小分子直接合成石墨烯基复合纳米催化剂

Among the novel applications of carbon-based materials (especially graphene-based materials)in the realm of catalysis,the mass production, the control in the doping level and distribution of the heteroatoms, keeping their high surface area,and tuning the meso-structure of graphene in nanoscale are the main hurdles that limited their real applications. In this application-oriented project, we aim to optimize the catalytic performance of graphene-based materials in conventional catalytic reactions, fuel cells and also other energy-storage devices by controlling the synthetic process and thus the composition and structure of the graphene-based materials. We will try to develope a series of synthetic approaches for thermalcondensation of small molecules into graphene based nanomaterials (including modified graphenes and graphene-based nanocomposites) in large quantities. Moreover, we plan to study the relationship between the structure and catalytic activity of graphene-based materials by controlling their composition and structure in atomatic level and monitoring the change in structure and property.This project could supply some useful information on the effect of dopants, coupling components and meso-nanostructure on the catalytic performace of these graphene-based catalysts,which are important for rational design of efficient graphene-based catalysts with novel functions.

在以碳材料特别是石墨烯材料为催化剂的诸多新型应用领域中，石墨烯材料的宏量制备、杂原子掺杂程度与分布的控制、比表面积的保持以及纳米结构的调控依然是限制其实际应用和性能改进的主要因素。本项目以催化应用为导向，通过控制合成条件来调控石墨烯基催化材料的组成、结构以及与其他材料的复合，进而实现催化性能的优化。同时，探索从小分子有机原料直接宏量合成石墨烯基催化剂的方法，以解决制约相关催化剂工业应用的瓶颈问题。本项目有助于探索从原子分子水平对石墨烯材料进行结构调整的方法，找到结构和组成与催化性能的正相关性，提高催化转化效率，完善石墨烯基催化材料的催化反应体系特别是绿色催化反应体系，以实现功能导向的石墨烯催化剂的设计合成。

近年来，以石墨烯结构为基础的碳基纳米材料以其高热稳定性，大比表面积和丰富活性位点等结构特征，在催化领域展露出良好的发展趋势。为解决制约石墨烯基相关催化剂工业应用中大批量制备困难，活性低等瓶颈问题，一方面我们利用廉价小分子的热聚合反应，设计合成了一系列石墨烯结构碳基复合纳米材料，围绕材料的宏观制备，结构组成，以及电子结构与催化性能之间的相互关系进行了深入研究。另一方面通过半导体-金属界面上的Mott-Schottky效应构筑了高度耦合的金属/半导体界面，调节金属粒子的电荷密度，从而达到提高催化反应活性的目的。经过研究表明，石墨烯结构和类石墨烯结构碳基复合材料在电催化氧气还原，电催化和生物质产氢，以及液相氧化，氢化等绿色有机催化反应中表现出优异的催化活性和循环稳定性，这归结于催化剂合理的纳米化设计和复合组分与载体间Mott-Schottky电子诱导效应对于材料催化活性的增强作用。新型的绿色可持续催化反应体系要求反应底物环保，反应过程低能耗，零排放并且无添加剂和副产物，应用Mott-Schottky载体效应概念合成设计的类石墨烯结构碳基复合材料将有望实现这一目标。