School of Chemistry, Newcastle University, Newcastle upon Tyne, NE1 7RU, UK.
Chem Soc Rev. 2017 Oct 16;46(20):6194-6209. doi: 10.1039/c7cs00322f.
The arguments for converting sunlight and HO to H to provide cleaner fuels and chemicals are very powerful. However, there is still no efficient means of direct solar energy conversion to H on a large scale despite a large research effort worldwide. This review describes strategies to develop robust devices which exploit the selectivity of a molecular catalyst but avoids the use of sacrificial electron donors by adsorbing them onto an electrode surface. By assembling the photocathodes with photoanodes, the electrons provided by water oxidation are used to reduce H to H. By separating the functions of light absorption, charge transport and catalysis between the colloidal semiconductor and molecular components, the activity of each can be optimised. However, the complexity of the system requires advanced experimental techniques to evaluate the performance. Current understanding of the factors governing electron transfer across the interface between the semiconductor, dye and catalyst is described and future directions and challenges for this field are outlined.
将阳光和水转化为氢气以提供更清洁的燃料和化学品的观点非常有力。然而，尽管全球范围内进行了大量研究，但仍没有高效的大规模直接太阳能转化为氢气的方法。本综述描述了开发稳健器件的策略，这些器件利用分子催化剂的选择性，但通过将电子供体吸附到电极表面上来避免使用牺牲性电子供体。通过将光电阴极与光阴极组装在一起，可以利用水氧化提供的电子将氢气还原为氢气。通过在胶体半导体和分子组件之间分离光吸收、电荷传输和催化的功能，可以优化每个组件的活性。然而，系统的复杂性要求先进的实验技术来评估性能。描述了目前对半导体、染料和催化剂之间界面电子转移的因素的理解，并概述了该领域的未来方向和挑战。
