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微波—微乳法制备燃料电池催化剂的研究

发布时间:2018-12-21 16:00
【摘要】: 现在新型制备方法的研究对于燃料电池催化剂的性能的提升变得十分重要。本文利用微波多元醇的方法合成了高分散的Pt/C催化剂并研究了不同制备条件对催化剂性能的影响。接着以碳纳米管作为催化剂载体,用微波加热法合成了Pt和Pt-Ru二元金属催化剂。初步探讨了将微波和微乳相结合的方法用于制备Pt-Ru二元合金催化剂。得到了如下结论: 1.本论文通过加入醋酸钠,调节溶液pH值,改变催化剂的铂碳质量比,对碳载体进行预处理制备了Pt/C催化剂。利用XRD,TEM,SEM-EDS,CV等手段对制备的纳米粒子的粒径,表面形貌,元素比例以及电催化性能进行了分析表征。实验结果证明添加0.6ml醋酸钠,调节pH值至10,硝酸处理碳载体,铂质量含量为40%的条件下所制备的催化剂具有最均匀的Pt纳米粒子粒径分布和最佳催化性能。 2.本论文以改性后的碳纳米管(CNTs)作为载体制备了催化剂。通过XRD,FTIR以及CV等手段进行了表征。结果证明,以碳纳米管作为载体要优于碳粉。碳纳米管经过酸处理改性后,红外测试证明其表面接枝了许多羟基和羧基官能团。酰胺化处理使其表面接枝上了酰胺基团。负载Pt催化剂后其甲醇峰电流密度分别达到580Ag-1Pt和600Ag-1Pt。XRD测试证明Pt-Ru合金纳米粒子的平均粒径为5.2nm。SEM-EDS测试表明Pt与Ru的元素物质的量之比与理论值相符合。催化剂的甲醇氧化电流峰值达到6.15mA,其氧化峰的起始电位比一元Pt催化剂的更低。 3.将微波法和微乳法相结合制备Pt-Ru二元催化剂。催化剂经170℃,250℃,600℃处理后粒径在5.2nm,5.5nm和7.1nm左右。TEM测试表明,制备的催化剂纳米粒子具有良好的分散性。经250℃热处理后,纳米粒子的粒径大概在5nm左右。通过SEM-EDS测试了Pt:Ru的物质的量之比,结果与理论值相符。通过控制加料顺序使纳米粒子中的成分得到很好的控制。循环伏安测试表明,不同的温度下,250℃热处理的催化剂催化性能最好,而在triton-100/异丙醇/环己烷/乙二醇的微乳体系中制备的Pt-Ru催化剂具有最佳的电催化性能。
[Abstract]:The research of new preparation methods is very important for improving the performance of fuel cell catalysts. In this paper, the highly dispersed Pt/C catalyst was synthesized by microwave polyol method and the effect of different preparation conditions on the catalyst performance was studied. Then Pt and Pt-Ru binary metal catalysts were synthesized by microwave heating using carbon nanotubes as catalyst carrier. The method of microwave and microemulsion was used to prepare Pt-Ru binary alloy catalyst. The conclusions are as follows: 1. In this paper, the Pt/C catalyst was prepared by adding sodium acetate, adjusting the pH value of the solution and changing the platinum / carbon mass ratio of the catalyst. The particle size, surface morphology, elemental ratio and electrocatalytic properties of the prepared nanoparticles were characterized by XRD,TEM,SEM-EDS,CV. The experimental results show that the catalyst prepared by adding 0.6ml sodium acetate, adjusting pH to 10, treating carbon carrier with nitric acid and platinum content of 40% has the most uniform particle size distribution and the best catalytic performance of Pt nanoparticles. 2. In this thesis, the modified carbon nanotube (CNTs) was used as the support to prepare the catalyst. It was characterized by XRD,FTIR and CV. The results show that carbon nanotubes are better than carbon powder. After modified by acid treatment, the surface of carbon nanotubes was grafted with many hydroxyl and carboxyl functional groups. The amide group was grafted on the surface by amidation. The methanol peak current density of the supported Pt catalyst reached 580Ag-1Pt and 600Ag-1Pt.XRD respectively. The average particle size of the Pt-Ru alloy nanoparticles was 5.2nm.SEM-EDS. The results showed that the ratio of the content of Pt to the element substance of Ru was higher than that of Pt. In accordance with the theoretical values. The peak value of methanol oxidation current of the catalyst is 6.15mA.The initial potential of the oxidation peak of the catalyst is lower than that of the monolithic Pt catalyst. 3. Pt-Ru binary catalyst was prepared by microwave method and microemulsion method. The catalyst was treated at 170 鈩,

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