氨基聚膦腈微球的合成、功能化及应用
发布时间:2018-01-06 23:21
本文关键词:氨基聚膦腈微球的合成、功能化及应用 出处:《郑州大学》2017年硕士论文 论文类型:学位论文
更多相关文章: 聚膦腈 聚乙烯亚胺 微球 中空 染料 选择性吸附 催化 电化学
【摘要】:聚合物纳米材料不仅结构丰富,而且具有独特的性能,可通过功能化修饰来制备具有特殊功能的聚合物复合纳米材料,又可作为碳前驱体来制备碳纳米材料。基于这些独特的结构和性能,功能聚合物纳米材料在环境、催化、生物、医药、能源等诸多方面都有着广泛的应用研究,因而对聚合物纳米材料的制备及其应用进行研究具有重要的理论和实际意义,这也是当前科研人员研究的热点之一。本文制备了一种富含氨基的聚膦腈微球,并通过其负载贵金属纳米微粒和高温碳化制备了两种衍生的纳米材料,分别研究了所构建纳米材料在染料吸附、催化和电化学方面的应用。主要的研究内容和结果如下:(1)利用沉淀聚合法,在超声条件下,以六氯环三磷腈(HCCP)和低分子量支化聚乙烯亚胺(PEI)作为共聚单体,三乙胺(TEA)作为缚酸剂,乙腈作为溶剂,成功合成出了富含氨基的实心聚膦腈微球。并且又利用丙酮处理60min,便可得到中空氨基聚膦腈微球,并通过不同的测试方法(SEM、TEM、FITR、BET和Zeta电位等)对其结构进行了表征。(2)以中空氨基聚膦腈微球为吸附剂,通过吸附法处理水溶液中携带不同电荷的署红Y、酸性铬兰K、甲基橙、署红B、孔雀石绿、臧红T、中性红、罗丹明B和亚甲基蓝染料。发现对阴离子染料署红Y、酸性铬兰K和甲基橙的吸附容量都在1000 mg/g以上。系统、深入地探索了影响阴离子染料署红Y、酸性铬兰K和甲基橙吸附的相关因素(溶液pH、温度、浓度等),使用吸附模型研究了吸附动力学和热力学,并且探索和研究了其高效吸附的机理。(3)以合成的富含大量氨基的实心聚膦腈微球为催化剂载体,在其表面负载单金属纳米粒子Au、Ag和双金属纳米粒子Au-Ag后,制备出负载贵金属纳米粒子的复合微球,并研究了其催化还原对硝基苯酚的性能。研究结果表明粒径均一的贵金属纳米粒子可以在微球载体表面均匀分散,载体中含氮官能团的存在可导致载体与金属离子之间有较强的络合作用。催化性能研究结果表明,负载双金属相比于负载单金属其催化性能明显提高,归结于金和银的协同效应。(4)以不同单体比例制备的实心氨基聚膦腈微球为前驱体,通过控制不同的碳化工艺,得到不同氮含量掺杂的碳球,当碳微球作为超级电容器负极材料时,对其做了一些必要的电化学测试。发现在750℃碳化温度下,其在1 A/g的电流密度下比电容可达到348 F/g,在20 A/g的电流密度下比电容仍可达到200F/g,电容保持率在57.5%。并且在20 A/g的电流密度下进行10000次充放电后,比电容仍保持在96.7%,表现出较好的循环稳定性。
[Abstract]:Polymer nanomaterials are not only rich in structure but also have unique properties. Polymer nanocomposites with special functions can be prepared by functionalized modification. Based on these unique structures and properties, functional polymer nanomaterials have been widely used in environment, catalysis, biology, medicine, energy and so on. Therefore, it is of great theoretical and practical significance to study the preparation and application of polymer nanomaterials, which is one of the hotspots of current researchers. In this paper, a polyphosphonitrile microsphere rich in amino groups has been prepared. Two kinds of derivative nanomaterials were prepared by loaded noble metal nanoparticles and carbonized at high temperature, and the adsorption of the constructed nanomaterials on dyes was studied respectively. Applications in catalysis and electrochemistry. The main research contents and results are as follows: 1) using precipitation polymerization under ultrasonic conditions. Hexachlorocyclotriphosphazene (HCCP) and low molecular weight branched polyimide (PEI) were used as comonomer, triethylamine (tea) as acid binding agent and acetonitrile as solvent. Solid polyphosphonitrile microspheres rich in amino groups were successfully synthesized and then treated with acetone for 60 min to obtain hollow amino polyphosphonitrile microspheres. Its structure was characterized by FITR BET and Zeta potential. (2) the hollow aminopolyphosphonitrile microspheres were used as adsorbent to treat the red Y with different charge in aqueous solution by adsorption method. Acid chrome blue K, methyl orange, red red B, malachite green, Zang Hong T, neutral red, Rhodamine B and methylene blue dyestuff. The adsorption capacities of acid chrome blue K and methyl orange were all over 1 000 mg/g. The factors affecting the adsorption of anionic dye red Y, acid chrome blue K and methyl orange (pH solution) were systematically explored. The adsorption kinetics and thermodynamics were studied by using the adsorption model. The mechanism of its high efficiency adsorption was explored and studied. The solid polyphosphonitrile microspheres containing a large amount of amino acids were used as the catalyst carrier and the monometallic nanoparticles au were loaded on its surface. After Ag and bimetallic nanoparticles Au-Ag, composite microspheres loaded with noble metal nanoparticles were prepared. The catalytic reduction of p-nitrophenol was studied. The results showed that the noble metal nanoparticles with uniform particle size could be uniformly dispersed on the surface of the microspheres. The existence of nitrogen-containing functional groups in the support can lead to a strong complexation between the carrier and metal ions. The results of catalytic performance study show that the catalytic performance of the supported bimetallic is significantly higher than that of the supported monometallic. Due to the synergistic effect of gold and silver, the carbon spheres doped with different nitrogen content were obtained by controlling different carbonization processes using solid polyphosphonitrile microspheres prepared with different monomer ratios as precursors. When carbon microspheres were used as anode materials for supercapacitors, some necessary electrochemical tests were carried out. It was found that the carbon microspheres were carbonized at 750 鈩,
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