【摘要】：多孔碳材料由于其獨特的結(jié)構(gòu)和性質(zhì)引起了人們的廣泛關(guān)注并在吸附、分離、催化及電化學等方面展現(xiàn)了優(yōu)異的應用性能。通過選擇合適的合成條件與方法,可對其進行形貌及結(jié)構(gòu)的可控制備。但純的多孔碳材料表面存在一定惰性,反應活性低,為提高化學活性位,可通過引入雜原子對其進行功能化修飾,從而進一步提高碳材料的物理和化學性能,使其具有更加廣闊的應用發(fā)展前景。論文的主要研究內(nèi)容如下:1)提出一種簡單而獨特的制備具有二維六方有序結(jié)構(gòu)的介孔碳的方法,即“熱解-沉積”法。該方法以樹脂聚合物在高溫碳化中釋放的尾氣為碳源,鐵修飾的SBA-15為模板劑,將樹脂聚合物和SBA-15模板放在同一個通氮氣的碳化爐中碳化。在碳化過程中,樹脂聚合物熱解釋放出的尾氣隨著氮氣可同時被沉積并捕獲到SBA-15模板的孔道結(jié)構(gòu)中,在鐵的催化下合成MCs。并對該介孔碳材料在6 mol L-1 KOH溶液中進行了其電化學性質(zhì)的研究,探討其做為電極材料的超級電容器的性能。2)以間氨基苯酚為碳、氮源,正硅酸乙酯為結(jié)構(gòu)輔助劑,十六烷基三甲基溴化銨做為表面活性劑,在氨水的催化下,通過“硅助劑”的方法一步制備高度分散且粒徑均勻可調(diào)的氮摻雜中空介孔碳球。該方法以間氨基苯酚同時做為碳源和氮源原位地對中空碳球進行氮摻雜實現(xiàn)功能化修飾,并研究溶液中乙醇、水的體積比,對所制備的N-HMCSs的直徑、空腔直徑、壁厚的影響。而且考察氮摻雜中空介孔碳球做為電極材料的超級電容器性能,探討對材料進行氮摻雜后對其電容性能的影響。3)提出了一種簡單、可行的一步溶膠-凝膠法制備了粒徑和形貌可調(diào)的氮摻雜的中空介孔碳球。在這個合成過程中,樹脂做為碳源,正硅酸乙酯做為結(jié)構(gòu)助劑,咪唑類離子液體(1-alkyl-3-methylimidazolium bromide,[CnMim]Br,n=4,8,12,16)具有“三合一”的作用,即不僅做為軟模板又做為氮源和部分碳源。該方法根據(jù)離子液體摻氮的性質(zhì)及離子液體在堿性溶液中與帶負電荷的二氧化硅低聚物、樹脂集聚體之間較強的靜電相互作用,一步原位的合成了氮摻雜的中空介孔碳球。通過改變離子液體的量研究其對所制備的N-HMCSs粒徑、形貌、結(jié)構(gòu)、均勻性的影響。同時通過改變離子液體烷基鏈的長度,探究烷基鏈的長度對N-HMCSs形貌形成的作用,并考察氮摻雜的中空介孔碳球用作超級電容器電極材料的電化學性能。
[Abstract]:Porous carbon materials have attracted wide attention due to their unique structure and properties, and have shown excellent applications in adsorption, separation, catalysis and electrochemistry. The morphology and structure can be controlled by selecting suitable synthesis conditions and methods. However, the surface of pure porous carbon materials is inert and the reaction activity is low. In order to improve the chemical active sites, the physical and chemical properties of carbon materials can be further improved by introducing hetero-atoms to functionalize them. So that it has a broader application and development prospects. The main contents of this paper are as follows: (1) A simple and unique method for preparing mesoporous carbon with two-dimensional hexagonal ordered structure is proposed, which is called "pyrolysis-deposition" method. In this method, the tail gas released by resin polymer in high temperature carbonation was used as carbon source, and the ferric modified SBA-15 was used as template. The resin polymer and SBA-15 template were carbonated in the same nitrogen carbonization furnace. During carbonation, the tail gas released from the pyrolysis of the resin polymer can be deposited simultaneously with nitrogen and trapped in the pore structure of SBA-15 template, and then synthesized by the catalysis of iron. The electrochemical properties of the mesoporous carbon material in 6 mol L-1 Koh solution were studied. The performance of the supercapacitor as electrode material was discussed. The mesoporous carbon was composed of m-aminophenol as carbon, nitrogen source and ethyl orthosilicate as structural auxiliary agent. Using cetyltrimethylammonium bromide as a surfactant and catalyzed by ammonia, N-doped hollow mesoporous carbon spheres with highly dispersed and uniform particle size were prepared by the method of "silicon promoter". In this method, m-aminophenol was used as carbon source and nitrogen source to functionalize the hollow carbon spheres in situ, and the effects of the volume ratio of ethanol and water in solution on the diameter, cavity diameter and wall thickness of N-HMCSs were studied. Furthermore, a simple method was proposed to investigate the performance of nitrogen doped hollow mesoporous carbon ball as electrode material and to investigate the effect of nitrogen doping on the capacitance performance of the supercapacitor. Nitrogen doped hollow mesoporous carbon spheres with adjustable particle size and morphology were prepared by one step sol-gel method. In this process, resin is used as carbon source, tetraethyl orthosilicate as structural assistant, and imidazole ionic liquid ([CnMim] Brnbumin 4CnMim) has the function of "three-in-one", which is not only used as a soft template, but also as a nitrogen source and a part of carbon source. According to the properties of nitrogen-doped ionic liquids and the strong electrostatic interaction between ionic liquids and negatively charged silica oligomers and resin aggregates, nitrogen-doped hollow mesoporous carbon spheres were synthesized in one step in situ. The effects of ionic liquids on the particle size, morphology, structure and homogeneity of N-HMCSs were studied by changing the amount of ionic liquids. The effects of alkyl chain length on the morphology of N-HMCSs were investigated by changing the length of ionic liquid alkyl chain. The electrochemical properties of N-doped hollow mesoporous carbon spheres as electrode materials for supercapacitor were investigated.
【學位授予單位】：河北科技大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TQ127.11;TB383.4

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本文編號：2132447