Anderson型杂多酸烷氧化合物催化氧化性能的应用研究

发布时间：2018-04-29 08:11

  本文选题：Anderson型杂多酸 + 烯烃环氧化　； 参考：《上海应用技术大学》2017年硕士论文

【摘要】：在最前沿和最新的文献中,催化术语通常与“绿色化学”和“可持续性”等概念密切相关,因为催化是降低许多化学工业过程的能耗和环境负担最有效的方案。选择性催化氧化反应在当前化工行业中特别重要。许多关键的化学品和中间体如醇,环氧化物,醛,酮和有机酸都是通过选择性催化氧化作用产生的。多金属氧酸盐具备很好氧化还原性质,持久的对抗氧化剂和环境兼容性。本论文是对Anderson型杂多酸烷氧化合物催化氧化性能的应用进行探究。(1)使用双边氨基共价修饰的Mn-Anderson型多金属氧酸盐作为催化剂,H2O2为氧化剂,无需自由基引发剂,对苯乙烯进行催化氧化,能够精确可控进行专一选择性生成环氧化合物或顺式—二羟基化合物。通过单因子变量的方法优化反应。经研究发现,当反应温度为50℃时,用CH3CN作为溶剂,对环氧化合物具有专一选择性,其中选择性≥99%,收率≥90%。当反应温度为70℃时,用CH3CN/H20作为溶剂,对二羟基化合物具有专一选择性,其选择性及收率均≥99%。并成功地将各种烯烃转化成相应的环氧化物和顺式二醇,具有优异的选择性和收率。(2)在水中使用单边氨基修饰的Fe-Anderson型多酸[FeMo6018(OH)3{(OCH2)3CNH2}](FeⅢMo6-NH2)作为催化剂,1 atm 氧分子作为氧化剂,催化氧化苯甲醛生成苯甲酸,其中收率和选择性均≥90%。许多种醛类已成功转化为相应的羧酸且具有优良的产率。所需反应条件温和,可在FeⅢMo6-NH2催化剂极低使用量进行,底物甚至可以扩大量到克级,其收率和选择性收率和选择性均≥90%。其操作的简单性、所需条件温和、催化剂绿色环保以及可以回收循环使用。使其在工业规模上使用的潜力。
[Abstract]:In the cutting-edge and most recent literature, catalytic terminology is often closely related to concepts such as "green chemistry" and "sustainability", as catalysis is the most effective way to reduce the energy consumption and environmental burden of many chemical industrial processes. Selective catalytic oxidation is particularly important in the chemical industry. Many key chemicals and intermediates such as alcohols epoxides aldehydes ketones and organic acids are produced by selective catalytic oxidation. Polyoxometalates have good redox properties, persistent antioxidant and environmental compatibility. In this paper, the application of Anderson type heteropolyacid alkoxy compounds in catalytic oxidation was investigated. The Mn-Anderson type polyoxometalates modified by bilateral amino groups were used as catalyst H _ 2O _ 2 as oxidant without free radical initiator. The catalytic oxidation of styrene can produce epoxy compounds or cis-dihydroxyl compounds. The response was optimized by the method of single factor variable. It was found that when the reaction temperature was 50 鈩，

本文编号：1819115