Materials Engineering of Efficient Solar Fuels

该研究计划的长期目标是设计一种具有技术竞争力的地球丰富，低成本，阳光稳定和无毒的光催化剂材料，可以使用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使用阳光通过光合作用转化二氧化碳和水的方式。这种材料可用于设计太阳能电池板的“人造叶子”模拟物，将阳光转化为可储存的碳氢化合物燃料，而不是电力。该研究计划将侧重于光热/光化学催化，并考虑材料性能的最佳组合，使二氧化碳和水能够快速，选择性和有效地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。气相光辅助还原二氧化碳是一种实用的选择，也是本研究的重点，因为气相过程可以很容易地与现有的化学和石化工业基础设施进行规模化和集成，尽管在全球范围内进行了大量的研究工作，光热催化的机理细节仍然需要澄清不同类别的材料和支持，以实现工业相关性。高分辨率环境扫描透射电子显微镜（ETEM）将被定制用于纳米结构催化剂的显微镜/光谱学。一个定制的光端口，用于集中的太阳能照明的标本加上在可变温度下的原位气体反应的能力，将实施新的基本表征研究的速率限制本地化的结构和电子转换操作在纳米结构的光催化剂在原子分辨率。这种类型的实验装置和方法在世界上是独一无二的，因此将实现对控制细胞凋亡的操作机制的新见解。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，将证明有可能设计和合成具有组成和结构、化学和物理性质的纳米级催化剂，这些催化剂用于最大限度地将气态二氧化碳还原为增值化学品和燃料，使用来自太阳光的热和光。如果这种利用和稳定二氧化碳的方法能够以工业上显著的速度、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，提供能源安全并保护环境。

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.