Tuning the (magneto)optical properties of supported plasmonic metal catalysts towards high performance and stability in photo(electro)catalytic water splitting

在阳光的帮助下，光（电）催化水分解过程产生氢和氧具有很高的潜力，有助于解决全球能源问题。目前已知的多相光催化体系缺乏对可见光的低利用率和活性不足。为了克服这些问题，本提案的主要任务是开发新型半导体/等离子体金属催化剂。潜在的表面等离子体共振效应是一个强大的工具，有可能同时实现这两个目标，即红移吸收边和活性位点数量的增加。进一步提高催化效率将实现额外的金属共催化剂的实施。在一个迭代的过程中，催化剂的开发将伴随着对实时电子转移过程的光诱导动力学的详细研究，以及通过最先进的原位光谱方法，包括超快瞬态技术，研究不同催化剂组分的作用。为了更好地理解化学过程，研究将首先集中在使用牺牲试剂的两个半反应上。值得注意的是，这些模型研究将通过在催化测试和光谱原位研究期间提供偏置电压来扩展。因此，一种基于半导体/等离子体金属催化剂的高效实用的水分解装置将被开发出来。

Photo(electro)catalytic water splitting processes to hydrogen and oxygen with the help of sunlight possess a high potential to contribute to solutions to the global energy problem. So far known heterogeneous photocatalytic systems lack inefficient utilization of visible light and insufficient activities. To overcome these problems the main task of this proposal is the development of novel semiconductor/plasmon metal catalysts. The underlying surface plasmon resonance effect is a powerful tool with the potential to achieve both, the red shifted absorption edge as well as the increase of number of active sites, simultaneously. Further improvement of the catalytic efficiency will be achieved by implementation of additional metal co-catalysts. In an iterative process the catalyst development will be accompanied by detailed investigations of the light-induced dynamics of electron transfer processes in real time as well as the role of different catalyst components by state-of-the-art spectroscopic in situ methods, including ultrafast transient techniques. For better understanding of the chemical processes investigations will focus initially onto the two half reactions applying sacrificial reagents. Notably, these model studies will be extended by supplying a bias voltage during catalytic tests and spectroscopic in situ studies. Thus, a more efficient and practical water splitting device based on semiconductor/plasmon metal catalysts will be developed.