【作者】 李媛；

【导师】 尹雪峰；

【作者基本信息】 内蒙古大学 ， 环境工程（专业学位）， 2015， 硕士

【摘要】 为了改善载氧体在多次循环后的碳沉积现象,本文以研究多环芳烃(PAHs)的生成特性为切入点来探究煤化学链燃烧反应机理以及铜基载氧体和PAHs的相互作用机制。在不同因素水平下对负硅铜基及负钛铜基载氧体进行实验研究,利用气相色谱法对反应后收集烟气中和煤渣中的PAHs进行定性定量分析。实验研究方面主要有：载氧体的制作方法；化学链燃烧反应的条件；比较两种铜基载氧体的PAHs排放特性,寻找控制碳沉积的有效方法。本文的主要研究结果如下：(1)煤化学链燃烧较生成三环芳烃最多,PAHs产量的差异主要表现在烟气中；对于CuO/SiO2载氧体来说烟煤1较适合,对于CuO/TiO2载氧体来说烟煤2较适合；高温区(800～1000℃)有利于控制PAHs的产量。(2)CuO本身具有多元催化功能,对PAHs既有催化合成作用又有氧化分解作用,温度小于800℃,CuO有利于催化合成PAHs,温度大于800℃,催化合成作用逐渐减弱。(3)TiO2有较大的比表面积,有较好的光催化活性,并且有较高的氧化性,可催化分解PAHs,TiO2为惰性载体表现出很好的反应性。(4)采用不同的CuO与惰性载体的制备比例,利用机械混合法所得的两种载氧体最合适的制备比例均为7：3。浸渍法较机械混合法更有利于控制载氧体的碳沉积。(5)对CuO/TiO2载氧体在使用机械混合法制备过程中添加了一定量的分散剂,制备出的载氧体具有较好的孔隙结构,并在实验中表现了较好的反应活性,使燃烧反应彻底,有效控制了PAHs的产量。更多还原

【Abstract】 In order to improve phenomenon that the carbon deposition of oxygen carriers after repeated cycling, in this paper, based on the study of Polycyclic Aromatic Hydrocarbons (PAHs) generation characteristics to explore the reaction mechanism of chemical-looping combustion of coal and the interaction mechanism of copper-based oxygen carriers and PAHs. At different levels for the experimental study of Cu-based oxygen carrier with titanium and Cu-based oxygen carrier with silicon, after the reaction, the experiments carried out by GC for qualitative and quantitative analysis of PAHs in smoke and cinders. Experimental studies are:production methods oxygen carrier; chemical-looping combustion conditions; PAHs emission characteristics of different copper-based oxygen carriers; look for effective methods to control carbon deposits.The main findings are as follows:(1) Tricyclic aromatic hydrocarbons were produced most during the chemical-looping combustion; the difference is mainly in the production of PAHs in flue gas; coal 1 is more suitable for the CuO/SiO2 oxygen carrier; coal 2 is more suitable for the CuO/TiO2 oxygen carrier; the zone of high temperature (800-1000℃) can control the production of PAHs.(2) CuO having a multi catalytic function, it could catalytic synthesis PAHs and oxidative decomposition PAHs. The temperature less than 800℃, CuO beneficial catalytic synthesis of PAHs; When the temperature is above 800, catalytic synthesis of gradually weakened.(3) TiO2 has larger surface area, better photocatalytic activity, and has high oxidation resistance, can catalyze the decomposition of PAHs, TiO2 as inert carrier showed good reactivity.(4) Preparation of oxygen carriers with different proportions of CuO and inert carrier, the suitable preparation proportion was 7:3 with the mechanical mixing. Impregnation method is more conducive to control carbon deposition than mechanical mixing.(5) Adds a certain amount of dispersant in the preparation process with mechanical mixing method of CuO/TiO2 oxygen carrier, it has better pore structure, and showed good activity in the experiment, the combustion reaction completely, effectively controlled the production of PAHs.更多还原