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Chloride, Bromide, and Iodide Photooxidation in Acetonitrile/Water Mixtures Using Binuclear Iridium(III) Photosensitizers. | LitMetric
Two iridium(III) binuclear photosensitizers, [Ir(dFCFppy)(N-N)Ir(dFCFppy)], where N-N is tetrapyrido[3,2-:2',3'-:3″,2″-:2‴,3‴-]phenazine (Ir-TPPHZ) and 1,4,5,8-tetraazaphenanthrene[9,10-]-1,4,5,8,9,12-hexaazatriphenylene (Ir-TAPHAT) are reported for iodide, bromide, and chloride photooxidation in acetonitrile and acetonitrile/water mixtures using blue-light irradiation. Excited-state reduction potentials * of +2.02 and +2.09 V vs NHE were determined for Ir-TPPHZ and Ir-TAPHAT, respectively. Both photosensitizers' excited states were efficiently quenched by iodide, bromide, and chloride with quenching rate constants in the (3.5-9.2) × 10 and (0.0036-2.9) × 10 M s ranges in neat acetonitrile and acetonitrile/water mixtures, respectively. Nanosecond transient absorption spectroscopy provided unambiguous evidence of reductive excited-state electron transfer, with all halides in the solvent mixtures containing up to 50% water. Cage-escape yields were large (55-96%) in acetonitrile and dropped below 32% in 50:50 acetonitrile/water mixtures.
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