废弃含铜催化剂资源化研究
发布时间：2018-02-20 08:02
本文关键词： 废弃含铜催化剂 热解 动力学 氨浸 氧化亚铜 出处：《西南科技大学》2015年硕士论文 论文类型：学位论文
【摘要】：经热解及氨浸方法回收废弃含铜催化剂中的铜,并通过蒸氨还原法制备工业级氧化亚铜。研究了升温速率、热解终温、终温保持时间和空气流量等因素对热解废弃含铜催化剂中有机物的影响;利用TG-DTG动力学分析方法,采用多重升温速率和单重升温速率结合的方法分析废弃含铜催化剂的热解动力学;对热解产生的尾气进行处理,分析了碱液比、尾气流速和吸收液温度对尾气吸收率的影响;采用氨浸方法浸出热解后的废催化剂中的铜,研究了氨浸温度、总氨浓度、氨-铵摩尔比、搅拌速率和粒径对铜浸出率的影响,并研究了氨浸过程的动力学,得到铜浸出的活化能E和反应级数n;采用蒸氨还原方法制备工业级氧化亚铜。结果表明:热解废弃含铜催化剂中有机物的最佳条件为:升温速率20℃·min-1,热解终温600℃,停留时间90min,空气流量3.0L·min-1。废催化剂热解分为四个阶段,四个阶段的活化能Eα分别为16.181k J·min-1、43.841k J?mol-1、90.561k J?mol-1、52.313k J?mol-1,指前因子A分别为4.696×109s-1、1.457×1013s-1、8.662×1012s-1、4.939×105s-1,四个反应阶段的反应机制和最概然函数分别为:化学反应控制机制,符合Reaction order方程,f(α)=(1-α)2,g(α)=(1-α)-1-1、成核与长大(n=3)控制机制,符合Avrami-Erofeev方程,f(α)=1/3(1-α)[-ln(1-α)]-2,g(α)=[-ln(1-α)]3、第三、四步均为成核与长大(n=4)控制机制,符合Avrami-Erofeev方程,f(α)=1/4(1-α)[-ln(1-α)]-3,g(α)=[-ln(1-α)]4。碱液对热解尾气的吸收最佳条件为:氨液质量比为1:2,温度为50℃,尾气流速为0.6L·min-1,尾气吸收率为99.95%。氨浸条件为40℃的氨浸温度,总氨浓度为4mol·L-1,氨-铵摩尔比为1:4,搅拌速率为300r·min-1,粒径29.43μm条件下,铜的浸出率可达98%,铜浸出的活化能E为7.59 k J·min-1,反应级数为0.6158。最终通过蒸氨还原法制的工业级氧化亚铜,按照HGT2961-2010检测,符合HGT2961-2010标准,纯度可达97%。
[Abstract]:After pyrolysis and ammonia leaching method for recovering copper containing catalysts of copper in waste, and through ammonia reduction preparation method. The study of industrial grade cuprous oxide heating rate, pyrolysis temperature, temperature holding time and air flow rate and other factors of organic compounds containing copper catalyst in the pyrolysis of waste; using TG-DTG dynamic analysis method, the multiple heating rate and single rate combined with the analysis of heating method for waste pyrolysis kinetics of copper containing catalyst; exhaust on the pyrolysis of processing, analysis of alkali ratio, gas flow rate and temperature of absorption liquid of the tail gas absorption rate influence; the ammonia waste catalyst leaching method for leaching after pyrolysis of copper ammonia leaching temperature the study of concentration of total ammonia, ammonia - ammonium molar ratio, stirring speed and the influence of particle size on the leaching rate of copper, and to study the kinetics of ammonia leaching process, the leaching of copper activation energy E and the reaction order of N obtained by ammonia also; 鍘熸柟娉曞埗澶囧伐涓氱骇姘у寲浜氶摐.缁撴灉琛ㄦ槑:鐑В搴熷純鍚摐鍌寲鍓備腑鏈夋満鐗╃殑鏈，
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