论文总字数：25502字

摘 要

苯胺对我们的生产生活各领域都发挥着重大的作用, 苯胺在染料、农药、医药、橡胶助剂及异氰酸酯的生产仍有很大的需求，有待进一步地寻找更为能大量简便的生产技术，并且一些合成苯胺的方法仍然存在很多不足之处，需要进一步完善。至今，苯胺的应用领域仍在不断扩大，合成苯胺的原料和方法也很多。如何开发经济、方便、污染小的合成方法以及开发苯胺新的应用领域是当前化学工作者面临的一个巨大的挑战。本文通过研究，对一步胺化的几种方法的催化剂及条件进行改进优化改进，使其能更好地在工业方面起作用。

本论文通过改变催化剂种类，反应温度、时间，反应底物等不同方法，以采用高效液相色谱（HPLC）为检测手段，研究不同反应条件下苯胺的产率。主要工作包括以下方面:

（1）相同条件下，分别以石墨烯负载Cu和以石墨烯负载Fe作为催化剂，改变反应温度，采用高效液相色谱（HPLC）检测反应情况，从而来研究得出两个结论。首先，石墨烯负载Cu作催化剂的效果比Fe要好，前者在苯的转化率（0.079％）和苯胺的选择性（51.22％）上都比后者（分别为0.041％和47.14％）要有较为明显的优势。其次，选用Gra-Cu作为催化剂，且其他条件相同时，在45^oC时的效果最佳，苯的转化率（0.079％）和苯胺的选择性（51.22％）最高。

（2）相同条件下，即在最适温度，最佳催化剂条件下，改变反应底物，以苯、对二氯苯和氯苯为例，采用高效液相色谱（HPLC）检测反应情况，从而得出如下结论，即随着活性基团氯基的引入，促进了氨化反应的进行，氯苯的转化率提高至0.11%，对氯苯胺选择性达到51.38%，1,4-二氯苯表现出最佳的反应活性，转化率达到0.126%，选择性达到54.66%。

关键字:苯胺 催化剂 石墨烯负载Cu 石墨烯负载Fe

Abstract

Aniline production in various fields for our life are playing an important role, in aniline dyes, pesticide, medicine, rubber additives and isocyanate production still have a large demand, further to find the larger number of simple production technology, the synthesis methods of aniline and some still exist many shortcomings, need further perfect. To date, the application field of aniline continues to expand, materials and methods of the synthesis of aniline is very much also. How to develop economic, convenient, low pollution of synthesis methods and new applications development of aniline make the current chemical workers face a huge challenge. Based on the research, several methods of step amination catalysts and conditions need to be improve to develop the optimization improvement, to make it better and able to play a role in industry.

In this paper by changing the types of catalyst, reaction temperature, reaction time, reaction substrate and by using high performance liquid chromatography (HPLC) for the detection means, to research under different reaction conditions the yield of aniline. Main work includes the following aspects:

(1) Under the same conditions, respectively by Gra-Cu and Gra-Fe as a catalyst to change the reaction temperature, using high performance liquid chromatography (HPLC) reaction conditions, to study two conclusions. First of all, Gra-Cu as the effect of the catalyst is better than that of Gra-Fe, the former in benzene conversion rate (0.079%) and selectivity (51.22%) of aniline (0.041% and 47.14%, respectively) than the latter have more obvious advantages. Secondly, choose Gra-Cu as catalyst, and other things being equal, the best results when 45^oC, benzene conversion rate (0.079%) and selectivity (51.22%), the highest of aniline.

(2) Under the same conditions, namely, the optimum temperature, the best catalyst under the condition of changing reaction substrate, with benzene, 1,4-dichlorobenzene, and chlorobenzene, for example, by high performance liquid chromatography (HPLC) reaction, thus conclude that with the introduction of reactive chlorine base, namely to promote the ammoniation reaction of chlorobenzene conversion rate up to 0.11%, selectivity of chloroaniline reached 51.38%, 1,4-dichlorobenzene showed the best reactivity, conversion rate reached 0.126%, the selectivity of 54.66%.

Keywords: Aniline ; Catalyst ; Gra-Cu ; Gra-Fe

目录

摘要 I

Abstract II

第一章 文献综述 1

1.1引言 1

1.2苯胺的供需 1

1.2.1世界苯胺的供需情况 1

1.2.2我国苯胺的供需情况 3

1.3传统苯胺合成方法优缺点 5

1.3.1硝基苯铁粉还原法 5

1.3.2硝基苯催化加氢法 5

1.3.3苯酚、卤代苯胺化法 7

1.4直接氨化法合成苯胺 8

1.4.1氨水作为胺化试剂 8

1.4.2以羟胺为胺化剂 8

1.4.3以氨气为胺化试剂 8

1.4.3.1无氧化剂 8

1.4.3.2以晶格氧为氧化剂 10

1.5研究的目的、内容和意义 10

第二章 催化剂、温度对苯的直接催化胺化影响 12

2.1引言 12

2.2 实验仪器与药品 13

2.2.1实验仪器 13

2.2.2 实验药品 13

2.3实验过程 14

2.4产物分析 14

2.5计算方法 14

2.6结论与讨论 14

2.6.1不同的催化剂对苯直接氨化的影响 14

2.6.2反应温度对苯直接胺化的影响 15

2.7本章小结 18

第三章 不同底物的直接催化胺化反应 19

3.1引言 19

3.2实验仪器和药品 19

3.3.1仪器 19

3.3.2药品 19

3.3实验过程 20

3.4产物分析 20

3.5计算方法 20

3.6结果与讨论 20

3.6.1可能的反应机理 21

3.7本章小结 22

第四章、结论与展望 23

4.1结论 23

4.2展望 23

参考文献 24

致谢 28

第一章 文献综述

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