五元环碳酸酯的合成及其在润滑油领域的应用
罗燕平
学位类型硕士
导师侯震山 ; 吾满江.艾力
2013-06-01
学位授予单位中国科学院大学
学位授予地点北京
学位专业材料物理与化学
关键词二氧化碳 环氧丙烷 碳酸丙烯酯 生物基碳酸酯 多相催化剂
其他摘要

本文以环氧丙烷、环氧棉籽油与CO2加成反应制备五元环碳酸酯,实现温室气体CO2的化学固定的同时得到了具有重要工业应用价值的碳酸丙烯酯和生物基润滑材料棉籽油碳酸酯。本文主要包括以下内容:

以碱金属卤化物KI为主催化剂,卤化锌为助催化剂,采用等体积浸渍法将它们负载于不同的载体(纤维素、金属氧化物γ-Al2O3,分子筛MCM-41等单组份载体以及纤维素和γ-Al2O3的复合载体)制备得到多相负载型催化剂用以催化CO2与环氧丙烷的环加成反应。这些多相负载型催化剂在间歇釜中催化CO2和环氧丙烷的加成反应时表现出较高的催化活性,但稳定性较差,难以实现循环。以催化剂纤维素+γ-Al2O3/KI为例,考察其在间歇釜反应中稳定性较差的原因,结果表明,KI在高温反应后易被空气中的氧气氧化而使催化剂活性降低。将催化剂纤维素+γ-Al2O3/KI用于固定床连续反应装置,碳酸丙烯酯的单程收率最高可达50%左右,反应16 h催化剂活性没有明显下降。

以四丁基溴化铵为催化剂,催化CO2与环氧棉籽油加成制备棉籽油碳酸酯。考察反应温度、反应压力、反应时间和催化剂用量对该加成反应的影响。将得到的产物进行润滑基础油性能测试,测试结果显示,与环氧棉籽油相比,棉籽油碳酸酯的氧化安定性、热稳定性及摩擦学性能得到改善。

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In this thesis, the five-membered cyclic carbonates were synthesized by cycloaddition reactions of propylene oxide, epoxidized cottonseed oil and carbon dioxide, which not only reduced the emission of the greenhouse gas carbon dioxide but obtained propylene carbonate and bio-based material carbonated cottonseed oil that could be applied in the lubrication industry. The main contents and conclusions were as follows. Heterogeneous supported catalysts whose supports included cellulose, γ-Al2O3, MCM-41 and composite cellulose/γ-Al2O3 were prepared by impregnation method in which KI was used as the main catalyst and zinc halides as the promoters. Those heterogeneous supported catalysts exhibited high catalytic activity when they were used as the catalysts of the cycloaddition reaction of propylene oxide and carbon dioxide in the batch autoclave. However, they exhibited poor stability for recycling in the batch autoclave. The reason for their poor stability in the batch autoclave was that after taking part in the high temperature and pressure reaction the main catalyst KI was prone to be oxidized by the oxygen in the air. When the catalyst cellulose/γ-Al2O3 was applied in the continous fixed-bed reactor to catalize the cycloaddition of propylene oxide and carbon dioxide, it was observed that the highest single-pass yield of propypene cabonate was about 50% and the catalytic activity of the catalyst did not decrease until sixteen hours. The carbonated cottonseed oil was prepared by adding carbon dioxide to epoxidized cottonseed oil using tetrabutylammonium bromide as the catalyst. The effect of reaction temperature, pressure, time, and the amount of catalyst on the cycloaddition reaction was also investigated. The properties of the products as the lubricant base oil were investigated and the results showed that compared with the epoxidized cottonseed oil, the carbonated cottonseed oil possessed better oxidation and thermal stability, friction-reducing, anti-wear and extreme pressure properties.

文献类型学位论文
条目标识符http://ir.xjipc.cas.cn/handle/365002/2488
专题新疆维吾尔自治区精细化工工程技术研究中心
作者单位中国科学院新疆理化技术研究所
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罗燕平. 五元环碳酸酯的合成及其在润滑油领域的应用[D]. 北京. 中国科学院大学,2013.
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