine (trpy) of the general formula {[RuII(trpy)]2(μ-[M(X)2(bpp)2])}(PF6)2, where M = CoII, MnII and X = Cl-, AcO- (M = CoII, X = Cl-: Ru2Co-Cl2 ; M = MnII, X = Cl-: Ru2Mn-Cl2 ; M = CoII, X = AcO-: Ru2Co-OAc2 ; M = MnII, X = AcO-: Ru2Mn-OAc2 ), have been prepared for the first time. The complexes have been characterized using different spectroscopic techniques such as UV-vis, IR, and mass spectrometry. X-Ray diffraction analyses have been used to characterize the Ru2Mn-Cl2 and Ru2Mn-OAc2 complexes. The cyclic voltammograms (CV) for all four complexes in organic solvent (CH3CN or CH2Cl2) display three successive reversible oxidative waves corresponding to one-electron oxidations of each of the three metal centers. The oxidized forms of the complexes Ru2Co-OAc2 and Ru2Mn-OAc2 are further characterized by EPR and UV-vis spectroscopy. The magnetic susceptibility measurements of all complexes in the temperature range of 2-300 K reveal paramagnetic properties due to the presence of high spin Co(ii) and Mn(ii) centers. The complexes Ru2Co-OAc2 and Ru2Mn-OAc2 act as precatalysts for the water oxidation reaction, since the ac...Continue Reading

References

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Jan 10, 2012·Inorganic Chemistry·Stephan RoeserAntoni Llobet
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Jun 8, 2013·Journal of the American Chemical Society·Heejung YoonShunichi Fuhkuzumi
Nov 22, 2013·Angewandte Chemie·Isidoro LópezAntoni Llobet
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Jan 30, 2014·Chemical Society Reviews·Serena BerardiAntoni Llobet
Oct 30, 2014·Chemical Reviews·Markus D KärkäsBjörn Åkermark
Mar 3, 2015·ChemSusChem·Anett C SanderFranc Meyer
May 20, 2015·Journal of the American Chemical Society·Pablo Garrido-BarrosAntoni Llobet
Jul 8, 2015·Chemical Reviews·James D BlakemoreGary W Brudvig
Oct 2, 2015·Faraday Discussions·Lianpeng TongRandolph P Thummel

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Citations

Jul 19, 2017·Chemical Society Reviews·Pablo Garrido-BarrosAntoni Llobet
Jun 5, 2018·Chemical Record : an Official Publication of the Chemical Society of Japan ... [et Al.]·Junqi LinYong Ding
Jul 12, 2017·Chemistry, an Asian Journal·Wei SuFrancis Verpoort
Feb 9, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Hai-Jie LiuXavier Sala
Aug 17, 2016·Journal of the American Chemical Society·Justin J TalbotRyan P Steele

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Methods Mentioned

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