薄壁纳米碳管杂原子可控掺杂及官能团催化作用研究

Carbon nanomaterials, e.g. fullerene, carbon nanotube and graphene, are one of the hottest topics inside the research field of nanoscience. Doping with oxygen, nitrogen, boron and other heteroatoms can efficiently improve the surface reactivity of graphitic domains. The doped carbon materials have wide applications in the fields of catalysis, environmental protection, energy storage, drug delivery, etc.. It is necessary to investigate the doping mechanism of heteroatoms and controllable doping methods, and this will promote the applications of doped carbon nanomaterials. This project will focus on the doped thin-walled carbon naotubes materials, analyze the distribution of doped speices by using synchrontron-excited and spectroscopic technologies, understand the mechanistic and kinetic features of heteroatoms (e.g. oxygen, nitrogen, boron) doping graphitic structure, and explore some structurally controllable, economical and applicable doping methods. The catalytic performance of doped carbon nanotubes and its composited materials will be explored in selective oxidation reactions. The research of doping chemistry mainly includes the structure identification, doping mechanism and structure-performance relationship, which will provide the solid theoretical support for the batch applications of carbon nanotubes in the field of industrial catalysis.

以纳米碳管为代表的纳米碳材料是国际纳米科学领域研究的热点之一。氧、氮、硼等杂原子在石墨结构中掺杂后可显著提高其表面活性，掺杂材料在催化、环保、储能、药物输送等领域有着广泛的应用前景，解析杂原子渗入机制、探索可控掺杂方法对纳米碳材料应用研究将起到关键作用。本项目以薄壁纳米碳管掺杂材料为主要研究对象，采用同步辐射与光谱表征技术分析掺杂物种分布，掌握氧、氮、硼等原子掺入石墨结构机制与动力学特征，开发结构可控、经济实用的掺杂新技术，探索纳米碳管掺杂材料及其金属复合材料在选择氧化反应中的催化性能。本项目将着重从"结构解析、掺杂机理、构效关系"三个方面开展纳米碳管掺杂研究，为纳米碳管复合材料在工业催化领域的规模化应用提供理论支撑。

纳米碳催化的重点是对碳催化剂进行可控掺杂并研究掺杂物种在催化反应中的作用机理。氧、氮、硼等杂原子掺入石墨结构中后可显著提高其催化活性，并改变反应微观机理。本项目以氮、氧两类杂原子掺杂的薄壁纳米碳管为主要研究对象，通过可控制备、结构解析、构效关系三个步骤研究了掺杂物种分布、掺杂机制和催化作用机理，主要发现了掺入碳材料结构中的石墨氮物种在丙烷氧化脱氢制丙烯、丙烯醇和丙烯醛选择氧化中起到关键作用，而碳管表面的羧酸基团是生物质果糖氧化脱水和电化学氧还原反应的活性位点。这两项主要的创新研究成果是本项目目前最重要的发现之一，将会对碳催化领域的研究起到积极的推动作用。