Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 111, Issue 17, Pages 6561-6567Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp067458t
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We report a transient absorption study of the kinetics of re-reduction of ruthenium bipyridyl dye cations adsorbed to nanocrystalline TiO2 films by iodide ions, employing a series of Ru-II(dcbpy)(2)X dyes, where dcpby = 4,4'-dicarboxy-2,2'-bipyridyl and X = (NCS)(2), (CN)(2), DTC (diethyldithiocarbamate), and Cl-2. The data indicate that this re-reduction (or 'regeneration') reaction proceeds via a transient (dye(+)-iodide) intermediate complex formed by reaction of photogenerated dye cations with one iodide ion. The subsequent reaction of this complex with a second iodide ion, forming I-2(-), is shown to be the kinetically and thermodynamically limiting step in the overall regeneration reaction. The implications of this reaction scheme for the function of dye sensitized photoelectrochemical cells are discussed, considering in particular the high photovoltaic efficiencies obtained for such devices employing such ruthenium bipyridyl senstiser dyes in combination with iodide/tri-iodide based redox electrolytes.
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