含氮多孔炭材料及负载型贵金属催化剂的制备和性能研究

发布时间：2018-03-21 04:31

本文选题：含氮炭材料　切入点：多级孔结构　出处：《南京大学》2017年博士论文　论文类型：学位论文

【摘要】：炭材料由于其来源广泛,成本低廉,比表面积大,稳定性好,无毒,孔道丰富等特点,在吸附、分离等领域引起了人们广泛的关注。为了进一步提高材料的性能,在炭骨架中引入氮基团,不仅可以提供碱性位点,缺陷活性位增加,而且亲水性和导电性增强,极大扩展了其在能源存储、电催化和催化剂载体等方面的应用。此外,得益于多级孔结构带来的质量传递性能的改进,在含氮炭材料中构造多级孔结构也受到了极大的关注。因此开发设计简单有效的方法合成同时具有高含氮量、高比表面积和多级孔结构的炭材料对于材料的应用具有重大的意义。本论文围绕含氮多孔炭材料的设计合成,将其应用于储能领域和催化剂载体方面,并且开发了一种简单制备高度分散负载型贵金属催化剂的方法。主要研究工作如下:(1)发展了一种简单的初湿浸渍法,以轻质氧化镁为模板,富含氮的对苯二胺和吡啶二醛为前体,制备了一种高含氮量(10 wt.%)高比表面积(904 m2/g)多级孔炭材料。此材料具有优异的超级电容器(419F/g@0.5A/g)和锂离子电池(2722mAh/g@0.1A/g)容量,且具有良好的倍率性能和循环稳定性。(2)以含氮多孔炭材料(CN)为载体,制备了双金属Pd10Au/CN催化剂。相比于纯炭作为载体和负载单金属Pd,PdioAu/CN具有更高的稳定性和活性;合金效应是苯酚加氢活性提高的原因。(3)发展了一种固相分散法,制备了高度分散Pd/HAP催化剂。对比传统浸渍法制备样品,Pd的颗粒粒径减小(1.2nm);活性Pd0含量的增多是加氢活性显著提高的可能原因。
[Abstract]:Because of its wide source, low cost, large specific surface area, good stability, non-toxic and rich pore channels, carbon materials have attracted wide attention in the fields of adsorption, separation and so on. The introduction of nitrogen groups into the carbon skeleton can not only provide basic sites, increase the active sites of defects, but also enhance hydrophilicity and conductivity, greatly expanding their applications in energy storage, electrocatalysis and catalyst carriers. Due to the improvement of mass transfer performance brought about by multistage pore structure, the construction of multistage pore structure in nitrogen-containing carbon materials has attracted much attention. Therefore, a simple and effective method for synthesis with high nitrogen content has been developed and designed. Carbon materials with high specific surface area and multilevel pore structure have great significance for the application of materials. In this paper, the design and synthesis of nitrogen-containing porous carbon materials are applied in the field of energy storage and catalyst support. A simple method for preparing highly dispersed supported noble metal catalysts was developed. The main research work is as follows: 1) A simple initial wet impregnation method was developed, using light magnesium oxide as template. The nitrogen-rich p-phenylenediamine and pyridine dialdehyde were used as precursors to prepare a kind of multiporous carbon material with a high specific surface area of 904 m2 / g and a high nitrogen content of 10 wt.This material has excellent supercapacitor 419F / g @ 0.5A / g) and lithium-ion battery / battery capacity of 2722m / g / g / g / 0.1A / g. Bimetallic Pd10Au/CN catalyst was prepared by using nitrogen-containing porous carbon as the carrier. Compared with pure carbon as support and supported on single metal PdPdioAu-CN, bimetallic Pd10Au/CN catalyst has higher stability and activity. The alloy effect is the reason for the improvement of phenol hydrogenation activity. (3) A solid phase dispersion method has been developed. A highly dispersed Pd/HAP catalyst was prepared. The particle size of Pd prepared by the traditional impregnation method was decreased by 1.2 nmM, and the increase of the active Pd0 content was the possible reason for the significant increase of the hydrogenation activity.
【学位授予单位】：南京大学
【学位级别】：博士
【学位授予年份】：2017
【分类号】：O643.36

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