Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Publication date: 11th May 2021
Dye-sensitized photoelectrochemical cell is one of the prospective systems for photocatalytic water splitting. Recently, a remarkable achievement has been made based on ruthenium molecular complexes as sensitizer and catalyst coadsorbed on titania [1]. The maximum incident photon to current efficiency (IPCE) has reached 25% and stable photocurrent of 1.7 mA/cm2 has been obtained [1]. We have recently studied the systems with popular sensitizer RuP and two types of ruthenium complexes with different pyridine rings and anchoring group [2,3]. In both cases we have observed a very fast quenching of the oxidized RuP by the catalyst, taking place with the time constant below 200 ps and the quantum yield close to 100%. The dynamics of this process was independent on the water-based electrolyte composition [2], excitation fluence and dimer formation of the catalyst [3].
The initial photocurrent recorded in water-based electrolyte is significantly (about two times) higher for the photoanodes sensitized with a mixture of RuP and the catalyst than the sum of the separate individual contributions of photoanodes with RuP and the catalyst. Due to the observed fast electron transfer process from the catalyst, RuP is quickly regenerated, allowing more frequent photon absorption and injection into titania, resulting in higher initial photocurrents. However, the photocurrent quickly decays into low stationary values (comparable to the sum of separated RuP and catalyst contributions), most likely due to the disappearance of the catalyst in the lowest oxidation state. So far, the interpretations of the initial photocurrent spike were based on fast interfacial charge recombination and/or slow catalytic turnover.
Our results reveal that ruthenium complexes-based chromophore-catalyst-assemblies on titania should serve as efficient systems for simple photocatalytic processes involving single electron transfer. For more complex mechanisms such as water splitting, its optimization requires finding solutions to accelerate the electron relay from higher valent catalyst species.
This study was supported by the NCN (National Science Centre, Poland), under project 2015/18/E/ST4/00196.
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