Journal
INORGANIC CHEMISTRY
Volume 48, Issue 22, Pages 10498-10506Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ic9007763
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- NSF CAREER [CHE-0449755]
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A photocatalytic water-reducing system utilizing a bis-cyclometalated bipyridyl iridium(III) photosensitizer (PS) and a platinum or palladium heterogeneous catalyst was used to identify systematic property-activity correlations among a library of structural derivatives of [lr(ppr)(2)(bpy)](+). A heterogeneous Pd catalyst proved to be more durable than its previously reported Pt-based counterpart, allowing for more reliable photosensitizer study. The deliberate steric and electronic variations of the ppy and bpy moieties resulted in a dramatic decrease of the degradation rates observed with selected photosensitizers when compared to the more substitution-labile [lr(ppy)(2)(bpy)](+) parent compound. An improved photosensitizer structure with a Pd catalyst in a nonligating solvent exhibited a 150-fold increase in catalyst turnover numbers compared to the system using [lr(ppy)(2)(bpy)](+) and a Pt catalyst. Furthermore, photocatalytic and photophysical studies at varied temperatures provided information on the rate-limiting step of the photocatalytic process, which is shown to be dependent on both the PS and the Pt or Pd catalytic species.
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