膦功能化离子液稳定的纳米钯催化喹啉高选择性加氢  

Palladium nanoparticles stabilized by phosphine functionalized ionic liquid for highly selective hydrogenation of quinoline

作　　者：蒋和雁 吴志峰 JIANG He-yan;WU Zhi-feng(Key Laboratory of Catalysis Science and Technology of Chongqing Education Commission,Chongqing Key Laboratory of Catalysis and New Environmental Materials,College of Environmental and Resources,Chongqing Technology and Business University,Chongqing 400067,China)

机构地区：[1]重庆工商大学环境与资源学院,重庆高校催化理论与应用技术市级重点实验室,催化与环境新材料重庆市重点实验室,重庆400067

出　　处：《化学研究与应用》2018年第3期349-356,共8页Chemical Research and Application

基　　金：国家自然科学基金项目(21201184)资助;重庆工商大学自然科学基金项目(1751039)资助;催化与环境新材料重庆市重点实验室项目(CQCM-2016-02)资助

摘　　要：通过简单的还原方法在离子液体[BMMIM]PF_6(1-丁基-2,3-二甲基咪唑六氟磷酸盐)中,以膦功能化离子液体[BMMIM][tppm](1-丁基-2,3-二甲基咪唑间三苯基膦单磺酸盐)为稳定剂制备了纳米钯催化剂。采用透射电镜(TEM)、X-射线衍射(XRD)、X-射线光电子能谱(XPS)等方法对纳米钯催化剂进行了表征。结果表明:[BMMIM][tppm]稳定的纳米钯催化剂分散均匀,平均粒径约为3.9 nm,且Pd(Ⅱ)完全转化为Pd(0)。在喹啉加氢反应过程中,考察了稳定剂种类、稳定剂用量、溶剂、温度、压力等因素对喹啉选择性加氢的影响。在50℃和氢气压力为3.5MPa的温和条件下,纳米钯催化剂催化喹啉及其衍生物加氢显示出高活性和高化学选择性。在循环过程中,膦功能化离子液体稳定的纳米钯催化剂能保持良好的催化活性和化学选择性。Through simple reduction method,the Pd nanocatalyst was prepared in[BMMIM]PF6 by using phosphine functionalized ionic liquid[BMMIM][tppm]as a stabilizing agent.The catalyst was characterized by transmission electron microscopy(TEM),Xray diffraction(XRD),Xray photoelectron spectroscopy(XPS)The results showed that Pd nanoparticles stabilized by[BMMIM][tppm]were highly dispersed,the average size was about 3.87 nm and Pd(Ⅱ)was completely reduced to Pd(0)The influences of different stabilizers,the amount of the stabilizer,solvents,temperature and hydrogen pressure on selective hydrogenation of quinoline were investigated.Pd nanocatalyst exhibited high activity and chemoselectivity in hydrogenation of quinoline and its derivatives under mild conditions(50℃,35MPa H2)Pd nanocatalyst stabilized by phosphine functionalized ionic liquid could maintain satisfactory catalytic activity and chemoselectivity in catalytic recycles.

关 键 词：膦功能化离子液体 钯 多相催化 喹啉 选择性加氢 

分 类 号：O625.[理学—有机化学] 42[理学—化学]