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The effects of replacing a single polypyridyl ligand with an analogous anionic cyclometalating ligand were Investigated for a set of three structurally related series of Ru(II) compounds formulated as [Ru(bpy)2(L)] z, [Ru(tpy)(L)]z, and [Ru(tpy)(L)Cl]z, where z=0, -1, or +2, and L = polypyridyl (e.g., bpy=2,2′-blpyridlne, tpy = 2,2′:6′,2″-terpyridine) or cyclometalating ligand (e.g., deprotonated forms of 2-phenylpyridlne or 3-(2-pyridinyl)-benzoic acid). Each of the complexes were synthesized and characterized by1H NMR spectroscopy, electrospray ionization mass spectrometry (ESI-MS), and/or elemental analyses (EA). Cyclic voltammetry reveals that cyclometalation causes a shift of the first oxidation and reduction potentials by -0.5 to -0.8 V and -0.2 to -0.4 V, respectively, relative to their polypyridyl congeners. These disparate shifts have the effect of inducing a bathochromic shift of the lowest-energy absorption bands by as much as 90 nm. With the aid of time-dependent density functional theory (DFT), the lowest-energy bands (lambdamax = 500-575 nm) were assigned as predominantly metal-to-ligand charge-transfer (MLCT) transitions from Ru to the polypyridyl ligands, while Ru?C^N(or C^N^Nor N^C^N transitions are found within the absorption bands centered at ca. 400 nm. The properties of a series of compounds furnished with carboxylic acid anchoring groups at various positions are also examined for applications Involving the sensitization of metal-oxide semiconductors. It Is determined that the thermodynamic potentials of many of these compounds are appropriate for conventional photoelectrochemical cells (e.g., dye-sensitized solar cells) that utilize a titania electrode and iodide-based electrolyte.
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Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI