This work elaborates the effect of dynamic irradiation on light-driven molecular water oxidation to counteract deactivation. It highlights the importance of overall reaction engineering to overcome limiting factors in artificial photosynthesis reactions. Systematic investigation of a homogeneous three-component ruthenium-based water oxidation system revealed significant potential to enhance the overall catalytic efficiency by synchronizing the timescales of photoreaction and mass transport in a capillary flow reactor.
View Article and Find Full Text PDFThe synthesis of a new Ru-based water oxidation catalyst is presented, in which a nitrophenyl group is introduced into the backbone of dpp via a pH-sensitive imidazole bridge (dpp = 2,9-di-(2'-pyridyl)-1,10-phenanthroline). This modification had a pronounced effect on the photophysical properties and led to the appearance of a significant absorption band around 441 nm in the UV-vis spectrum upon formation of the monoprotonated species under neutral conditions. Theoretical investigations could show that the main contributions to this band arise from transitions involving the imidazole and nitrophenyl motif, allowing us to determine the p value (6.
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