摘 要:环己酮是比较重要的化工原料，它是制造尼龙和已二酸以及己内酰胺的重要的中间体。同时在工业上的主要的作用是被用作有机原料和溶剂。主要被用于制造已内酰胺和已二酸。另外，通过环己酮作为有机合成的原料，还可以制得药物如咳美切的中间体，即环己烯乙胺。即在药物的制备中广泛运用于被作为中间体，市场潜力也是比较巨大的。在前人的研究基础上可以知道，金属纳米粒子可以在氧化化学反应中对化学反应进行催化的作用。但是由于它的性能不是很稳定,所以不容易被合成制备相对可以均匀分布同时又可以稳定的存在。研究结果也表明，分子筛材料SBA-15，因为它的比表面较大,同时它的孔道构造比较好,所以可以利用金属纳米粒子规则的纳米空间的限域作用来合成制备可控的粒径。本论文旨将制备合成金属Pd纳米粒子限域于SBA-15孔道内的,然后在氮气的氛围下，即在无氧的情况下，然后利用实验得到的金属Pd多相催化剂进行对醇的选择氧化反应。通过在SBA-15上氨基化，并将过渡金属（例如钯、铜等）负载于其上，以来对醇进行一级氧化反应。本文采用以环己醇为原料，以氯化钯作为催化剂并将其负载在SBA-15上，通过脱氢氧化反应，得到最终的产物环己酮。在本文也研究了各个反应的条件，探讨最佳的反应条件。本文研究了催化环己醇制备环己酮的反应时间、反应温度、催化剂使用量、催化剂循环使用次数、溶剂中水醇比对催化性能的影响，其最佳反应时间是7h、80℃、20-40mg，另外催化剂循环使用次数、溶剂中水醇比对催化性能的影响较小可以忽略。在环己醇氧化转化实验中所用的杂化催化剂表现出较高的活性。该催化剂也可以对多种醇进行选择性氧化反应,最终生成与参加反应的醇所相对应的羰基化合物。77933

毕业论文关键词：Pd纳米粒子；嫁接法；SBA-15；醇的选择氧化反应

Study on Preparation and Alcohol Oxidation of Hybrid Catalytic Materials

Abstract：Cyclohexanone is a relatively important chemical raw material, it is the manufacture of nylon and adipic acid and caprolactam important intermediates。 At the same time the main role in industry is to be used as organic raw materials and solvents。 Mainly used in the manufacture of caprolactam and adipic acid。 In addition, through the cyclohexanone as organic synthesis of raw materials, can also be prepared as a catecrime cut intermediates, namely cyclohexene ethylamine。 That is widely used in the preparation of drugs used as an intermediate, the market potential is relatively large。 Based on previous studies, it can be seen that metal nanoparticles can catalyze the chemical reactions in oxidative chemical reactions。 But because of its performance is not very stable, it is not easy to be prepared by the relative distribution can be evenly distributed at the same time can be stable。 The results also show that the molecular sieve material SBA-15, because of its larger surface area, while its pore structure is better, so you can use the metal nanoparticles of the regular nano-space limiting role in the synthesis of controlled particle size。 In this paper, it is proposed to prepare the metal Pd nanoparticles in the SBA-15 pore domain, and then in the nitrogen atmosphere, that is, in the case of oxygen, and then use the experimental results of the metal Pd heterogeneous catalyst for the choice of alcohol Oxidation reaction。 The primary oxidation of the alcohol is carried out by amination on SBA-15 and loading the transition metal (e。g。, palladium, copper, etc。) thereon。 In this paper, cyclohexanol was used as raw material, palladium chloride as catalyst and supported on SBA-15, and the final product cyclohexanone was obtained by dehydrogenation reaction。 In this paper, the conditions of each reaction were also studied, and the optimum reaction conditions were discussed。 In this paper, the reaction time, the reaction temperature, the amount of catalyst used, the number of times of catalyst cycling and the ratio of water to alcohol in the catalyst were studied。 The optimum reaction time was 7h, 80 ℃, 20 -40mg, in addition to the number of times the catalyst used, the solvent in the water and alcohol than the catalytic performance of the smaller can be ignored。 The hybrid catalyst used in the cyclohexanol oxidation conversion experiment showed high activity。 The catalyst may also undergo selective oxidation of a plurality of alcohols to ultimately produce a carbonyl compound corresponding to the alcohol to which it is reacted。