Department of Chemistry, Yale University, New Haven, CT, 06520, USA.
Yale Energy Sciences Institute, Yale University, West Haven, CT, 06516, USA.
ChemSusChem. 2017 Nov 23;10(22):4526-4534. doi: 10.1002/cssc.201701693. Epub 2017 Oct 23.
The development of water-splitting dye-sensitized photoelectrochemical cells has gained interest owing to their ability to generate renewable fuels from solar energy. In this study, photoanodes were assembled from a SnO film sensitized with a combination of a high-potential CF -substituted porphyrin dye with a tetrahydropyranyl-protected hydroxamic acid surface-anchoring group and a CpIr (Cp=pentamethylcyclopentadienyl) water-oxidation catalyst containing a silatrane anchoring group. The dye/catalyst ratios were varied from 2:1 to 32:1 to optimize the photocatalytic water oxidation. Photoelectrochemical measurements showed not only more stable and reproducible photocurrents for lower dye/catalyst ratios but also improved photostability. O production was confirmed in real time over a 20 h period with a Clark electrode. Photoanodes prepared from 2:1 and 8:1 dye/catalyst sensitization solutions provided the most active electrodes for photocatalytic water oxidation and performed approximately 30-35 turnovers in 20 h.
由于水分解染料敏化光电化学电池能够将太阳能转化为可再生燃料，因此引起了人们的兴趣。在这项研究中，采用高电位 CF 取代卟啉染料与四氢吡喃保护的羟肟酸表面锚定基团组合对 SnO 薄膜进行敏化，组装了光阳极，并用含有硅氮烷锚定基团的 CpIr（Cp=五甲基环戊二烯基）水氧化催化剂对其进行了修饰。改变染料/催化剂的比例从 2:1 到 32:1，以优化光催化水氧化过程。光电化学测量结果表明，较低的染料/催化剂比例不仅具有更稳定和可重复的光电流，而且具有更好的光稳定性。通过克拉克电极实时确认了在 20 小时内的 O2 产生情况。由 2:1 和 8:1 染料/催化剂敏化溶液制备的光阳极为光催化水氧化提供了最活跃的电极，在 20 小时内进行了约 30-35 次循环。
