QIBEBT-IR  > 热化学转化研究组
一步法合成二甲醚整体式催化剂的制备及反应性能研究
李超
导师杨成
2010-05
学位授予单位中国科学院研究生院
学位授予地点北京
学位专业热能工程
关键词二甲醚 一步法合成 整体式催化剂 协同作用 比较研究
其他摘要二甲醚是一种用途广泛的化工原料和清洁燃料,从煤/含碳生物质经合成气制二甲醚是现代煤化工和生物质化工发展的重要方向之一。目前,合成二甲醚的工艺主要分为一步法和两步法。合成气一步法合成二甲醚打破了反应体系中存在的热力学平衡限制,相比经甲醇脱水的两步法工艺更具应用前景。为进一步提高工艺过程的经济性,降低二甲醚生产成本,推进其产业化进程,迫切需要开发出高活性、高选择性和稳定性的催化剂以及传热传质效果良好的高性能反应器。本文以蜂窝陶瓷为整体式载体、γ-Al2O3为惰性涂层,引入传统合成二甲醚双功能复合催化剂活性组分(C301/HZSM-5 NC207/SO42--γ-Al2O3)制备出一步法合成二甲醚整体式催化剂,采用XRDBETSEM等手段表征催化剂的结构和织构特性,并且分别与C301/HZSM-5 NC201/SO42--γ-Al2O3颗粒状催化剂进行比较研究。本论文工作的主要内容包括:1)针对一步法合成二甲醚催化剂的物理及化学方面的特点,选取适宜的制备方法,对一步法合成二甲醚整体式催化剂的制备工艺进行研究。2)采用优化的制备方法,以一步法合成二甲醚整体式催化剂制备工艺研究结果为基础,以C301/HZSM-5 NC207/SO42--γ-Al2O3 为活性组分,分别制备出C301/HZSM-5/蜂窝陶瓷整体式催化剂和NC207/SO42--γ-Al2O3/蜂窝陶瓷整体式催化剂。3)在固定床反应器中考察了两种不同的整体式催化剂上CO加氢一步法合成二甲醚的反应性能,并分别与C301/HZSM-5 颗粒催化剂和NC207/SO42--γ-Al2O3颗粒催化剂进行比较研究。4)催化剂的 XRDBETSEM 表征,对整体式催化剂的结构和织构特性进行了初步研究。5)对C301/HZSM-5/蜂窝陶瓷整体式催化剂和NC207/SO42--γ-Al2O3/蜂窝陶瓷整体式催化剂的反应性能进行对比研究。本论文工作表明整体式催化剂作为一种多功能结构化催化剂应用于一步法合成二甲醚具有优良的反应性能。研究发现催化剂的结构特性和活性组分的协同作用对 CO 加氢反应的活性、选择性和稳定性都产生重要的影响,为该类型的催化剂在二甲醚合成中的应用奠定了一定的理论和技术基础。; Dimethyl ether (DME) is widely used as chemical feedstocks or clean fuels. DME synthesis from coal or carbonaceous biomass via syngas is an important direction of modern coal chemical industry and biomass chemical industry. At present, it’s known that there are two methods for DME from syngas, i.e. two-step method and one-step method. Comparing to two-step method which pass by methanol dehydration, one-step method has more prospects because it breaks the thermodynamic equilibrium restriction of the reaction system. To further enhance the economy of the process, reduce the cost of DME production and promote the industrialization process, it urgently needs to develop a catalyst with high activity, high selectivity and stability and a good performance reactor with favorable heat and mass transfer.In this paper, two different monolith catalysts has been prepared by γ-Al2O3 coating honeycomb ceramic supported C301/HZSM-5 and NC207/SO42--γ-Al2O3, respectively, which are active components of the traditional bifunctional catalyst for DME synthesis. The structural and textural properties of the prepared catalysts has been characterized by SEM, XRD and BET methods. Furthermore a comparable study of these two monolithic catalysts and corresponding particle catalysts for one step synthesis of dimethyl ether from CO hydrogenation was carried out in a fixed-bed reactor. Additionally, we compared the catalytic performance of the two different monolithic catalysts.The main contents of our work as follows:(1) In view of special physical and chemical characteristics of the catalysts for direct synthesis of DME, we chose a suitable preparation method and then studied the preparation technology of the monolith catalyst.(2)Using the optimized preparation method and based on the result of the preparation technology research, two different monolith catalysts for dimethyl ether synthesis were prepared with C301/HZSM-5 and NC207/ SO42--γ-Al2O3 as the active component.(3) The catalytic performance of the monolith catalysts and the particle catalysts for one step synthesis of dimethyl ether from syngas was studied and compared in a fix bed reactor.(4) The prepared catalysts were characterized by XRDBET and SEM, and the structural and textural properties of the monolith catalyst were investigated.(5) A comparative study between C301/HZSM-5 monolithic catalyst and NC207/SO42-- γ-Al2O3 monolithic catalyst for the catalytic performance of onestep synthesis of DME was carried out.In summury, monolithic catalyst as a kind of multifunctional structure catalyst showed good performance for the synthesis of dimethyl ether. It was found that the synergestic effect between the structure and active component of the monolith catalyst played an important role for the activity, selectiviy and stability of CO hydrogenation reaction, which laid a theoretical and technical basis for the application of this type of catalyst within DME synthesis reaction.
作者部门热化学转化团队
学科领域热化学转化
公开日期2011-08-30
学位类型硕士
语种中文
文献类型学位论文
条目标识符http://ir.qibebt.ac.cn/handle/337004/334
专题热化学转化研究组
推荐引用方式
GB/T 7714
李超. 一步法合成二甲醚整体式催化剂的制备及反应性能研究[D]. 北京. 中国科学院研究生院,2010.
条目包含的文件
文件名称/大小 文献类型 版本类型 开放类型 使用许可
一步法合成二甲醚整体式催化剂的制备及反应(1356KB)学位论文 暂不开放CC0请求全文
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[李超]的文章
百度学术
百度学术中相似的文章
[李超]的文章
必应学术
必应学术中相似的文章
[李超]的文章
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。