新型取向碳纳米管/金属酞菁复合电催化体系的构建及其电催化性能研究

Due to the novel properties and unique structures,such as high conductivity, convenient regulation of structures, and superhigh surface area, aligned carbon nanotubes (ACNTs) exhibit promising applications in the field of electrocatalysis. However, how to further improve the electrocatalysis activities is still a big challenge to the research community. One key is to supporting appropriate catalyst on ACNTs to develop composite electrodes. Metallophthalocyanines (MPcs) have been intensively studied as one family of catalysts with high catalytic activities for various reactions. They can be functionalized with different groups and coordinated with different metal atom, which will enable MPcs with different catalytic activities and selectivities. ACNTs electrode surface modifications with MPcs can enhance electron transfer reactions, which will facilitate the coordination electrocatalysis activities of ACNTs and MPcs and largely improve the electrocatalysis activities of ACNT. This research plan developed a series of methods for the preparation of ACNTs with different structures, and MPcs with various substituents on the conjugated ring and different metal atom in the center of the ring. Several routes were also designed for the composite of ACNTs and MPcs. All the influence factor on the electrocatalysis activities of the composite electrode will be carefully studied. The influence factor include the structure of ACNT, the molecule structure of MPcs, and the composite structure between ACNT and MPcs. Electrocatalysis degradation of organic pollutants and electrocatalysis of oxygen reduction will be chose as models for the electrocatalysis study of the ACNTs/MPcs composite electrodes. The mechanisim of these electrocatalysis reaction will be carefully studied, which will be of great value for the development of materials with high electrocatalysis activities.

取向碳纳米管具有良好的导电性和结构可调控性，在电催化领域显示出良好的应用前景。目前限制其应用的瓶颈是其电催化性能还有待进一步提高。金属酞菁是一种广泛研究的高活性催化剂，其共轭环上的取代基和中心金属原子的可设计性为金属酞菁电催化活性的开发提供了广阔的空间。构建取向碳纳米管/金属酞菁复合电催化体系，充分发挥取向碳纳米管与金属酞菁的协同电催化作用，对于高电催化活性电极的开发具有重要意义。项目设计制备不同结构的取向碳纳米管，合成不同取代基和金属原子的金属酞菁，采用不同的复合方法，发展一系列具有高电催化活性的取向碳纳米管/金属酞菁复合电极。重点以有机污染物的电催化降解和氧气的电催化还原为模型，通过系统研究，探索取向碳纳米管结构、金属酞菁的分子结构、取向碳纳米管与金属酞菁的复合结构等多层次结构对复合电极电催化性能的影响规律，阐明协同电催化和选择性电催化机理，为高电催化活性材料的开发提供理论基础。

随着人们越来越关注生态环境以及个人健康，对环境或食品中的有害物质进行快速有效检测和降解成为目前研究的重点。本项目通过电化学法，将具有高催化活性的金属酞菁成功负载到具有高导电性和稳定性的取向碳纳米管阵列和纤维上，构建了两种高结构稳定性的复合电催化体系，包括取向碳纳米管阵列/四氨基钴酞菁和取向碳纳米管纤维/四硝基铁酞菁。并以常见的工业污染物和食品添加剂——亚硝酸盐为目标物，考查了该复合电催化体系对目标物的电催化活性，结果显示该复合电催化体系具有良好的电催化活性和选择性，对目标物的浓度检测显示出良好的灵敏度、较高的检测下限和极好的抗干扰能力，初步证明该取向碳纳米管/金属酞菁复合电催化体系在污染物的快速电催化检测和传感器的制备方面具有良好的应用前景。同时对取向碳纳米管/金属酞菁复合电催化体系的电催化机理进行了深入研究，初步揭示了取向碳纳米管的结构、金属酞菁的结构和取向碳纳米管与金属酞菁的组成比等因素对协同电催化作用的影响规律，探讨了污染物的电催化降解机理，对高性能电催化体系的开发提供了理论参考价值。