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

光化学燃烧逆转的模拟研究：利用H2O氢化CO2

• 批准号: 46508-2013
• 负责人: Gambarotta, Sandro
• 金额: $ 6.12万
• 依托单位: University of Ottawa
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2017
• 资助国家: 加拿大
• 起止时间: 2017-01-01 至 2018-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=632716
• 关键词: Modeling; studies; photochemical; combustion; reversal

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.

任何燃料或任何有机物质的燃烧都会从大气中吸收氧气并产生二氧化碳和水。利用光化学输入可以恢复这一过程。换句话说，在适当的催化剂的存在下，CO2和H2O的照射能够释放氧气并重组有机材料，而有机材料又可以用作标准发动机或燃料电池的燃料。实现这种显著转变的可能性仅局限于微观尺度和极少数选择性系统。最近的文献表明，至少有可能将选择性提高到理想水平。然而不幸的是，到目前为止，这些引人注目的过程的活动和规模还没有超过实验室的规模。我们提出了一种机制/建模研究，旨在理解现有系统之一。我们特别选择了基于BiVO4的光系统，因为它不需要任何电化学输入来生产乙醇。本项目分为三个子项目，分别是：1 .分析和改进现有催化体系，引入改性，提高催化剂性能；2：对催化剂活性位点进行建模研究，了解CO2的还原是如何随着O2的演化而发生的。这项工作有望产生的数据可能是未来催化剂设计和修改的进一步灵感的基础；3：分析CO2催化生成C-C键的因素。这将通过制备与光半导体BiVO4相关的分子系统来实现。再一次的理解，期望产生宝贵的信息，指导未来的研究，旨在发现更高效的催化体系。