杂原子掺杂碳纳米复合材料的制备及其电催化应用研究
发布时间：2018-09-17 19:00
【摘要】：碳纳米材料因比表面积高、孔隙率发达、环境友好、价格低廉及独特的构架组成等特点而成为一种优良的催化剂载体。近年来,碳纳米材料在电化学领域得到了更广泛的应用,例如用作传感器或燃料电池的电极催化剂等。所以,为了提高燃料电池电催化剂的电化学性能,通过向碳材料中掺杂杂原子可以调节其结构和表面化学性能,改善它的电催化行为。本论文详细探究了氮、磷杂原子单或双掺杂低铂或无金属碳纳米材料的制备方法,并且将其作为低温燃料电池催化剂时的电化学性能。本论文主要内容由绪论、实验和结论三部分组成,具体如下:1.使用硬模板法合成了不同磷含量的有序介孔碳纳米复合材料Pt/POMCs,并将其作为直接甲醇燃料电池的阳极催化剂。利用透射电镜(TEM)、X-射线光电子能谱法(XPS)等表征了Pt/POMCs的表面结构,用循环伏安法(CV)和计时电流法(CA)研究了修饰电极表面的电化学行为。实验结果显示,与Pt/OMCs、Pt Ru/XC和商业Pt/C催化剂相比,Pt/POMC有更大的电化学活性比表面积(ECSA)、对甲醇有更高的电催化氧化性能,同时有较强的抗CO中毒能力。这些性能的改善表明了掺杂适量P的纳米复合材料Pt/P7OMCs可作为一种优良的直接甲醇燃料电池阳极催化剂。2.磷掺杂、聚吡咯功能化的含氮碳纳米管(P/NCNTs)作为无金属的电催化剂,用于增强碱性溶液中氧化还原反应(ORR)活性。TEM、XPS等表征显示P/NCNTs复合材料中P原子和碳骨架共价结合,这可以在催化剂中引进缺陷位点并且可以诱导电荷不均匀分布。另外,掺杂磷原子后吡啶氮含量增加,这对提高ORR活性有很大的促进作用。CV和旋转圆盘电极(RDE)循环伏安法结果显示P/NCNTs复合材料可大幅度提高ORR的电催化活性、稳定性和抗甲醇干扰能力。这些性能的提高表明了P/NCNTs复合材料可作为一种优良的非金属氧还原电催化剂。
[Abstract]:Carbon nanomaterials have become an excellent catalyst carrier due to their high specific surface area, developed porosity, environmentally friendly, low cost and unique structure composition. In recent years, carbon nanomaterials have been widely used in the field of electrochemistry, for example, as electrode catalysts for sensors or fuel cells. Therefore, in order to improve the electrochemical performance of fuel cell electrocatalysts, the structure and surface chemical properties can be adjusted by doping hetero-atoms into carbon materials, and its electrocatalytic behavior can be improved. In this paper, the preparation methods of low platinum or metal-free carbon nanomaterials with single or double doped nitrogen and phosphorus atoms were investigated in detail, and their electrochemical properties were used as catalysts for low temperature fuel cells. This thesis is composed of three parts: introduction, experiment and conclusion, as follows: 1. Ordered mesoporous carbon nanocomposites (Pt/POMCs,) with different phosphorus contents were synthesized by hard template method and used as anode catalysts for direct methanol fuel cells (DMFC). The surface structure of Pt/POMCs was characterized by transmission electron microscopy (TEM) X-ray photoelectron spectroscopy (XPS). The electrochemical behavior of the modified electrode was studied by cyclic voltammetry (CV) and chronoamperometric method (CA). The results showed that compared with Pt/OMCs,Pt Ru/XC and commercial Pt/C catalysts, (ECSA), had higher electrochemical activity and higher specific surface area for methanol oxidation, and had a stronger ability to resist CO poisoning. The improvement of these properties indicates that the nano-composite Pt/P7OMCs doped with appropriate amount of P can be used as an excellent anode catalyst for direct methanol fuel cell (DMFC). Phosphorus doped and polypyrrole functionalized nitrogen-containing carbon nanotubes (P/NCNTs) were used as metal-free electrocatalysts to enhance the (ORR) activity of redox reaction in alkaline solution. The defect sites can be introduced into the catalyst and the charge distribution can be induced inhomogeneously. In addition, the content of pyridine nitrogen increased after doping phosphorus atom, which promoted the activity of ORR greatly. CV and (RDE) cyclic voltammetry of rotating disk electrode showed that P/NCNTs composite could improve the electrocatalytic activity of ORR significantly. Stability and ability to resist methanol interference. The improvement of these properties indicates that P/NCNTs composite can be used as an excellent electrocatalyst for non-metallic oxygen reduction.
【学位授予单位】：东北师范大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：O613.71;TM911.4
本文编号：2246810
[Abstract]:Carbon nanomaterials have become an excellent catalyst carrier due to their high specific surface area, developed porosity, environmentally friendly, low cost and unique structure composition. In recent years, carbon nanomaterials have been widely used in the field of electrochemistry, for example, as electrode catalysts for sensors or fuel cells. Therefore, in order to improve the electrochemical performance of fuel cell electrocatalysts, the structure and surface chemical properties can be adjusted by doping hetero-atoms into carbon materials, and its electrocatalytic behavior can be improved. In this paper, the preparation methods of low platinum or metal-free carbon nanomaterials with single or double doped nitrogen and phosphorus atoms were investigated in detail, and their electrochemical properties were used as catalysts for low temperature fuel cells. This thesis is composed of three parts: introduction, experiment and conclusion, as follows: 1. Ordered mesoporous carbon nanocomposites (Pt/POMCs,) with different phosphorus contents were synthesized by hard template method and used as anode catalysts for direct methanol fuel cells (DMFC). The surface structure of Pt/POMCs was characterized by transmission electron microscopy (TEM) X-ray photoelectron spectroscopy (XPS). The electrochemical behavior of the modified electrode was studied by cyclic voltammetry (CV) and chronoamperometric method (CA). The results showed that compared with Pt/OMCs,Pt Ru/XC and commercial Pt/C catalysts, (ECSA), had higher electrochemical activity and higher specific surface area for methanol oxidation, and had a stronger ability to resist CO poisoning. The improvement of these properties indicates that the nano-composite Pt/P7OMCs doped with appropriate amount of P can be used as an excellent anode catalyst for direct methanol fuel cell (DMFC). Phosphorus doped and polypyrrole functionalized nitrogen-containing carbon nanotubes (P/NCNTs) were used as metal-free electrocatalysts to enhance the (ORR) activity of redox reaction in alkaline solution. The defect sites can be introduced into the catalyst and the charge distribution can be induced inhomogeneously. In addition, the content of pyridine nitrogen increased after doping phosphorus atom, which promoted the activity of ORR greatly. CV and (RDE) cyclic voltammetry of rotating disk electrode showed that P/NCNTs composite could improve the electrocatalytic activity of ORR significantly. Stability and ability to resist methanol interference. The improvement of these properties indicates that P/NCNTs composite can be used as an excellent electrocatalyst for non-metallic oxygen reduction.
【学位授予单位】：东北师范大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：O613.71;TM911.4
【参考文献】
相关期刊论文 前1条
1 朱绍文,贾志杰,李钟泽;碳纳米管及其应用前景[J];科技导报;1999年12期
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