Modeling studies on photochemical combustion reversal: using H2O to hydrogenate CO2

任何燃料或任何有机材料的燃烧都会从大气中吸收氧气，并产生二氧化碳和水。可以通过使用光化学输入来恢复该过程。换句话说，在适当的催化剂存在下，CO2和H2O的照射能够释放氧气气体并重整有机材料，这些有机材料反过来可以用作标准发动机或燃料电池的燃料。实现如此显著的转变的可能性仅限于微型和极少数有选择的系统。最近的文献表明，至少有可能将选择性提高到理想的水平。然而，不幸的是，到目前为止，这种非凡过程的活动和规模还没有超过实验室的规模。我们提出了一种机械/建模研究，旨在了解现有系统之一。特别是，我们选择了基于BiVO4的光系统，因为它不需要任何电化学输入来生产乙醇。该项目分为三个分项目，分别针对： 1：分析和改进现有催化系统，引入改进措施，以提高催化剂性能； 2：对催化剂活性中心进行模拟研究，以了解二氧化碳还原是如何随着O2的释放而发生的。这项工作有望产生数据，这些数据可能是关于未来催化剂设计和修改的进一步启发的基础； 3.分析了二氧化碳催化生成C-C键的因素。这将通过制备与光半导体BiVO4相关的分子体系来实现。再一次，了解将产生宝贵的信息，以指导未来的研究，旨在发现更有效的催化体系。

Combustion of any fuel, or of any organic material, uptakes oxygen from the atmosphere and generates CO2 and H2O. It is possible to revert the process by using a photochemical input. In other words, the irradiation of CO2 and H2O and in the presence of an appropriate catalyst is capable of releasing oxygen gas and reforming organic material, which in turn can be used as a fuel for standard engines or fuel cells. The possibility of performing such a remarkable transformation is solely limited to micro-scale and a very few selective systems. Recent literature claims indicated that it is at least possible to improve the selectivity to ideal level. Unfortunately though, the activity and scale of such remarkable processes so far do not exceed the lab scale. We propose a mechanistic/modeling study aiming at understanding one of the existing systems. In particular we have selected the photosystem based on BiVO4 due to the fact that it does not require any electrochemical input for the production of ethanol. The project is organized in three sub-projects aiming respectively at: 1: analyzing and improving the existing catalytic systems to introduce modifications for catalyst performance improvements; 2: modeling studies on the catalyst active site to understand how the CO2 reduction occurs along with the O2 evolutions. This work is expected to produce data that may be the foundation for further inspiration about future catalyst design and modification; 3: analyzing the factors catalytically generating C-C bond from CO2. This will be carried out by preparing molecular systems related to the photosemiconducting BiVO4. Once again understanding is expected to generate precious information for guiding future research aiming at the discovery of more performing catalytic systems.