碳纤维基复合材料负载铂催化剂的制备及其电催化性能研究

发布时间：2018-03-09 20:26

本文选题：碳纤维基复合碳材料　切入点：Pt电催化剂　出处：《新疆大学》2017年硕士论文　论文类型：学位论文

【摘要】：直接甲醇燃料电池(DMFC)体现着燃料电池技术的诸多优势,在固定式和移动式电源应用领域吸引了人们的广泛关注。电极催化剂的活性和稳定性是促进DMFC商业化的重要因素。催化剂的性能与载体材料的性质息息相关,碳纳米纤维作为一种具有较大的比表面积、物理化学性质稳定且易与其它物质复合的碳材料,作为燃料电池催化剂的载体具有很大应用潜力。本文以简单高效的静电纺丝技术,采用聚丙烯腈(PAN)分别与氧化煤、氧化石墨烯(GO)、聚乙烯吡咯烷酮(PVP)等复合制备出了一系列碳纳米纤维基复合材料,并以上述碳材料负载Pt制备了负载型Pt电催化剂,研究了所制备催化剂对甲醇氧化和氧气还原反应的催化性能。主要研究结果如下:1.分别采用PAN、PAN+新疆大黄山褐煤、PAN+醋酸钴及PAN+新疆大黄山褐煤+醋酸钴为原料,利用静电纺丝法制备得到碳纤维(CF)、煤基碳纤维(coal-CF),含钴碳纤维(Co-CF)及含钴的煤基碳纤维(Co-coal-CF)。分别以上述碳材料负载Pt制备得到系列Pt电催化剂:Pt/CF,Pt/coal-CF,Pt/Co-CF和Pt/Co-coal-CF。物理化学表征和电化学性能测试结果表明:在Co-coal-CF的协同作用下,Pt纳米颗粒均匀良好的分散于Co-coal-CF碳载体材料上,所得到的Pt/Co-coal-CF电极催化剂显示出较高的抗CO毒化能力,以及良好的甲醇电氧化活性(甲醇氧化的峰电流值达到92.7A?g-1)和稳定性。2.分别采用静电纺丝、化学还原+静电纺丝方法制备了两种结构不同的石墨烯/碳纤维复合材料:石墨烯嵌入碳纤维(RGO-CF)及石墨烯插层碳纤维(RGO/CF)。并以上述复合材料承载Pt制备得到Pt/RGO-CF和Pt/RGO/CF电极催化剂。物理化学表征及电化学测试结果显示:RGO/CF复合材料表面丰富的石墨氮及含氧官能团、较小的电荷传递阻力以及RGO/CF与Pt之间强烈的相互作用,使Pt/RGO/CF显示出优良的甲醇电氧化和氧还原反应的催化性能,其氧还原催化活性及甲醇电氧化/氧还原反应的催化稳定性甚至优于商业Pt/C催化剂。3.以不同配比的PAN和聚乙烯吡咯烷酮(PVP)为原料,采用静电纺丝技术制备了一系列的复合基碳纤维材料(PCFx,x表示PVP与PAN的质量比),以此负载Pt纳米颗粒得到系列Pt/PCFx催化剂。初步的研究结果表明:一定量PVP与PAN复合制备的PCF材料能有效提高其负载的Pt电催化剂的甲醇电催化氧化活性和稳定性。
[Abstract]:Direct methanol fuel cell (DMFC) embodies many advantages of fuel cell technology. The activity and stability of the electrode catalyst are important factors to promote the commercialization of DMFC. The performance of the catalyst is closely related to the properties of the support material. As a kind of carbon material with large specific surface area, stable physical and chemical properties and easy to compound with other materials, carbon nanofibers have great application potential as catalysts for fuel cell. A series of carbon nanofiber matrix composites were prepared by blending polyacrylonitrile (pan) with oxidized coal, graphene oxide, polyvinylpyrrolidone (PVP) and supported Pt electrocatalysts. The catalytic properties of the catalysts for methanol oxidation and oxygen reduction were studied. The main results were as follows: 1. Pan pan and PAN Xinjiang Dar Huang Shan lignite acetate were used as raw materials, respectively. Carbon fiber (CFT), coal-based carbon fiber (CFC), coal-containing carbon fiber (Co-CFC) and coal-based carbon fiber (Co-coal-CFC) were prepared by electrospinning method. Pt was loaded with the above mentioned carbon materials to prepare a series of Pt electrocatalysts: PT / CFT / PtP / Co-CF and PtP / Co-coal-CFC. Physicochemical characterization and electrochemical characterization and electrochemical properties of Pt / Pt / Coal-CFT / Co / Co-CF were obtained respectively by loading Pt with the above mentioned carbon materials. The results of chemical properties test showed that the Pt nanoparticles were well dispersed on the Co-coal-CF carbon carrier under the synergistic action of Co-coal-CF. The obtained Pt/Co-coal-CF electrode catalyst shows high resistance to CO poisoning and good methanol electrooxidation activity (the peak current value of methanol oxidation is up to 92.7A? G-1) and stability. 2. Electrospinning, Two graphene / carbon fiber composites with different structure: graphene intercalated carbon fiber (RGO-CFC) and graphene intercalated carbon fiber (RGO-CFN) and graphene intercalated carbon fiber (RGO / CFN) were prepared by chemical reduction electrospinning method. Pt/RGO-CF and Pt/RGO/CF were prepared by loading Pt with the above composite materials. Electrode catalysts. Physicochemical characterization and electrochemical measurements show that the surface of the w / r o / CF composite is rich in graphite nitrogen and oxygen-containing functional groups. Because of the small charge transfer resistance and the strong interaction between RGO/CF and Pt, Pt/RGO/CF showed excellent catalytic performance in methanol electrooxidation and oxygen reduction. The catalytic activity of oxygen reduction and the catalytic stability of methanol electrooxidation / oxygen reduction reaction were even better than that of commercial Pt/C catalyst. A series of composite carbon fiber materials (PCFxX x) have been prepared by electrospinning technique to express the mass ratio of PVP to PAN, so as to support Pt nanoparticles to obtain a series of Pt/PCFx catalysts. The preliminary results show that a certain amount of PVP is combined with PAN. The prepared PCF material can effectively improve the catalytic activity and stability of Pt supported electrocatalysts for methanol oxidation.
【学位授予单位】：新疆大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O643.36;TM911.4

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