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电与乙烯共生固体氧化物燃料电池的制备及性能研究

发布时间:2018-11-07 19:36
【摘要】:固体氧化物燃料电池(SOFC)由于其能量转换率高、产物无污染、系统安全性高、模块化结构等优点,对优化能源结构、减少环境污染、促进相关高新技术产业的发展等方面都有着积极的作用,已成为国际上研究的热点。气电共生SOFCs电池可以以烷烃作为燃料气,质子导体型材料作为电解质,在阳极材料的催化作用下,在阴极一侧产生水蒸汽,避免了燃料稀释的弊端,减小了电池系统的复杂性,同时在阳极一侧产生具有工业价值的化学中间体烯烃化学品,这为固体氧化物燃料电池的开发与研究提供新思路。本文在这样的背景下主要针对共生SOFCs电解质和电极材料的制备及成型工艺进行研究。本论文分别采用溶胶凝胶法和高温固相法制备BaCe_(0.7)Zr_(0.2)Y_(0.1)O_3(BCZY)粉体,探究了溶胶凝胶法和高温固相法在不同实验条件下粉体颗粒尺寸的演化情况。通过对比实验得出:当乙二胺四乙酸(EDTA)和柠檬酸的添加量与金属离子摩尔比为1:1.25时,溶胶凝胶法制备的粉体颗粒最小,约25 nm左右;当采用高温固相法制备电解质粉体时,以ZrO_2为锆源,1100℃高温烧结6 h的条件下制备的BCZY粉体颗粒较小,约为50 nm,这样的粉体粒径有利于后续电解质成型工艺的优化。作为共生SOFCs阳极材料,氮化钒是一种类Pt型催化材料,本研究中对BCZY粉体热收缩曲线测试,对其烧结性能进行了研究,发现当温度高达1590℃时,BCZY粉体均未出现收缩平台,烧结性能不够理想,为此分别采用CuO、ZnO、NiO作为烧结助剂来提高电解质的烧结活性,其中CuO效果最佳。论文中探索了不同CuO烧结助剂添加量对电解质致密性及烧结温度的影响,当CuO添加量为1.8 wt%,烧结温度为1300℃时,电解质性能最佳。最后本论文将VN应用为共生SOFCs阳极材料,通过实验研究,采用尿素在氮气气氛下对偏钒酸铵制备的溶胶凝胶进行氮化,在900℃高温烧结2 h得到了纯相氮化钒(VN)。通过将CuO与固相法合成BCZY粉体的前驱体混合、流延、一步烧结的工艺制备阳极支撑电解质半电池,采用浸渍法制备阳极,丝网印刷法制备阴极得到了阳极支撑型全电池,并对其进行了性能测试,测试结果表明电池在700℃时,乙烷转化率为30.8%,乙烯选择性高达90.3%,同时,电池的最大功率密度达到了102 mW cm~(-2)。
[Abstract]:Solid oxide fuel cell (SOFC) has many advantages, such as high energy conversion rate, no pollution, high system safety and modularization structure, so it can optimize energy structure and reduce environmental pollution. Promoting the development of related high-tech industries has played an active role and has become a hot spot in international research. The gas-electric symbiotic SOFCs cell can use alkanes as fuel gas and proton conductor material as electrolyte. Under the catalysis of anode material, water vapor is produced on the cathode side, which avoids the disadvantage of fuel dilution and reduces the complexity of battery system. At the same time, olefin chemicals with industrial value are produced on the anode side, which provides a new idea for the development and research of solid oxide fuel cells. In this context, the preparation and molding process of symbiotic SOFCs electrolytes and electrode materials were studied. In this paper, BaCe_ (0.7) Zr_ (0.2) Y _ (0.1) O _ 3 (BCZY) powders were prepared by sol-gel method and high-temperature solid-state method, respectively. The particle size evolution of sol-gel method and high-temperature solid-state method under different experimental conditions was investigated. The results show that when the molar ratio of ethylenediamine tetraacetic acid (EDTA) and citric acid to metal ion is 1: 1.25, the particle size prepared by sol-gel method is about 25 nm. When the electrolyte powder was prepared by high temperature solid state method, ZrO_2 was used as zirconium source and the size of BCZY powder sintered at 1100 鈩,

本文编号:2317370

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