离子液体催化合成三聚甲醛动力学研究

发布时间：2018-06-15 02:39

本文选题：三聚甲醛 + 离子液体　；参考：《兰州大学》2014年硕士论文

【摘要】：三聚甲醛是一种性能优良的化工原料,广泛应用于工程塑料和其他化学品中间体。传统的方法是在酸性催化剂硫酸的作用下合成,此工艺存在着均相催化本身不可避免的缺点,如易腐蚀设备、选择性差、产物与催化剂难分离等。所以,为改善三聚甲醛生产过程效率低下、能耗较高的劣势,很多新方法被提出。到目前为止,关于三聚甲醛合成、分离技术方面的研究已经取得了很大进展。近年来,中国科学院兰州化学物理研究所开发了具有自主知识产权的离子液体催化剂合成三聚甲醛的方法。与传统技术相比,离子液体合成三聚甲醛技术是一项清洁合成技术,可减少环境污染和设备腐蚀,极大地降低投资,已完成万吨/年工业化试验。然而,有关离子液体催化此类反应的动力学过程还未见报道。此方面研究的空缺,不利于离子液体催化三聚反应的控制和工业化推广。本论文主要以多种离子液体为催化剂,对甲醛环化三聚反应的动力学过程进行了研究,通过考察催化剂结构、催化剂浓度、反应物浓度、温度和压力对产物分布的影响,建立动力学模型,获得了相关的动力学参数值,如反应速率常数Ki,活化能Ea和指前因Ai。在合成催化剂基础上,考察了甲醛羰基化反应。研究发现,在一定反应条件下反应,乙醇酸甲酯的收率达到了97.6%,催化剂和溶剂重复使用8次,反应活性未见明显下降。
[Abstract]:Triformaldehyde is a kind of chemical raw material with excellent properties, which is widely used in engineering plastics and other chemical intermediates. The traditional method is synthesis under the action of acid catalyst sulfuric acid. This process has the inevitable shortcomings of homogeneous catalysis, such as easy to corrode equipment, poor selectivity, difficult to separate the product from catalyst and so on. Therefore, many new methods have been proposed to improve the low efficiency and high energy consumption of triformaldehyde production process. Up to now, great progress has been made in the synthesis and separation of formaldehyde. In recent years, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, has developed a method for the synthesis of formaldehyde with ionic liquid catalysts with independent intellectual property rights. Compared with the traditional technology, the synthesis of triformaldehyde by ionic liquids is a clean synthesis technology, which can reduce environmental pollution and equipment corrosion, greatly reduce investment, and has completed the industrial test of ten thousand tons per year. However, the kinetics of such reactions catalyzed by ionic liquids has not been reported. The lack of research in this field is not conducive to the control of ionic liquid catalyzed trimerization and industrial popularization. In this paper, the kinetic process of cyclization trimerization of formaldehyde was studied with various ionic liquids as catalyst. The effects of catalyst structure, catalyst concentration, reactant concentration, temperature and pressure on the distribution of the product were investigated. The kinetic model was established and the related kinetic parameters such as reaction rate constant Kia activation energy EA and antecedent Aii were obtained. The carbonylation of formaldehyde was investigated on the basis of synthesis catalyst. It was found that under certain reaction conditions, the yield of methyl glycolate reached 97.6, the catalyst and solvent were reused for 8 times, and the reaction activity was not significantly decreased.
【学位授予单位】：兰州大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：TQ317;O643.1

【参考文献】