掺氮碳纳米管的制备与氧还原性能研究

发布时间：2018-03-22 04:28

  本文选题：顺子交换膜燃料电池　切入点：掺氮碳纳米管　出处：《北京化工大学》2015年硕士论文　论文类型：学位论文

【摘要】：质子交换膜燃料电池作为一种清洁高效能源受到越来越多的关注,而阴极催化剂因其对燃料电池成本和性能的重要影响而成为研究热点。迄今为止,人们研究较为成熟的催化剂为铂或铂合金催化剂因价格昂贵而限制了质子交换膜燃料电池的商业化发展。本文以苯胺,三聚氰胺,吡咯为氮源制备了掺氮碳纳米管催化剂,并对制备的温度和掺氮比例进行优选,目的是制备出适合工业化生产的高效、低成本催化剂。具体内容如下：1.通过传统Hummer法制得了中度氧化碳管(moCNTs),并通过LSV, EIS, SEM, FT-IR等测试测试表明所制备的moCNTs表面含有较多的含氧基团,内壁结构保持完整。2.以苯胺作为氮源,通过原位复合和高温热解的方法制备出moCNTs/PANI-Fe体系的催化剂,并优化了制备条件。详细考察了温度与掺氮比例对催化剂性能和形貌的影响。电化学测试表明：在650℃下掺苯胺比例为mmoCNTs/PANI-1:0.4时制备的催化剂具有最好催化活性,其氧还原起始还原电位是0.73 V。3.以苯胺和三聚氰胺作为氮源,利用原位复合法高温热解的方法制备出moCNTs/PANI/Mela(FeCl3)体系的催化剂。详细考察了温度与掺氮比例对催化剂性能和形貌的影响。电化学测试表明：在650℃下投料比例为mmocNTs/PANI/Mela= 1:13:6.5,铁加入量为5%时制备的催化剂具有最好的ORR活性,在酸性电解液中其氧起始还原电位是0.87V,优于同类非铂催化剂。通过结构表征发现该催化剂为类石墨烯片状结构,且石墨氮含量较高,证明这一特征有利于提高ORR催化活性。4.以苯胺和吡咯作为氮源,利用原位复合法高温热解的方法制备出moCNTs/PANI/Pyrr-Fe体系的催化剂。详细考察了温度与掺氮比例对催化剂性能和形貌的影响。电化学测试表明：在650℃下投料比例为mmocNTs/PANI/Pyrr=1:0.8:0.4时制备的催化剂具有最好的ORR活性,其氧起始还原电位是0.70 V。
[Abstract]:As a kind of clean and efficient energy, proton exchange membrane fuel cell (PEMFC) has attracted more and more attention, and cathodic catalyst has become a research hotspot because of its important influence on the cost and performance of fuel cell. The more mature catalysts are platinum or platinum alloy catalysts, which limit the commercial development of proton exchange membrane fuel cells due to their high price. In this paper, nitrogen-doped carbon nanotube catalysts were prepared using aniline, melamine and pyrrole as nitrogen sources. The preparation temperature and the ratio of nitrogen to nitrogen were optimized for the purpose of producing high efficiency suitable for industrial production. Low cost catalyst. 1. Moderate carbon oxide tube moCNTsN was obtained by conventional Hummer method. The results of moCNTs, EIS, SEM and FT-IR tests showed that there were more oxygen-containing groups on the surface of the prepared moCNTs. Using aniline as nitrogen source, the catalyst of moCNTs/PANI-Fe system was prepared by in situ recombination and pyrolysis at high temperature. The effects of temperature and nitrogen ratio on the performance and morphology of the catalyst were investigated in detail. The electrochemical test showed that the catalyst prepared at 650 鈩，

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