聚合离子液体设计及催化环己烷选择性氧化性能研究
Study on design of polymeric ionic liquids and the performance for selective oxidation of cyclohexane
王瑞瑞 1金颖 2刘玉梅 1李梦悦 1朱胜文 1闫瑞一 1刘瑞霞1
作者信息
- 1. 中国科学院过程工程研究所,离子液体清洁过程北京市重点实验室,北京 100190
- 2. 郑州大学河南先进技术研究院,河南 郑州 450003
- 折叠
摘要
以乙烯基咪唑为单体,添加不同量的引发剂,采用常规热聚合中自由基聚合的方式,合成了不同分子量的聚乙烯基咪唑,热重(TG)分析表明该聚合物具有良好的热稳定性.采用季铵化反应,对最优聚合物进行1-氯代十八烷、1-氯代十二烷以及1-氯代正己烷三种不同烷基链长度的取代,合成系列聚合离子液体(PIL).通过傅里叶红外光谱(FT-IR)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、接触角等表征手段分析了聚合离子液体的化学结构及形貌特征,并考察了PIL-C18、PIL-C12、PIL-C6催化环己烷选择性氧化为己二酸的性能,进而选取PIL-C12深入研究了离子率对催化性能的影响规律.结果表明,烷基链段长度以及离子率可以有效调控亲疏水性和反应活性位点,进而提高反应性能,使得反应生成己二酸的转化率达到21.8%,选择性为41.5%.
Abstract
Different molecular weights of poly(vinylimidazole)were synthesized by using vinyl imidazole as a monomer and different amounts of initiators.Thermogravimetric(TG)analysis showed that the polymer had good thermal stability.A series of polymeric ionic liquids(PIL)were synthesized by quaternization of the optimal polymer with three different alkyl chain lengths:1-chlorooctadecane,1-chlorododecane,and 1-chlorohexane.The chemical structure and morphology of the polymeric ionic liquids were analyzed by Fourier transform infrared spectroscopy(FT-IR),scanning electron microscopy(SEM),X-ray photoelectron spectroscopy(XPS),and contact angle testing.The catalytic performance of PIL-C18,PIL-C12,and PIL-C6 for selective cyclohexane oxidation was investigated.Furthermore,PIL-C12 was selected to conduct in-depth research on the influence of ion rates(PIL-C12-X,X=10,25,50,75,100)on catalytic performance.The results showed that the length of alkyl chain segment and the ionic ratio could effectively influence the hydrophobicity and active site of the catalysts to improve the performance with the conversion of 21.8%and selectivity of 41.5%for cyclohexane oxidation to adipic acid.
关键词
聚合离子液体/离子率/环己烷/催化/氧化Key words
polymeric ionic liquids/ionic rate/cyclohexane/catalytic/oxidation引用本文复制引用
出版年
2024
国家科技期刊平台
NSTL
万方数据