摘 要
本文简单介绍了固体超强酸的发展、研究方向、及存在的问题。并采用沉淀－浸渍法制备SO4/ZrO2固体超强酸，分别以氧氯化锆和氨水为锆源和沉淀剂，110℃干燥后经硫酸浸渍、干燥和焙烧制得催化剂。同时考察不同焙烧温度对催化剂性能的影响。在最优的条件下用正交设计法考察锆源（Zr(NO3)4•5H2O,ZrOCl2•8H2O）、沉淀剂（氨水、乙胺）和硫酸化试剂（硫酸、硫酸铵）对催化剂性能的影响，并通过乙酸和正丁醇的酯化反应的酯化率检测所制备的SO4/ZrO2催化剂的催化效果。结果表明采用硫酸浸渍液浓度为0.5mol/L，焙烧温度为550℃时所制备的催化剂在正丁醇和乙酸的物质的量比为1.3及不添加任何带水剂的密闭条件下酯化效果最好，酯化率为52.5%。正交设计实验中锆源、沉淀剂、硫酸化试剂的极差分析结果分别为1.54%，2.27%，5.11%，此结果说明硫酸化试剂对催化剂的影响最大，其次是沉淀剂，锆源的影响最小，同时表明以Zr(NO3)4•5H2O为锆源、乙胺为沉淀剂、硫酸为硫酸化试剂是催化剂的最佳制备方案。
关键词：SO4/ZrO2 ;固体超强酸；正交实验设计；乙酸丁酯
Abstract
The development of superacid was introduced with the direction of its research and problems in this text. A solid superacid catalyst, SO42-/ZrO2,was prepared by precipitation-impregnation method.The catalysts was prepared with zirconium oxychloride as zirconia sources and aqueous ammonia as precipitant ,respectively, then drying at 110℃ ,impregnating with sulfated acid and calcinating .At the same time,the effects of the different calcination temperatures on the catalytic performance of SO42-/ZrO2 was studied.The orthogonal experimental design was applied to investigate the effects of zirconia source (Zr(NO3)4•5H2O, ZrOCl2•8H2O),precipitants (aqueous ammonia ,ethylamine) and sulfating agent (sulfuric acid, ammonium sulfate) on the catalytic performance of the catalysts unde the most superior condition .The catalytic activity was tested in esterification of acetic acid with butanol .The results show that the yield of butyl acetate using the 无忧论文 【http://www.uklunwen.com】catalysts prepared with the concentration of H2SO4 by 0.5 mol•l-1 and the calcination temperature of 550℃ is the best,which is up to 52.5% when the molar ratio of butyl alcohol to acetic acid is 1:1.3 and without addition of entrainer in the hermetic reactor. In the orthogonal designable experiment ,the analysis results of zirconium source, precipitation , the sulfating agent is 1.54%, 2.27%, 5.11% ,respectively. This result show that the influence of sulfating agent to the catalytic activity is the biggest. Under the same density of the sulfuric acid soaks, the effect of sulfuric acid is well compared to ammonium sulfate .The second is the precipitation, but the influence of the zirconia source is the smallest.
Key words: SO4/ZrO2 ;Solid superacid ; Orthogonal experimental designt;
Butyl acetate
目 录
1．前言
1．1 固体超强酸催化剂的发展前景
1．2 固体超强酸目前存在的问题
1．3 固体超强酸的研究方向
1．4 本课题的研究意义及方案
2．实验理论
2．1固体超强酸的酸度定义
2．2固体超强酸的合成方法
2．3催化剂合成原理
2．4催化剂酸性中心结构
2．5酸性中心形成机理
2．6催化剂失活机理
2．7催化剂酯化反应机理
2．8酯化反应原理
3．实验部分
3．1 主要仪器与设备
3．1．1主要仪器
3．1．2主要设备
3．2主要试剂与配制
3．2．1主要试剂
3．2．2主要试剂配制
3．3实验内容
3．3．1催化剂的制备
3．3．2酯化反应
3．3．4酯化率的测定
3．4正交实验设计
3．4．1正交实验设计概念
3．4．2本实验正交设计方案
3．4．3实验步骤
3．5对比实验
4．结果与讨论
4．1 焙烧温度对催化剂的影响
4．2 正交设计实验结果
4．2．1正交实验结果分析步骤
4．2．2正交实验表的分析结果
4．3沉淀剂对催化剂的影响
4．4硫酸化试剂对催化剂的影响
4．5对比实验结果讨论
4．6实验中存在的问题讨论
5．结论
6．参考文献
7．谢辞
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