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氮摻雜多孔碳材料的制備及其電化學性能研究

發(fā)布時間:2018-04-10 07:08

  本文選題:超級電容器 切入點:氮摻雜 出處:《揚州大學》2017年碩士論文


【摘要】:碳材料由于其來源豐富、導電性好、比表面積大且穩(wěn)定性好,成為超級電容器最重要的電極材料。但其主要是通過雙電層電容進行儲能,能量密度較小。因此,如何提高電極材料的能量密度成為當前學術界關注的研究熱點。根據能量密度計算公式知:E=0.5CV2,可以通過增大電壓窗口或比電容來提高材料的能量密度。本文以明膠為碳源,分別通過尿素作為氮源對其氮摻雜改性,SiO_2作為模板增加比表面積,然后進一步負載2,5-二甲氧基-1,4-苯醌(DMQ)制備復合材料增加比電容。通過透射電鏡(TEM)、掃描電鏡(SEM)、X-射線衍射(XRD)以及拉曼光譜(Raman)等手段,對材料的形貌和結構等情況進行表征。采用多種電化學測試手段研究祠料的電化學性能以及循環(huán)穩(wěn)定性。主要研究工作包括以下幾個方面:(1)以明膠為碳源、尿素為氮源和模板,通過“原位”摻氮法合成氮摻雜介孔碳納米纖維(N-m-CNFs)。研究了尿素的模板作用、摻入量以及煅燒溫度對材料形貌、結構和電化學性能的影響。利用三電極體系,1MH2SO4作為電解液,測試不同氮摻雜量及碳化溫度下碳纖維的電化學性能。結果表明,尿素摻入后,碳材料呈纖維狀,氮含量高達14.632 wt%。在1Ag~(-1)的電流密度下,碳纖維的比電容值可達到230.9Fg~(-1),遠大于不摻氮的碳材料(86.9Fg~(-1)),且具有較好的循環(huán)穩(wěn)定性。(2)以明膠為碳源和氮源、SiO_2為模板,通過模板法得到孔徑均一的氮摻雜多孔碳片層材料(N-p-CSs)。通過加入不同粒徑SiO_2,調控制備不同孔徑和比表面積的多孔碳片層材料,研究不同煅燒溫度對所合成碳材料形貌、結構以及電化學性能的影響。結果表明,相對于無孔碳材料,不同粒徑SiO_2所制備的碳材料比電容明顯增大。其中,20nmSiO_2作為模板制備得到的碳材料,比電容值在電流密度為1 A g~(-1)時達到252.3 F g~(-1)。(3)以上述制備的多孔碳片層材料為基材,利用水熱法在碳材料表面負載DMQ,制備DMQ@N-p-CSs復合材料。探討了 DMQ負載量對所合成碳材料形貌、結構的影響,并分別測試了不同復合材料的電化學性能。實驗表明,當DMQ與N-p-CSs質量比為1:1制備得到的復合材料具有較好的循環(huán)性能和較高的比電容。在電流密度為1 Ag~(-1)時,比電容可達到356.4 F g-2,經過10000次循環(huán)之后保持98.6%的初始比電容。
[Abstract]:Carbon is the most important electrode material for supercapacitors due to its rich source, good conductivity, large specific surface area and good stability.However, the energy storage is mainly by double layer capacitance, and the energy density is small.Therefore, how to improve the energy density of electrode materials has become the focus of academic research.According to the calculation formula of energy density, we know that the energy density of the material can be increased by increasing the voltage window or specific capacitance.In this paper, using gelatin as carbon source and urea as nitrogen source to increase the specific surface area of nitrogen-doped modified SiO-2 as template, then the composite was prepared by further loading 2o 5-dimethoxy-4-benzoquinone (DMQ) to increase specific capacitance.The morphology and structure of the materials were characterized by means of transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray diffraction (XRD) and Raman spectroscopy (Raman).The electrochemical performance and cyclic stability of ancestral materials were studied by various electrochemical methods.The main research work includes the following aspects: (1) N-doped mesoporous carbon nanofibers N-m-CNFsO were synthesized by "in-situ" nitrogen-doped method, using gelatin as carbon source and urea as nitrogen source and template.The effects of the template, the dosage of urea and the calcination temperature on the morphology, structure and electrochemical properties of urea were studied.The electrochemical properties of carbon fibers with different nitrogen doping amount and carbonization temperature were measured by using the three-electrode system of 1MH _ 2SO _ 4 as electrolyte.The results showed that the carbon material was fibrous and the nitrogen content was as high as 14.632 wts after the addition of urea.The specific capacitance value of carbon fiber can reach 230.9 FG ~ (-1) at current density, which is much larger than that of carbon material without nitrogen (86.9 FG ~ (-1)), and has good cycling stability. 2) gelatin as carbon source and nitrogen source SiO2 as template.N-p-CSsN doped porous carbon laminates with uniform pore size were obtained by template method.Porous carbon lamellar materials with different pore size and specific surface area were prepared by adding SiO-2 with different particle sizes. The effects of calcination temperature on the morphology, structure and electrochemical properties of the synthesized carbon materials were studied.The results show that the specific capacitance of carbon materials prepared with different particle sizes of SiO_2 is significantly larger than that of non-porous carbon materials.The DMQ@N-p-CSs composites were prepared by hydrothermal method on the surface of carbon materials prepared by using SiO-2 as template, and the specific capacitance reached 252.3 F g / g ~ (-1) when the current density was 1 A / g ~ (-1)). The porous carbon lamellar material was used as the base material.The effects of DMQ loading on the morphology and structure of the synthesized carbon materials were investigated, and the electrochemical properties of different composites were tested.The experimental results show that the composites prepared at 1:1 mass ratio of DMQ to N-p-CSs have better cycling performance and higher specific capacitance.The specific capacitance can reach 356.4 F g ~ (-2) when the current density is 1 Agg ~ (-1), and the initial capacitance is 98.6% after 10000 cycles.
【學位授予單位】:揚州大學
【學位級別】:碩士
【學位授予年份】:2017
【分類號】:TQ127.11;TB383.4

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