原子级精细合成负载型贵金属小团簇催化剂的研究

项目名称： 原子级精细合成负载型贵金属小团簇催化剂的研究

项目编号： No.21473169

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 路军岭

作者单位： 中国科学技术大学

项目金额： 90万元

中文摘要： 负载型贵金属催化剂在许多工业反应中有着广泛的应用。人们通过浸渍和沉淀等方法，调控金属颗粒的尺寸、成分和结构，理解催化活性与这些微观结构的关系，进而设计出催化性能更佳的催化剂。然而，实现原子层面的精细可控合成，至今仍是一个巨大的科学挑战。本项目拟利用原子层沉积(ALD)的技术优势——原子级精确可控，尝试在原子层面精细合成以Pt、Pd 为代表的单金属和双金属小团簇（原子个数少于10）负载型催化剂。通过采用原子分辨球差矫正扫描透射电镜、X-射线光电子能谱和扩展X 射线吸收精细结构谱等技术，重点研究：（1）负载型Pt、Pd 单原子及单金属小团簇催化剂的精细可控合成； （2）负载型PtPd 双金属小团簇催化剂的原子级精细设计与调控；（3）金属小团簇所包含的原子数和成分与其催化活性的关系。深入探索ALD 技术在原子层面精细调控金属小团簇的原子数、成分和结构的可行性，为未来设计与合成新型高效催化剂提供新思路。

中文关键词： 金属催化剂；催化剂设计与合成；原子层沉积；多相催化；构效关系

英文摘要： Supported noble metal catalysts have been widely used in many industrial catalytic reactions. Tremendous effort has been dedicated to achieving the control over the metal nanoparticle size, composition and structure using several methods such as impregnation, and precipitation, in order to establish the structure and reactivity relationships, and thus to design and synthesize a catalyst with better performance. However, it remains a grand challenge to achieve the precise control on an atomic level. In this project, we will take advantage of the unique feature of atomic layer deposition (ALD), atomically-precise controlled deposition, to synthesize supported ultrafine Pt, Pd monometallic and bimetallic clusters on the atomic level, where all the metal clusters contain less than 10 atoms. By employing the advanced characterization techniques such as aberration-corrected scanning transmission electron microscopy, x-ray photoemission spectroscopy and extended x-ray absorption fine structures, we will study: (1) atomically-precise synthesis of supported Pt, Pd ultrafine monometallic cluster catalysts; (2) atomically-precise synthesis of supported PtPd ultrafine bimetallic cluster catalysts; (3) the relationships between the atomic number and composition of the ultrafine metal clusters and their activity. In brief, we will systematically explore the ultimate capability of ALD in atomically-precise control over the atomic number, composition and structure of the ultrafine monometallic/bimetallic clusters. The gained knowledge would guide us to designing new catalytic materials with high performance.

英文关键词： Metal Catalyst;Catalyst Design and Synthesis;Atomic Layer Deposition;Heterogeneous Catalysis;Structure-Reactivity Relationships