Several substituted tris(2-pyridyl)phosphine oxide (OPPy3nMe) ruthenium complexes were prepared to examine their potential as water oxidation catalysts. The multi-step synthesis of these complexes from [Ru(η6-C6H6)Cl2]2 occurs cleanly through a κ2-intermediate – [Ru(κ2-OPPy3nMe)(η6-C6H6)(Cl)][PF6], which has been successfully prepared for the unsubstituted tris(2-pyridyl)phosphine as well as the 4-methyl, and 5-methyl substituted derivatives with yields ranging from 45-85%. The in situ formation of a DMF-solvate is followed by the addition of a N,N-chelating ligand (NN) to yield the target ruthenium complexes [Ru(κ3-OPPy3nMe)(NN)(Cl)][PF6] in nearly quantitative yields. The associated 2,2’-bipyridine, 4,4’-dimethylbipyridine, 4,4’-dimethoxybipyridine, 1,10-phenanthroline were successfully prepared, and the isolated products were characterized using 1H and 31P NMR spectroscopies in conjunction with single crystal X-ray diffraction. The potential of the complexes as water oxidation catalysts was examined by cyclic voltammetry.

Substituted tris(2-pyridyl) phosphine oxide ruthenium complexes: Towards water oxidation catalysts

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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