N、S掺杂纳米碳负载贵金属催化剂的可控制备及界面电子特性与催化性能调控

The reactions of alcohol selective oxidation and aromatic nitro-compound hydrogenation are significant in fine chemicals. The research is based on such reactions to develop novel doping (N, S, etc.) carbon supporting highly dispersed noble metals (Pt, Pd, etc.). Taking advantage of surface structure and electronic properties of specific sites on doped carbon, together with varying metal loading process, can realize the precise control of noble metal interfacial structure and electronic property at the atomic level, improving the utilization, stability and catalytic performance of noble metal catalyst, and realizing the selective application. In catalytic science, some concerns will be focused on: i) the nature of the bonding interaction (metal valence and the coordination environment) between noble metal and specific site on doped carbon; ii) the intrinsic mechanism between metal surface interfacial structure and its catalytic function; iii) the structure-activity relationship in selective oxidation and hydrogenation reactions. Based on the study, knowledge of the surface and interface catalysis will be promoted at the molecular level. According to the target reaction mechanism and structure-activity relationship, the metal surface interfacial structure and electronic property, which are advantageous to the target catalytic reaction, will be strengthened to realize the highly active and selective in target catalytic process. More scientific basis and theoretical guidance would be proposed for the high efficiency and environment-friendly noble metal catalyst design, preparation and selective application.

以精细化学品中具有重要地位的醇选择性氧化与芳香硝基化合物加氢等为模型反应，发展基于新型掺杂（N、S等）纳米碳负载的高分散贵金属（Pt、Pd等）催化剂。利用掺杂碳表面位点结构与电子特性，结合负载工艺，在原子层面上精准控制贵金属位点的界面结构与表面电子特性，提高贵金属的利用率、稳定性和催化性能，并实现贵金属催化剂的选择性应用。在催化科学方面，本项目将在分子层面上揭示高分散贵金属位点与掺杂碳上特定位点键合形式（金属价态与配位环境）的本质属性及其与催化功能的内在机制，构建结构与性能的“构效关系”，提出有利于氧化、加氢反应的表界面结构与电子特性，推进分子层次上表界面催化本质的认识。在氧化、加氢反应机理和“构效关系”的基础上，进一步强化有利于目标反应的催化剂表界面结构与电子特性，实现催化反应过程中的高活性与高选择性。为高效、环保的贵金属催化剂设计与选择性应用提供更多的科学依据与理论指导。

该项目以甘油选择性氧化为主要模型反应，基于金属与金属、金属与掺杂（N、S等）碳载体之间的相互作用，有效调控了掺杂碳负载的贵金属催化剂的几何和电子结构，并强化催化过程和性能。研究工作揭示了掺杂碳载体的组成、结构及催化剂的制备工艺对负载的活性位点Pt的表面结构、电子特性的影响，建立了掺杂碳载体与金属Pt间的“构效关系”，实现在原子层面上控制贵金属活性位点。在此基础上，深入分析Pt基催化剂结构对其催化性能的影响，构建了Pt基催化剂结构与其催化性能的“构效关系”。在反应机理和“构效关系”的基础上，强化有利于目标反应的催化剂表界面结构与电子特性，实现催化过程中的高活性与高选择性。为高效、环保的贵金属催化剂设计与选择性应用提供更多的科学依据与理论指导。