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《多孔SiO_2·xH_2O负载RuB纳米粒子催化喹啉加氢反应.pdf》由会员上传分享,免费在线阅读,更多相关内容在行业资料-天天文库。
1、物理化学学报(WuliHuaxueXuebao)2422ActaPhys.一Chim.Sin.,2010,26(9):2422—2428September【Article】www.whxb.pku.edu.ca多孔SiO2.xa20负载RuB纳米粒子催化喹啉加氢反应张磊胡博陈华李贤均李瑞祥(四川大学化学学院,绿色化学与技术教育部重点实验室,成都610064)摘要:通过水解,聚乙烯吡咯烷酮(PvP)保护,NaOH刻蚀等方法制备了多孔及富含表面羟基的Si02"xH20负载的RuB催化剂RuB/SiO2"xHO,并用x射线衍
2、射(XRD)、x射线光电子能谱(xps)、透射电子显微镜(TEM)、傅里叶变换红Pb(FT—IR)光谱和BET(Brunauer—Emmett—Teller)等手段对该催化剂进行了表征.结果表明该催化剂具有良好的抗中毒能力,在3.0MPa的H压力和80℃的温和反应条件下,喹啉的转化率高于95%,生成1,2,3,4一四氢喹啉的选择性高于97%.并系统研究了表面羟基和溶剂对催化剂性能的影响,发现以水为溶剂时,RuB/SiP2·xH20对喹啉加氢反应展示出较高的活性和对1,2,3,4一四氢喹啉较高的选择性,催化剂能够多次循环
3、使用.这一体系的优异催化性能归属于载体表面羟基和水的协同作用.关键词:钌;水合二氧化硅;喹啉;加氢;四氢喹啉中图分类号:0643CatalyticPerformanceofPorousSiOz。xHzOSupportedRuBNan0particlesfortheHydrogenationofQuinolineZHANGLeiHUBoCHENHuaLIXian—JunLIRui-Xiang(KeyLaboratoryofGreenChemistryandTechnologyoftheMinistryofEducatio
4、n,CollegeofChemistry,SichuanUniversity,Chengdu610064,PR.China)Abstract:Aporousandhydroxylgroup—richcatalystRuB/SiP2‘xH2Owaspreparedbyhydrolyzingethylsilicate,protectingSiO2‘HzOwithpolyvinylpyrrolidone(PVP),andetchingSi02‘xH20withNa0H.Thecatalystwascharacterizedb
5、yX-raydiffraction(XRD),X—rayphotoelectronspectroscopy(XPS),transmissionelectronmicroscopy(TEM),Fouriertransforminfrared(FIR)spectroscopy,andBET(Brunauer-Emmett-Teller).Wefoundthatthecatalystshowedexcellentperformanceforthehydrogenationofquinolineundermildconditi
6、on.Atahydrogenpressureof3.0MPaandflreactiontemperatureof80℃,theconversionofquinolinereached95%andtheselectivityfor1,2,3.4一tetrahydroquinolinewas97%.Thisporouscatalystalsoshowedanexcellentanti—poisoningcharacteristic.Thecatalystcanbereusedsevera1times.Wealsoinves
7、tigatedtheeffectofsurfacehydroxylgroupsandthesolventoncatalyticactivityandselectivity.Theresultsshowedthatusingwaterasasolventleadstohighercatalystactivityandselectivityforthehydrogenationofquinoline.Themechanismofquinolinehydrogenationoverthecatalystisdiscussed
8、.Thecoordinationoftl1enitrogenonqainolineontothesurfaceof/'utl1eniumnanoparticles.theeffectofhydrogenbondamongthesurfacehydroxylgroupsofthecatalystandthenitrogenprese
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