石墨烯片层和氮掺杂碳纳米笼的制备及其应用研究

发布时间：2018-01-11 03:17

本文关键词：石墨烯片层和氮掺杂碳纳米笼的制备及其应用研究　出处：《华东理工大学》2015年硕士论文　论文类型：学位论文

【摘要】：石墨烯片层(Graphene Nano Sheets, GNS)和碳纳米笼(Carbon Nano Cages, CNCs)是两类非常重要的碳纳米材料。GNS在纳米电子器件,太阳能电池,燃料电池催化剂等多领域有重要的应用价值,CNCs由于其独特的中空结构,较高的石墨化程度在存储,电子器件,燃料电池,药物载体等方面有潜在的应用前景。目前如何大量制备高质量GNS是亟待解决的问题。在燃料电池应用方面,GNS作为载体有望提升Pt催化剂耐久性。燃料电池催化剂仍然面临Pt催化剂成本过高的问题,研究表明,N掺杂碳材料具有一定的氧还原催化活性(ORR),如何制备高N含量高比表面积碳纳米材料也是研究的热点之一。针对上述两个问题,本论文分别在GNS的连续化制备和高N含量CNCs制备以及它们在燃料电池应用等方面进行了重点研究。首先本文采用喷射裂解法,以羰基铁为催化剂前驱体,吡啶为碳源,通过调节铁/碳比和反应温度,实现了GNS连续化制备,并将其用作Pt催化剂载体,研究催化剂耐久性。为了制备高N含量高比表面积CNCs,本文采用浮动气相沉积法,以液态羰基铁为催化剂前驱体,乙炔为碳源,氨气为氮源,制备实心CNC,利用NH4Cl除铁,再经氨气热处理,得到N掺杂空心CNCs,并将其作为ORR催化剂,考察其催化活性和耐久性。本文制备的GNS层数约为3-5层,具有良好的石墨化结构(IG/ID=2.8)和一定的N含量(3.42 at.%)。作为催化剂载体时,通过液相还原法在其表面均匀沉积纳米Pt颗粒,得到Pt/GNS催化剂,催化剂展现了高催化活性和优秀的耐久性。实验制备N掺杂CNCs具有非常高的比表面积(1344 m2 g-1),高N含量(5.3 at.%)。在酸性介质中,作为ORR催化剂展现出与商业Pt/C相当的电催化活性和更优异的耐久性。基于这些研究有望促进GNS的连续化制备研究和商业化应用。N掺杂CNCs作为一种重要的无贵金属催化剂将会在燃料电池领域有很好的应用前景。
[Abstract]:Graphene Nano sheets and carbon Nano Cages. CNCsare two kinds of very important carbon nano-materials. GNS has important application value in many fields such as nano-electronic devices solar cells fuel cell catalysts and so on. Due to its unique hollow structure, CNCs has a higher degree of graphitization in storage, electronic devices, and fuel cells. Drug carriers and other potential applications. How to prepare a large number of high-quality GNS is an urgent problem. In fuel cell applications. GNS is expected to improve the durability of Pt catalyst. The fuel cell catalyst still faces the problem of high cost of Pt catalyst. N-doped carbon materials have a certain catalytic activity of oxygen reduction. How to prepare high N content and high specific surface area carbon nanomaterials is one of the hot topics. In this thesis, the continuous preparation of GNS, the preparation of high N content CNCs and their applications in fuel cells were studied. Firstly, jet pyrolysis method was used in this paper. Using iron carbonyl as catalyst precursor and pyridine as carbon source, continuous preparation of GNS was realized by adjusting iron / carbon ratio and reaction temperature, and used as Pt catalyst support. In order to prepare CNCswith high N content and high specific surface area, liquid carbonyl iron was used as catalyst precursor, acetylene as carbon source and ammonia as nitrogen source in order to prepare CNCswith high N content and high specific surface area. Solid CNCs were prepared by using NH4Cl to remove iron and then treated with ammonia gas to obtain N-doped hollow CNCs and used as ORR catalysts. The catalytic activity and durability were investigated. The number of GNS layers prepared in this paper is about 3-5 layers. It has a good graphitization structure and a certain N content of 3.42 at.0.When it is used as catalyst support. Pt/GNS catalyst was obtained by homogeneous deposition of Pt nanoparticles on the surface by liquid phase reduction method. The catalyst exhibits high catalytic activity and excellent durability. The experimental preparation of N-doped CNCs has a very high specific surface area of 1344m2 / g ~ (-1). The high N content is 5.3 at.0.It is in acid medium. As a ORR catalyst, the electrocatalytic activity is comparable to that of commercial Pt/C with better durability. Based on these studies, it is expected to promote the continuous preparation of GNS and the commercial application of .N-doped CNCs. As an important noble metal-free catalyst, it will have a good prospect in the field of fuel cells.
【学位授予单位】：华东理工大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TQ127.11;TB383.1

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