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Enhancement of dye regeneration kinetics in dichromophoric porphyrin-carbazole triphenylamine dyes influenced by more exposed radical cation orbitals

机译:受更多暴露的自由基阳离子轨道影响的双色卟啉-咔唑三苯胺染料的染料再生动力学增强

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摘要

Reduction kinetics of oxidized dyes absorbed on semiconductor surfaces and immersed in redox active electrolytes has been mainly modeled based on the free energy difference between the oxidation potential of the dye and the redox potential of the electrolyte. Only a few mechanisms have been demonstrated to enhance the kinetics by other means. In this work, the rate constant of the reduction of oxidized porphyrin dye is enhanced by attaching non-conjugated carbazole triphenylamine moiety using iodine/triiodide and tris(2,2′-bispyridinium)cobalt II/III electrolytes. These results are obtained using transient absorption spectroscopy by selectively probing the regeneration kinetics at the porphyrin radical cation and the carbazole triphenylamine radical cation absorption wavelengths. The enhancement in the reduction kinetics is not attributed to changes in the driving force, but to the more exposed dye cation radical orbitals of the dichromophoric dye. The results are important for the development of high efficiency photo-electrochemical devices with minimalized energy loss at electron transfer interfaces.
机译:主要基于染料的氧化电势与电解质的氧化还原电势之间的自由能差,对吸附在半导体表面并浸入氧化还原活性电解质中的氧化染料的还原动力学进行了建模。已证明只有少数机制可以通过其他方式增强动力学。在这项工作中,通过使用碘/三碘化物和三(2,2'-双吡啶鎓)钴II / III电解质连接非共轭咔唑三苯胺部分,可以提高氧化卟啉染料的还原速率常数。这些结果是使用瞬态吸收光谱法通过选择性地探测卟啉自由基阳离子和咔唑三苯胺自由基阳离子吸收波长处的再生动力学而获得的。还原动力学的增强不是归因于驱动力的变化,而是归因于双发色染料的更暴露的染料阳离子自由基轨道。这些结果对于开发在电子传输界面处具有最小能量损失的高效光电化学装置至关重要。

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