To the best of our knowledge, according to the TOF and TON values, the designed PS system is one of the most efficient and robust photocatalytic H 2 generation systems adopting a TiO 2-anchoring molecular PS in the literature. Distinctive and prolonged hydrogen evolution performances of these PSs under visible-light irradiation from water in their platinized TiO 2 composites were demonstrated: a turnover number (TON) of up to 24 900 (252 h) with 1560 μmol (37.6 mL) hydrogen produced, an initial turnover frequency (TOF i) of 1130 h –1, initial activity (Activity i) of 705 mmol g –1 h –1, and initial apparent quantum yield (AQY i) of 12.1%. Their photophysical and electrochemical properties, together with their photocatalytic hydrogen evolution performance as photosensitizers (PSs), were investigated. Six donor–donor−π–acceptor (D–D−π–A) triphenylamine-based starburst organic dyes with different electron-donating moieties and thiophene-based π-linkers were synthesized and characterized.
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