相转移催化体系和离子液体催化体系下苯乙烯氧化反应工艺的研究
赵明泽
学位类型硕士
导师吾满江•艾力
2008-06-09
学位授予单位中国科学院研究生院
学位授予地点北京
学位专业有机化学
关键词苯乙烯 过氧化氢 氧化 相转移 离子液体
摘要

苯乙烯的氧化产物是重要的化工原料和中间体,应用非常广泛。但由于传统的合成方法合成难度较大,合成反应收率低、成本高,使其难以满足市场供给要求。因此,近年来人们正寻求研究和开发新的合成方法和途径来解决这一问题。研究苯乙烯的氧化反应分别采用了三种可回收催化体系:钼-铵相转移催化体系、离子液体催化体系、杂多酸-离子液体催化体系,以双氧水为氧化剂催化氧化苯乙烯,生成中间产物环氧苯乙烷,在催化剂催化下同时伴随着环氧苯乙烷的开环反应,生成苯甲醛和苯基乙二醇等产物。本论文研究了常压下催化剂用量、氧化剂用量、相转移剂用量、体系酸度、反应温度以及反应时间对苯乙烯氧化反应和产物选择性的影响,找出了该体系的最佳条件。钼-铵相转移催化体系作用下的单程转化率基于苯乙烯计算可达到28.44%;在55℃、二氯甲烷为溶剂、双氧水浓度为12%时反应生成苯甲醛的选择性为100%。离子液体催化体系以15%的H2O2 为氧化剂,单程转化率可达到20.1%;不同阳离子功能化的离子液体对反应的作用效果不同,引入磺酸基的功能化离子液体的催化活性较高,而未功能化的离子液体催化体系可以生成单一产物苯甲醛,单程转化率为10%;离子液体可以提高协同使用的其它催化剂的活性,同时可取代有机试剂作为溶剂,这使得反应后的分离变得非常容易。通过对平衡反应的研究,得到了不同参量对三种产物选择性的影响,工业上可以通过精馏分离,得到纯净的三种有机物。

其他摘要

The productions of styrene oxidation are very important chemical raw material and intermediate used over a wide range of field. However, because the traditional method of styrene oxidation is difficult, low yield, high cost and its output can not meet the needs of the developing market. the new methods to solve the problems have recently been focused on. Three different catalyst systems were studied on styrene oxidation, such as Mo-NH4+ phase transfer catalyst system, ionic liquid catalyst system, heteropoly acid – ionic liquid catalyst system. By using aqueous H2O2 as oxidant, Oxidation of styrene converted to styrene oxide and benzaldehyde. Following with the reaction, phenyl glycol could be obtained from styrene oxide which is the important fine chemical intermediate. The discourse sets out the effect of catalyst quantity、concentration of hydrogen peroxide、pH、reaction temperature and time on the conversion of styrene and the selectivity of products, the best technics parameter for products is found out. the conversion is 28.44%(based on styrene) under the Mo-NH4+ catalyst system, especially at 55℃ the selectivity for benzaldehyde is 100% by using 12% H2O2. With the ionic liquid(IL) catalyst system ,oxidation of styrene with 15% aqueous H2O2 converted to benzaldehyde, phenyl glycol at 55℃,the convertion is reached 20.1%. Different catalyst and solvent conditions were discussed and compared , the catalyst activity is higher with the SO3H functional IL and the single product benzaldehyde is converted 10% with the non-functional [BMIm]+ IL.The results demonstrated that IL also improved the effect of cooperating-catalyst. As solvent, the IL which was instead of organic reagent could improve the separation more effective among the products and reactant. By studying the balanced reaction, it was found that effects of various parameters for three production is obvious.The pure productions can be obtained by rectify in industry.

文献类型学位论文
条目标识符http://ir.xjipc.cas.cn/handle/365002/3536
专题新疆维吾尔自治区精细化工工程技术研究中心
作者单位中国科学院新疆理化技术研究所
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赵明泽. 相转移催化体系和离子液体催化体系下苯乙烯氧化反应工艺的研究[D]. 北京. 中国科学院研究生院,2008.
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