【作者】 周丽雯；

【导师】 肖文德；

【作者基本信息】 上海交通大学 ， 化学工程， 2008， 硕士

【摘要】 本文对稀酒精脱水反应体系进行了系统的研究和分析,筛选出适合本反应体系的催化剂,并利用XRD、Al MAS NMR和低温N₂吸附表征技术,考察了催化剂的结构和表面组成及其与催化性能之间的联系;对催化剂的活性和稳定性进行了全面研究,揭示了催化剂的活性和稳定性随时间变化的关系;研究了催化剂失活和再生的性能,为进一步开发抗积炭催化剂及寻找更好的催化剂再生方法奠定基础。全文内容分为以下几部分:1.筛选出了在低温下能有较高活性的催化剂,采用XRD、Al MAS NMR和低温N₂吸附表征技术对该催化剂进行了表征。结果表明,分子筛催化剂的改性并未改变催化剂的整体结构,六配位铝的存在有利于提高催化剂的稳定性。2.在固定床反应器中进行了分子筛催化剂催化稀酒精脱水生成乙烯反应的活性测试实验,催化剂经高温水蒸气处理,反应时间为1000小时。结果表明,改性后的催化剂对于稀酒精脱水反应具有良好的活性和稳定性,在反应1000小时后,乙醇转化率和乙烯选择性仍没有明显下降。3.采用XRD,低温N₂吸附,TG,IR和MAS NMR等方法对失活催化剂进行了表征,结果表明,在乙醇脱水反应中,催化剂表面积炭导致分子筛微孔堵塞是造成催化剂失活的主要原因,积炭的物种主要是带有双键的聚合态化合物（或芳香族化合物）。选择合适的温度对催化剂进行再生,实验结果表明,再生后催化剂对于稀酒精脱水制乙烯的反应具有良好的活性和稳定性。更多还原

【Abstract】 In this work, catalytic dehydration of ethanol has been studied in details. The optimum catalysts were chosen. The effects of bulk structure and surface component of catalysts on the catalytic performance were investigated. Activity and stability have been present. The performance of catalytic deactivation and regeneration has also been researched.The main contents of this paper are as follows:First, by means of XRD, Al MAS NMR, N₂-adsorption techniques, the results showed that the stability of catalyst was improved with increasing content of the octahedral aluminum.Second, activity experiments of catalyst during aqueous ethanol dehydration to ethylene were carried out in a fixed-bed reactor, the time of reaction was 1000 hours. The results showed that the catalyst had high activity and stability for aqueous ethanol dehydration.Third, by means of XRD, N₂ adsorption techniques, TG, IR and MAS NMR,the results showed that deactivation of catalyst due to the coke formed on the catalyst surface which blocked the pore mouth of zeolite channels for ethanol dehydration. Regeneration of catalyst was putted on appropriate temperature, the results indicated that the regenerated catalyst had high activity and stability for aqueous ethanol dehydration.更多还原