Materials Engineering of Efficient Solar Fuels

该研究项目的长期目标是设计出一种具有技术竞争力的地球资源丰富、成本低、阳光稳定且无毒的光催化剂材料，这种材料可以通过人工光合作用过程产生太阳能燃料，类似于植物和一些细菌利用阳光通过光合作用转化二氧化碳和水的方式。这种材料可以用来制造类似太阳能电池板的“人造叶子”，将阳光转化为可储存的碳氢化合物燃料，而不是电能。******该研究项目将专注于光热/光化学催化，并考虑材料性能的最佳组合，以实现二氧化碳和水的快速，选择性和高效的光转化为可储存和可运输的碳氢化合物燃料，如一氧化碳，甲烷或甲醇。气相光辅助减少二氧化碳是一种实用的选择，也是本研究的重点，因为气相工艺可以很容易地扩展并与现有的化学和石化工业基础设施集成。******尽管世界范围内进行了大量的研究工作，但为了实现工业应用，光热催化的机理细节仍有待澄清，以适用于不同类别的材料和载体。高分辨率环境扫描透射电子显微镜（ETEM）将定制用于纳米结构催化剂的显微镜/光谱。在原子分辨率下，将实现纳米结构光催化剂中限速局部结构和电子跃迁的新基本表征研究，用于样品的集中太阳照明以及在可变温度下的原位气体反应能力。这种类型的实验装置和方法在世界上是独一无二的，因此将实现对控制光催化作用机制的新见解。通过确定支持促进催化二氧化碳还原反应的光热效应的关键机制因素，将证明设计和合成纳米级催化剂是可能的，其成分和结构、化学和物理性质有助于最大限度地利用来自阳光的热和光将气态二氧化碳还原为增值化学品和燃料。******如果这种二氧化碳利用和增值的方法能够在工业上以显著的速度、效率和规模发展，并在经济上与化石化学品和燃料相竞争，那么未来设想的二氧化碳炼油厂将能够有助于减少温室气体排放，改善气候变化，提供能源安全和保护环境。

The long-term objective of the research program is to engineer a technologically competitive class of earth abundant, low cost, sunlight stable and non-toxic photocatalyst materials that can generate solar fuels using an artificial photosynthetic process akin to the way plants and some bacteria use sunlight to transform carbon dioxide and water through photosynthesis. Such materials can be used to engineer the 'artificial leaf' analogue of a solar panel that converts sunlight to storable hydrocarbon fuel as opposed to electricity.******This program of research will focus on photothermal/photochemical catalysis and consider the optimal combination of materials properties to enable fast, selective and efficient photo-transformation of carbon dioxide and water to storable and transportable hydrocarbon fuels such as carbon monoxide, methane or methanol. Gas-phase light-assisted reduction of carbon dioxide is a practical option and the focus of this research, since gas phase processes can be easily scaled and integrated with existing chemical and petrochemical industry infrastructure.******Despite a significant amount of research effort worldwide, the mechanistic details of photothermal catalysis remain to be clarified for different classes of materials and supports in order to achieve industrial relevance. A high-resolution environmental scanning transmission electron microscope (ETEM) will be customized for microscopy/spectroscopy of nanostructured catalysts. A custom light port for concentrated solar illumination of specimens coupled with the capability for in situ gas reaction at variable temperatures will be implemented for novel fundamental characterization studies of the rate-limiting localized structural and electronic transitions operative in nanostructured photocatalysts at atomic resolution. This type of experimental setup and approach is unique in the world and thus will realize novel insight into the operative mechanisms controlling photocatalysis. By identifying the key mechanistic factors which underpin the photothermal effect that promotes catalytic carbon dioxide reduction reactions, it will prove possible to design and synthesize nanoscale catalysts with compositions and structures, chemical and physical properties that serve to maximize the rate of reduction of gaseous carbon dioxide to value-added chemicals and fuels, using both the heat and light from sunlight. ******If this approach to utilization and valorization of carbon dioxide could be developed at industrially significant rates, efficiencies and scales and made economically competitive with fossil-based chemicals and fuels, then carbon dioxide refineries envisioned in the future would be able to contribute to the reduction of greenhouse gas emissions, ameliorate climate changes, provide energy security and enable protection of the environment.