钯基纳米晶体的表面结构控制及其对催化氢转移反应的性能调控研究

Designing new catalysts or catalytic systems will provide a novel approach to achieve green chemistry and address environmental and energy issues. Utilizing other hydrogen sources instead of hydrogen gas in hydrogenation reactions will play a vital role in the future energy and environmental fields. In this project, we propose to precisely control the surface structures of catalysts as well as take advantage of the high catalytic activities of palladium-based nanomaterials in hydrogenation reactions, towards transfer hydrogenation reactions. We will employ inorganic controlled synthetic methods to obtain single-faceted palladium-based nanocrystals. Leveraging these ideal model systems, we will investigate the effects of surface structures (including atomic arrangements and compositions) on catalytic activity and selectivity, in efforts to establish the structure-property relationship between catalyst surface structures and catalytic activities. It will provide fundamentals for the design of palladium-based nanomaterials towards transfer hydrogenation reactions.

新型高效催化剂及催化反应体系的设计与构建，将为实现绿色化学、缓解日益严重的环境和能源问题提供一种新的方法和途径。利用非氢气的氢供体来进行加氢反应，即氢转移反应，在未来的催化领域中将起到重要作用。在本项目中，我们提出通过催化剂表面结构的精细构筑，并有效地结合钯基催化剂对于加氢反应高催化活性的优势，用于氢转移反应高效催化剂的设计。我们将利用无机可控合成方法，精准控制催化剂的表面精细结构，构建具有单一表面晶面的一元或二元的钯基金属纳米催化剂。基于该理想材料模型，我们将进一步结合同步辐射表征技术，探究其表面结构包括原子排列方式和组分对催化活性及选择性的具体影响，从而系统地建立催化剂表面结构与催化活性的构效关系，为针对氢转移反应的催化剂设计提供理论基础。

日趋严重的能源压力在新型高效催化体系的设计与构建领域提出了新的要求。其中利用非氢气的氢供体来进行加氢反应，即氢转移反应，具有极大的潜力。由于钯纳米晶体对于催化甲酸产氢和有机物加氢反应都具有良好的催化活性，可以作为以甲酸为氢供体的氢转移反应的催化剂。我们可控合成了具有特定晶面、特定原子组分、排列方式的钯基纳米晶体作为反应模型催化剂，确定了甲酸分解和有机物加氢反应的催化活性位点位置，为针对氢转移反应的催化剂设计提供理论基础。