【作者】 黄刚；

【导师】 刘平乐；

【作者基本信息】 湘潭大学 ， 化学工程， 2013， 硕士

【摘要】 1,5-二氨基萘是一种非要重要的化工原材料和中间体，可广泛用于材料化工和生物医药等行业。其最重要的用途之一是用于合成1,5-萘二异氰酸酯，进而合成NDI基聚氨酯弹性体。NDI基聚氨酯弹性体材料由于其具有特殊的物理性能，可满足高温、高油脂、高磨损等特殊工况条件的要求，有着广泛的应用前景。本文围绕1,5-二硝基萘加氢制备1,5-二氨基萘进行研究，探讨了不同催化体系对反应过程的影响。本文采用高效液相色谱法测定1,5-二硝基萘及其加氢产物1,5-二氨基萘的含量，通过优化分析条件，各物质分离效果良好，检测结果的准确度高。本文首先使用5%Pd/C催化剂对其催化1,5-二硝基萘加氢过程进行了优化，采用单因素实验，分别考察了反应温度、反应时间、反应压力对1，5-二硝基萘加氢过程的影响。得到的最优工艺条件如下：反应温度80℃，反应时间4h，氢气压力0.8MPa。此时，原料1,5-二硝基萘完全转化，1,5-二氨基萘的选择性可以达到93.12%。此外，还考察了5%Pd/C催化剂的循环使用性能，催化剂一共进行了五轮循环利用。发现随着循环次数的增多，催化剂的催化活性会随之出现较小幅度下降，循环使用第六次时，1,5-二氨基萘选择性下降4.82%。在本文的研究工作中，制备了碳纳米管负载非贵金属镍催化剂，考察了不同溶剂、不同金属负载量以及不同载体对反应过程的影响：结果表明在使用苯胺作为溶剂时，反应效果最好；25%的Ni负载在MWCNTs-2这种型号碳纳米管上制备的催化剂具有更好的催化活性。本文选用不同型号碳纳米管作为载体，制备了不同型号Ni/CNTs催化剂，并对制备的催化剂进行氮气吸附-脱附、XRD、BET、SEM和氢气化学吸附表征分析。结果表明这5种催化剂均具有介孔结构，25%Ni/MWCNTs-2催化剂由于其具备良好的结构，且负载在其表面的Ni粒子形状更为规则，分散度更高，因此该催化剂具有更好的催化效果。本文对25%Ni/MWCNTs-2催化1,5-二硝基萘加氢过程进行了研究，并对反应的工艺条件进行了优化,采用单因素实验，得到的最优工艺条件如下：反应时间5h，反应温度120℃，氢气压力1.0MPa。此时，1,5-二硝基萘的转化率为100%，1,5-二氨基萘的选择性可以达到90.4%。更多还原

【Abstract】 1,5-diaminonaphthalene is an useful chemistry raw material and intermediatewhich is widely used in the material chemistry and biopharmaceutical industry. Oneof the most useful application is to produce1,5-naphthalene(NDI),which is an keyraw material in the synthesis of NDI polyurethane. NDI polyurethane with excellentphysical performance characteristics can used in high temperature, high grease andhigh mechanical wear occasion, which has an extensive application and wideforeground. This article focus on the effects of different catalyst systems on the1,5-dinitronaphthalene hydrogenation to1,5-diaminonaphthalene.In this study, A high performance liquid chromatographic method wasestablished for analysis of1,5-dinitronaphthalene and1,5-diaminonaphthalene. By theoptimization of analysis conditions, each substance can be separated and which has anprecise detection results.Firstly, The reaction condition for hydrogenation of1,5-dinitronaphthalene using5%Pd/C as catalyst was investigated, and we have investigated different reactiontemperature, reaction time and reaction pressure on hydrogenation of1,5-dinitronaphthalene. The optimum conditions were as follows: when the reactiontemperature was80℃, the reaction time was4h and the reaction pressure was0.8MPa, the reaction can get a better effect.1,5-dinitronaphthalene could beconverted completely and the selectivity of1,5-diaminonaphthalene was93.12%.Moreover, the recycle properties of5%Pd/C catalyst for hydrogenation of1,5-dinitronaphthalene was investigated. The results indicated that the activity of5%Pd/C would have a bit decrease with the increase of cycling times. When thecatalyst was reused for10times, the selectivity of1,5-diaminonaphthalene descended4.82%.we have preliminarily investigated the influences of different solvents, differentmetal loading and different supports on hydrogenation of1,5-DNN. The results showthat using aniline as solvent,the reaction can get a better effect. It was found that25%loading of Ni supported on MWCNTs-2catalyst have better catalytic activity onhydrogenation of1,5-dinitronaphthalene.Ni/CNTs catalysts were prepared with different types of carbon nanotubes andcharacterized by N2adsorption-desorption, XRD, BET, SEM and H2chemisorption.The results showed five Ni/CNTs catalysts were mesoporous in carbon nanotubes support.25%Ni/MWCNTs-2catalyst have the best catalytic performance onhydrogenation of1,5-dinitronaphthalene, because on the one hand it have an bettercatalyst structure, on the other hand the active component Ni which load on thesurface of the catalyst have more regular particle size and dispersion.the catalytic performance of25%Ni/MWCNTs-2was investigated onhydrogenation of1,5-dinitronaphthalene. The optimum reaction conditions wereobtained, when the reaction temperature was120℃, the reaction time was5h, thereaction pressure was1.0MPa,1,5-dinitronaphthalene could be convertedcompletely and the selectivity of1,5-diaminonaphthalene was90.4%.更多还原