Au催化剂论文：负载型Au催化剂的制备及其在肉桂醛选择性加氢反应中的应用研究.doc

Au催化剂论文：负载型Au催化剂的制备及其在肉桂醛选择性加氢反应中的应用研究【中文摘要】负载型纳米Au催化剂在许多化合物的【英文摘要】Supported gold catalysts are a kind of promising catalysts for selective hydrogenation based on their good activity and selectivity for the reduction of many compounds.In this paper, using several metal oxides doped TiO2 as supports, which were prepared by the sol-gel method, a series of gold catalysts were prepared by the deposition-precipitation （DP） method. Additionally, a series of Au/La（OH）3 catalysts were prepared by cocipitation （CP） method. All the catalyst were tested in cinnamaldehyde hydrogenation. Their phisico-chemical properties were investigated by XRD, TEM, XPS, BET and TPR techniques. The reaction conditions of cinnamaldehyde selective hydrogenation were optimized.The results show that the performance of Au/TiO2 catalyst is influenced by the type and the content of additives. Among the metal oxide promoters tested, La2O3 modified Au/TiO2 shows the best selectivity for the reduction of carbon-carbon double bond in cinnamaldehyde. The moderate amount of La2O3（10 wt%） can obviously improve the catalytic activity and selectivity of Au/TiO2 for cinnamaldehyde hydrogenation. The presence of La2O3 in TiO2 restrains the growth of TiO2 crystallites, increases the surface area of catalysts and makes the particle size distribution of Au crystallites more evenly. The gold on the surface of Au/TiO2 exists mainly as Au0, but on the La2O3 doped catalyst there is a small portion of Au3+ species besides Au0, which may benefit the activation of the C=O bond of cinnamaldehyde.The results show that La（OH）3 supported gold catalyst shows high selectivity for the reduction of carbon-carbon double bond. With the characterization results, the reason of the high selectivity is that the supporter La（OH）3 and Au interact to form a unique structure. The preparation conditions of Au/La（OH）3 catalyst are optimized as follows: 2 wt% of gold content, calcination temperature 100C and reduction temperature 150C.The reaction conditions of cinnamaldehyde selective hydrogenation over Au/La（OH）3 catalyst are optimized as follows: reaction temperature 180C, reaction pressure 2.0 MPa, catalyst dosage 0.25 g, solvent isopropanol. Under the optimal conditions, the conversion of cinnamaldehyde and the selectivity to cinnamyl alcohol can reach 100% and 75.7%, respectively, after reaction 22 h.【关键词】Au催化剂 助剂 La（OH）3 选择性加氢 肉桂醛 肉桂醇【英文关键词】gold catalyst promoter La（OH）3 selective hydrogenation cinnamaldethyde cinnamyl alcohol【目录】负载型Au催化剂的制备及其在肉桂醛选择性加氢反应中的应用研究摘要4-6ABSTRACT6-7第一章 文献综述11-301.1 肉桂醛催化加氢合成肉桂醇的研究进展11-201.1.1 肉桂醇的用途111.1.2 肉桂醇的合成方法11-131.1.3 非贵金属催化剂在肉桂醛选择性加氢中的应用进展13-161.1.4 贵金属催化剂在肉桂醛选择性加氢中的应用进展16-201.2 纳米Au 催化剂的研究进展20-281.2.1 负载型Au 催化剂的制备20-221.2.2 负载型纳米Au 催化剂性能的影响因素22-251.2.3 Au 催化剂在液相加氢中的应用25-281.3 立题依据及主要研究内容28-301.3.1 论文立题依据和意义28-291.3.2 论文主要研究内容29-30第二章 实验部分30-362.1 试剂与主要仪器30-312.1.1 主要试剂30-312.1.2 主要仪器及设备312.2 实验方案与步骤31-322.2.1 实验方案312.2.2 实验步骤31-322.3 催化剂的制备32-332.3.1 Au/M_xO_yTi0_2 催化剂的制备32-332.3.2 Au/La(OH)_3 催化剂的制备332.4 催化剂的活性评价33-342.4.1 实验方法332.4.2 产物分析33-342.5 催化剂的表征34-362.5.1 X 射线衍射(XRD)342.5.2 比表面和孔结构的测定(BET)342.5.3 元素分析(STEM-EDX)342.5.4 高分辨透射电镜(HRTEM)34-352.5.5 X 射线光电子能谱仪(XPS)352.5.6 程序升温还原(H_2-TPR)35-36第三章 助剂对Au/Ti0_2催化剂加氢性能的影响研究36-533.1 前言363.2 助剂对Au/Ti0_2 催化性能的影响36-393.2.1 助剂种类的影响36-373.2.2 助剂添加方式的影响37-383.2.3 助剂添加量的影响38-393.3 助剂La_20_3 对Au/Ti0_2 催化性能的影响39-513.3.1 助剂La_20_3 添加量对Au/Ti0_2 性能的影响39-483.3.2 焙烧温度对Au/10%La_20_3-Ti0_2 催化剂加氢性能的影响48-493.3.3 还原温度对Au/10%La_20_3-Ti0_2 催化剂加氢性能的影响49-503.3.4 还原时间对Au/10%La_20_3-Ti0_2 催化剂加氢性能的影响50-513.4 本章小结51-53第四章 纳米Au/La(OH)_3催化剂加氢性能的研究53-684.1 前言534.2 载体种类对Au 催化剂性能的影响53-564.2.1 载体种类对Au 催化剂加氢性能的影响53-544.2.2 不同载体负载的Au 催化剂的表征54-564.3 Au/La(OH)_3 催化剂上肉桂醛选择性加氢反应研究56-674.3.1 Au 负载量对Au/La(OH)_3 催化剂加氢性能的影响56-574.3.2 焙烧温度对Au/La(OH)_3 催化剂加氢性能的影响57-634.3.3 还原温度对Au/