【作者】 熊燕；

【导师】 蒋景阳；

【作者基本信息】 大连理工大学 ， 有机化学， 2006， 硕士

【摘要】 本文利用含聚醚链的季铵盐型离子液体与有机溶剂组成了具有“高温均相,室温分相”特性的离子液体/有机两相体系,将此体系的“温控”功能用于催化反应来实现“高温均相反应,室温两相分离”的过程。这是既具有均相催化高活性和高选择性,又能够通过简单相分离回收催化剂的新型液/液两相催化体系,为解决贵金属催化剂的分离回收提供了一条有效途径。 本文应用“温控”离子液体两相体系分别进行了1—十二烯、二聚异丁烯和SBS（苯乙烯—丁二烯嵌段共聚物）的催化加氢反应研究。考察了各种反应条件对加氢的影响,催化剂的循环使用及其在有机相中的流失情况。实验结果表明,此体系中RuCl₃/TPPTS催化的1—十二烯加氢反应有很高的活性,在优化的反应条件下产物收率达到98%,催化剂循环使用十次催化活性无明显下降,Ru在有机相中的流失平均小于0.2%。二聚异丁烯的催化加氢,产物收率在80%左右。含有催化剂的离子液体循环十次,从第五次开始催化活性稍有下降。反应后有机相检测不到Ru金属的流失。考察了离子液体两相体系中Ru（COD）Cl₂/TPPTS配合物催化的SBS加氢。其中,甲苯/环已烷/离子液体温控两相体系对SBS加氢仅达到25%的总加氢度。四氢呋喃/水/离子液体温控两相体系SBS加氢可达到65%的总加氢度,催化剂循环使用三次催化活性有所下降。以上结果表明,此温控离子液体两相体系对烯烃的催化加氢具有较高的催化活性,通过简单相分离即可实现含有催化剂的离子液体的回收,催化剂循环效果好,流失小。此体系在高聚物SBS的加氢方面的应用仍需进一步探索。更多还原

【Abstract】 A thermoregulated ionic liquid biphasic system was developed by using polyether modified quarternary ammonium salts ionic liquid and organic solvents. This ionic liquid biphasic system possesses a thermoregulated property i.e. "mono-phase under high temperature, bi-phase under room temperature". The hydrogenation of 1-dodecene, diisobutylene and SBS （Styrene-Butadiene-Styrene copolymer） catalyzed by Ru /TPPTS complex have been studied in this new system respectively. The reaction conditions have been optimized and the recycle efficiency and the leaching of the catalyst have been studied. In the hydrogenation of 1-dodecene the yield of n-dodecane reached 98% under the optimized reaction conditions. After reaction, the catalyst retained in ionic liquid can be easily recovered by phase separation at room temperature. The catalyst has been recycled for 10 times without obvious decrease of the catalytic activity. The average leaching of Ru in organic phase is about 0.2%. In the hydrogenation of diisobutylene the yield of product is about 80% and the catalyst can be recycled 10 times with a little decrease of the catalytic activity after the fifth run. There was not leaching of Ru in the organic phase detected by ICP-AES analysis. The hydrogenation degree of SBS reached about 60% in the THF/H₂O/ionic liquid system and the catalyst could be reused for three times. The hydrogenation degree of SBS in the toluene/cyclohexane/ionic liquid system was only 25% although the system was homogeneous at reaction temperature and came back to biphasic at room temperature. Hydrogenation of SBS in this ionic liquid system needs further research.更多还原