论文总字数：14802字

摘 要

TS-1是一种具有三维孔道结构的分子筛。Ti是反映的活性中心，Ti在骨架内的均匀分布形成Si-O-Ti结构使得TS-1具有特殊的性质，这使得其在具有催化氧化活性的同时兼具有择形催化性能。TS-1分子筛是一种环境友好无毒无害的催化剂，TS-1分子筛催化环己酮氨肟化是环境友好的绿色化工过程，具有条件温和、过程清洁、转化率选择性高、反应速度快优点。TS-1分子筛在烯烃的环氧化、环己酮氨氧化制环己酮肟、醇类的氧化、苯酚羟基化制邻、对苯二酚等已经取得成就。

本文研究了TS-1催化环己酮氨肟化反应过程，探究了无有机溶剂条件下TS-1催化环己酮氨肟化反应中TS-1催化剂失活的原因。考察了TS-1失活的原因及催化剂的寿命。主要方式通过FT-IR、XRD和TG对失活催化剂表征。将该工艺和已有的叔丁醇为溶剂的工艺进行比较考察叔丁醇对催化剂活性的影响。考察叔丁醇对催化剂活性的影响。反应温度为75℃，，反应时间为90min，催化剂13.7g，在此条件下考察催化剂的失活原因。

关键词：环己酮氨肟化反应 钛硅分子筛 失活

Coke deposition and characterization on titanium silicalite-1 catalystin cyclohexanone ammoximation

Abstract

TS-1 is a kind of molecular sieve with three-dimensional pore structure. Ti is a reflection of the active center, Ti in the framework of the uniform distribution of the formation of Si-O-Ti structure makes the TS-1 has a special nature, which makes it in the catalytic oxidation of the activity with a selective catalytic performance at the same time. TS-1 molecular sieve is a kind of environmentally friendly non-toxic and harmless catalysts and TS-1 molecular sieve catalytic cyclohexanone ammoximation is environment friendly green chemical process, with mild conditions, the cleaning process, conversion rate, high selectivity, fast response advantages. TS-1 molecular sieve achievement has been made in the oxidation of olefin epoxidation, ammoximation of cyclohexanone oxidation of cyclohexanone oxime, alcohols and hydroxylation of phenol preparation of catechol, hydroquinone etc..

In this paper, catalyzed by TS-1 cyclohexanone ammoximation process to explore the no reason for deactivation of TS-1 catalyst catalyzed by TS-1 cyclohexanone ammoximation reaction in organic solvents. The cause of TS-1 inactivation and the life of the catalyst were investigated. The deactivation catalysts were characterized by FT-IR, XRD and TG. The process was compared with the existing tert butyl alcohol as solvent, and the effect of tert butyl alcohol on the activity of the catalyst was investigated. The effect of tert butyl alcohol on the activity of catalyst was investigated. .The reaction temperature is 75 degrees C, reaction time is 90min, the catalyst is 13.7g. Under the conditions of the catalyst, the deactivation of the catalyst was investigated.

Keywords: Ammoximation of cyclohexanone;Titanium silicon molecular sieve;Inactivation

目录

摘要 I

Abstract II

第一章 文献综述 1

1.1引言 1

1.2环己酮肟的用途和生产概况 1

1.2.1环己酮肟的用途 1

1.2.2环己酮肟的生产概况 2

1.2.3改进的氨肟化工艺 3

1.2.4运用膜分布器改进的液相氨肟化工艺 4

1.3 TS-1催化环己酮氨肟化反应 5

1.3.1 TS-1的简介 5

1.3.2 TS-1的主要用途 5

1.3.3 TS-1分子筛的失活 6

1.3.4 TS-1的再生 7

第二章 实验方法及过程 8

2.1 实验原料及仪器 8

2.1.1 实验原料 8

2.1.2 实验仪器与设备 8

2.2 实验装置图 9

2.3实验条件 10

2.4 实验操作 10

第三章 实验结果与讨论 11

3.1 产物分析与计算方法 11

3.3 催化剂失活分析 14

3.3.1 催化剂的xrd 14

3.3.2 催化剂的FT-IR 15

3.3.3催化剂的热重 16

3.3.4 硅溶解变化 17

3.4 本章小结 17

第四章 结论与展望 18

4.1 结论 18

4.2展望 18

参考文献 19

致谢 21

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