【作者】 洪春；

【导师】 李勇；

【作者基本信息】 浙江大学 ， 化学工程， 2006， 硕士

【摘要】 本文对2-氰基吡嗪及其衍生物在医药、农药、香料等领域的应用进行了介绍,接着对2-氰基吡嗪研发态势、市场前景及研发意义进行了论述,并综述了2-氰基吡嗪及其原料2-甲基吡嗪的文献合成方法,确定2-甲基吡嗪氨氧化合成2-氰基吡嗪是目前最为先进、最有经济效益的路线。接着查阅了氨氧化类及选择性氧化类催化剂,确定以VPO型催化剂为2-甲基吡嗪氨氧化合成2-氰基吡嗪的催化剂。 研究了2-甲基吡嗪氨氧化合成2-氰基吡嗪催化机理,根据集团结构适应理论来配置催化剂,根据机理及影响VPO型催化剂的各个因素分别配制不同的催化剂,研究了还原剂、载体、P/V摩尔比及助剂钾（K）、铬（Gr）、钼（Mo）对催化剂性能的影响。配制各种催化剂,其中VPO型催化剂,V/P摩尔比为1.4,以涂Mo的活性氧化铝（Al₂O₃）为载体,通过实验考察了反应温度、氧气、氨气、空速及2-甲基吡嗪进料浓度的影响,得到其最优反应条件是:温度380℃,进料摩尔比为2-甲基吡嗪:水:氧气:氨气为1:7.8:8:8,空速为0.2h^-1时,选择性达到92%,收率达到85%,并连续120h实验验证催化剂稳定性能良好;另外GrVPO催化剂,在温度为360℃,进料摩尔比为2-甲基吡嗪:水:氧气:氨气为1:6:8:6,空速为0.2h^-1时,选择率达到89.36%,收率达到80.65%;另外我们在以MoVPO为催化剂的实验中发现在低温时,酰胺吡嗪是主要生成物,这可以用我们推断的机理来解释,也间接验证了机理的合理性。 考虑到固定床工业化面临的问题,设计了循环床提升管反应器,更多还原

【Abstract】 The applications of 2-cyanopyrazine and its derivatives in pharmaceutical, agricultural chemicals and spices were introduced. And then the research situation, market foreground and research purpose were discussed.2-Cyanopyrazine prepared from 2-methylpyrazine by ammoxidation is the most advanced way after all datas about synthesis about 2-cyanopyrazine and 2-methylpyrazine refered.The VPO catalyst was choosen for the ammoxidation reaction.The mechanism of 2-cyanopyrazine prepared from 2-methylpyrazine by catalytic ammoxidation was studied and explained with the theory of appropriate structure of group. Factors effecting the performance of VPO catalyst such as reducer, molar ratio of P and V, catalyst promoters like phosphorus（P） , chrome（Gr）, kalium（K）, molybdenum（Mo） and the supports of catalyst were investigated through experiments. The VPO catalyst with 1.4 molar ratio of P/V, and with activated alumina（Al₂O₃） with MoO₃ as support prepared by impregnation method has good performance both in activity and selectivity. Reaction factors such as reaction temperature, space velocity, feed composition and the service life of catalyst were investigated. 0.2 h^-1 of the space velocity , 380℃ of the reaction temperature and 1:7.8:8:8 molar ratio of 2-MP,water, oxygen and ammonia are optimum reaction condition ,and the selectivity could reach 92% and the yield could reach 85%. GrVPO catalyst also hasgood performance with 0.8:1.4:1 molar ratio of Gr ,V and P and with activated alumina as support. When 0.2h^-1 of the space velocity , 360℃ of the reaction temperature and 1:6:8:6 molar ratio of 2-MP,water, oxygen and ammonia, the selectivity could reach 89.36% and the yield could reach 80.65 % . Amidopyrazine was the main production in the experiments with MoVPO as catalyst which could be explained by the mechanism we have supposed.The circulated bed with reactor riser was designed to solve the problems of the reaction in fixed bed.The reaction in fixed bed will emit a lot quantity of heat in industrialization which is disadvantageous and easy to explode. The selectivity and conversion could be both enhanced in the circulated bed with reactor riser which could not be achieved in the fixed bed.更多还原