单原子催化剂M(Pt/ Pd)/MOF(金属有机框架化合物)的可控制备及催化机理研究

The ultimate in metal catalysts is that all the active metals are in the form of single-atom state and dispersed in the support materials, which is called as "single-atom catalysts". Because of the highly catalytic activity and atom economy, single-atom catalysts have become the new frontier and research hotspot in catalysis. In this project, metal-organic framework (MOF）will be applied as supporter, in which the suitable size of the cavity in MOF can act as "host" to hold the single-atom noble metals (M) and the coordination atoms in the MOF can further stabilize the implanted metal atoms. Finally, highly loaded and stable single-atom metal catalysts supported by MOF can be obtained after calcination in inert atmosphere. The local atomic/electronic structure and interactions between the supporter and the single-atom metals will be studied by techniques of X-ray absorption spectra (XAFS) and so on. With the combination of the first-principle calucidated, the mechanisms of the catalytic activity will be revealed. This study will provides examples and theoretical guidances for the cost-effective synthesis of the highly stable single-atom catalysts with high catalytic activity.

金属催化剂的极限是其所有的金属活性组分都以单原子的形式分散于载体中，称之为“单原子催化剂”。单原子催化剂由于具有高的催化活性和原子经济性，已经成为催化领域最新的前沿与研究热点。本项目拟采用金属有机框架（MOF）材料为载体，利用MOF腔体合适的大小做为“宿主（host）”容纳贵金属（M）单原子以及MOF上的配位原子（N等）对单原子进行固定。经过惰性气体下煅烧处理，最终合成出高负载量和稳定的M/MOF单原子催化剂。利用X射线吸收谱学（XAFS）等技术，研究M/MOF催化活性中心的局域原子/电子结构，揭示载体与单原子金属之间的相互作用机制，结合第一性原理理论计算，阐明催化活性机理。该项目的开展将为廉价、高效制备具有高效稳定性和高催化活性的单原子催化剂提供案例和理论指导。

金属催化剂最理想状态是金属中的每个原子都能够发挥催化作用，由此诞生的单原子催化剂，双原子催化剂，单原子和团簇混合多活性位点催化剂。这类催化剂由于具有高的催化活性和原子经济性，已经成为催化领域最新的前沿与研究热点。本项目拟采用碳氮化合物和MOF为载体，利用载体的“宿主（host）”或者载体上配位原子对金属原子进行容纳或者进行固定。经过惰性气体下煅烧处理，最终合成出高负载量和稳定的单原子催化剂，双原子催化剂，单原子与团簇混合多活性位点催化剂。利用X射线吸收谱学（XAFS）等技术，研究这类催化活性中心的局域原子/电子结构，揭示载体与金属之间的相互作用机制，结合第一性原理理论计算，阐明催化活性机理。该项目的开展将为廉价、高效制备具有高效稳定性和高催化活性的催化剂提供案例和理论指导。