水介质中Ullmann反应高效纳米介孔结构催化剂研制及催化机理研究.pdfVIP

11班}「},* 术刀沂功Ullmann反之论)忘者动术矛括群指撰介肩硬知巩粼麦君讼次理研男 6.通过对 Si-MCM-41为载体进行修饰，然后以其为载体制得催化剂 Pd/Ph-MCM-41，考察了苯基修饰量对该催化剂在水中Ullmann碘苯偶联反应活 性的影响。结果表明，随着苯基含量的增加，碘苯的转化率和联苯的选择性随之 增加，这可能是由于Si-MCM-41经过有机基团修饰后，提高了催化剂对反应物 。 G。 I-6 关键词:清洁有机合成;MCM-41/Al-MCM-41/Ph-MCM-41;负载型Pd催化 剂;水溶液中Ullmann反应;碘苯 助,h渗峥1~大爹 放户及功U!lnennnAn~.U逆 A分疙41V屏尸众 Abstract Therecentdiscoveryofnovelsilica-basedmesoporousmaterialsdesignatedas M41Shavedevelopedanewclassofporousmaterialsexhibitingorderedporous structurewithuniform diameterbetween 1.5nm and 10nm.Suchunique characteristics togetherwiththeirextremelyhighsurfaceareaexhibitpotential applicationsinadsorption,separation,biochemistry,andnano-assemlyetc.As catalysts,theiractivitiescouldevenmatchthehomogeneouscatalysts,whichshows goodpotentialinfuturecatalysisowingtotheeasyseparationbetweenthecatalysts andreactionproducts. Today,greenchemistryrepresentsgeneraltrendsowingtotherequirementsfor environmentalprotection.Torealizegreenchemistry,itisnecessarytodesignnew catalystswithhighactivityandexcellentselectivitytowarddesiredproducts.Besides, thechemicalreactionsshouldbeperformedincleanmediasincevariousorganic solventscauseenvironmentalpollution.Ofcourse,-themostcleanandsafetysolvent iswater.However,nearlyalltheorganicsyntheticreactionsneedorganicsolvents ratherthanwaterduetothesolubilitylimitation.Uptonow,onlythehomogeneous catalystshavebeenattemptedintheorganicreactionsinaqueoussolutionand sometimesaphase-transferringcatalystshouldbeused.Asmentionedabove,the homogeneouscatalystscouldnotbeusedrepetitivelysincetheseparationbetween catalystsandreactionproductsisusuallydifficult.Althoughheterogeneouscatalysts couldovercometheseparationdifficulty,theirpooractivityincomparisonwith homogeneouscatalystsseemsaproblem.Inthispaper,wedesignedthreekindsof catalysts,i.e.,Pd/MCM-41,Pd/Al-MCM-41andPd/Ph-MCM-41byimpregnation followingtheH