吸光/催化位点协同调控CO2和HCs选择性转化的机理研究

化石能源燃烧排放的大量二氧化碳（CO2）是造成温室效应的重要原因。催化技术可将CO2与甲烷（CH4）重整转化为合成气，是最有前景的CO2资源化利用技术之一。然而，靠热能驱动的CO2和CH4催化重整对反应体系的温度要求较高，且会生成积炭和水等副产物。此外，在实际生产中CH4往往和多种HCs共存，在重整反应条件下HCs会发生催化裂解、脱氢氧化等副反应，影响产物选择性。为此，本项目提出通过等离激元增强CO2和HCs催化制备合成气的研究思路，从光能/热能吸收转化和界面反应结合入手，通过原位瞬态实验和理论计算研究，探明等离激元效应对催化反应的影响机制；揭示反应关键中间物种，阐明气固界面CO2和多种HCs的催化转化反应路径；通过吸光/催化位点优化，调控复杂物理场作用下的能量传递和物质转化过程，最终形成利用等离激元效应增强CO2和多种HCs高选择性催化转化的新方法。

The massive emission of carbon dioxide (CO2) from the combustion of fossil fuels is one of the important reasons causing greenhouse effects. Catalytic reforming technology for converting CO2 and methane (CH4) into syngas is one of the most promising technologies for the resource utilization of CO2. However, thermal driven reforming of CO2 and CH4 not only requires high system temperature but also produces by-products such as water and soot. Besides, a variety of HCs may coexist with CH4 in production practice, and side reactions such as oxidative cracking and dehydrogenation oxidation of HCs under reforming conditions will affect the product selectivity. Therefore, a plasmon-enhanced route is proposed in this study for catalytic conversion of CO2 and HCs to syngas. Starting from optical/thermal energy absorption and interface reaction and combining with in-situ transient experiments and theoretical calculation methods, to explore the influence mechanism of plasmon on catalytic reaction; to reveal the key intermediate species of reaction and clarify the catalytic conversion pathways of CO2 and multiple HCs at gas-solid interface; to regulate the energy transfer and substance conversion process under complex physical fields by controllable preparation of optical absorbing/catalytic sites and finally form a new methodology for plasmon-enhanced catalytic reforming preparation of syngas from CO2 and multiple HCs with high selectivity.