基于金属酞菁功能化石墨烯复合材料载体的燃料电池阳极电催化剂构筑，性能及催化作用机理研究

本项目首次以金属酞菁功能化石墨烯复合材料为载体，建立新型高性能功能化石墨烯载Pt基（如Pt、PtRu等）燃料电池阳极催化剂的构筑方法。系统研究铜酞菁、铁酞菁、钴酞菁、镍酞菁、锰酞菁和铅酞菁等6种金属酞菁分子构筑的功能化石墨烯载Pt基催化剂对甲醇氧化的电催化性能，定量阐明金属酞菁化合物中金属元素的种类和酞菁分子的结构对催化剂性能的影响。尝试对负载Pt基纳米颗粒的表面结构进行可控合成，研究纳米晶催化剂的生长机制，揭示所合成催化剂的表面结构（包括表面化学组成与几何原子排列结构）与反应性能间的内在联系和规律。采用密度泛函理论（DFT）计算方法探索金属酞菁功能化石墨烯载Pt基催化剂的催化作用本质及相关电催化氧化反应机理。该课题研究对于在微观层次上发展电催化理论以及设计和构筑高性能的石墨烯基燃料电池催化剂具有重要的理论和实践意义。

With metal phthalocyanine functionalized graphene composite as the support, for the first time, this project put emphasis upon the fabrication methods of novel functionalized graphene supported Pt-based (e.g., Pt, PtRu) fuel cell anode catalysts with high performance. The electrocatalytic properties of functionalized graphene supported Pt-based catalysts fabricated by using six metal phthalocyanine molecules such as copper phthalocyanine, iron phthalocyanine, cobalt phthalocyanine, nickel phthalocyanine, manganese phthalocyanine and lead phthalocyanine for methanol oxidation are studied systematically, the effect of metal element kind in metal phthalocyanine compounds and structure of phthalocyanine molecules on the catalytic performance is analyzed quantitatively. Controlled-synthesis of the surface structure of supported Pt-based nanoparticles is carried out, the growth mechanism of nanocrystal catalysts is investigated, the intrinsic relationship between surface structure (including the chemical compositions and atomic arrangement on surface) of as-synthesized catalysts and their properties will be revealed. Density functional theory (DFT) calculation is used to investigate the catalytic essence of metal phthalocyanine functionalized graphene supported Pt-based catalysts and the mechanism of electrocatalytic oxidation reactions. This study is of significance for the development of electrocatalysis theory at a microscopic level, as well as in the design and construction of graphene-based fuel cell catalysts with high performance.