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Synthesis and Characterization of [Ru(NCNHCO)(bpy)L]+ Complexes and Their Reactivity towards Water Oxidation.

Abstract

While the role of negatively charged axial ligands (e.g. Cl-, Br- and I-) in tuning the reactivity and stability of molecular Ru water oxidation catalysts were well-documented, less were explored when axial ligands are neutral molecules. In this work, we reported the synthesis and full characterization of [Ru(NCNHCO)(bpy)L]+ complexes (L = DMSO, 1; L = 4-picoline, 2), where L is a neutral axial ligand. The effects of these axial ligands on the stability and reactivity of the catalysts were thoroughly investigated. Both complexes were competent to oxidize water with turnover numbers up to 463 and 107, respectively. Complex 1 initiated the water oxidation involving a PCET process. It was found that complex 2 afforded its corresponding Ru-aqua complex owing to the carboxylate dissociation, while complex 1 exhibited a considerable stability in acidic aqueous solution. Whereas in the presence of an oxidant, for complex 1 DMSO/H2O exchange happened facilitating water oxidation. In contrast, the Ru-O bond cleavage of complex 2 was inhibited, leading to an inferior catalytic performance.

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Publication details

The article was received on 25 Aug 2017, accepted on 04 Jan 2018 and first published on 05 Jan 2018


Article type: Paper
DOI: 10.1039/C7NJ03198J
Citation: New J. Chem., 2018, Accepted Manuscript
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    Synthesis and Characterization of [Ru(NCNHCO)(bpy)L]+ Complexes and Their Reactivity towards Water Oxidation.

    F. Cai, W. Su, H. A. Younus, K. Zhou, C. Chen, S. chaemchuen and F. Verpoort, New J. Chem., 2018, Accepted Manuscript , DOI: 10.1039/C7NJ03198J

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