γ-Al_2O_3负载的Pd-Ni双金属催化剂催化合成γ-十一内酯
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摘要
采用浸渍法制备了γ-Al2O3负载的Pd-Ni双金属催化剂(Pd-Ni(x∶y)/Al2O3;x∶y为Pd与Ni的质量比),并将其应用于合成γ-十一内酯的反应.所制Pd-Ni/Al2O3催化剂经过X射线衍射仪、X射线光电子能谱仪及场发射透射电子显微镜等检测手段分析,确认了Pd及Ni两种金属均匀地分布于载体γ-Al2O3之上.在催化反应中,考察了单(双)金属催化剂、反应温度、反应时间等因素对于反应的影响.Pd-Ni(1∶1)/Al2O3(PN-1∶1)催化剂展现出了最佳的催化性能,其催化的反应中γ-十一内酯的产率达到85%左右.
In order to efficiently synthesizeγ-undecalactone,γ-Al2O3 supported Pd-Ni bimetallic catalysts(Pd-Ni(x∶y)/Al2O3;x∶y represents mass ratio of Pd and Ni)were prepared by impregnation method and used for synthesis ofγ-undecalactone.The catalysts were detected by X-ray photoelectron spectroscopy,X-ray diffraction and transmission electron microscopy,which demonstrated Pd and Ni were uniformly distributed on theγ-Al2O3.The catalytic ability was measured by different types of catalyst,temperature,time,etc.The PN-1∶1displayed extremely high catalytic activity,the yield ofγ-undecalactone reaching 85%.
In order to efficiently synthesizeγ-undecalactone,γ-Al2O3 supported Pd-Ni bimetallic catalysts(Pd-Ni(x∶y)/Al2O3;x∶y represents mass ratio of Pd and Ni)were prepared by impregnation method and used for synthesis ofγ-undecalactone.The catalysts were detected by X-ray photoelectron spectroscopy,X-ray diffraction and transmission electron microscopy,which demonstrated Pd and Ni were uniformly distributed on theγ-Al2O3.The catalytic ability was measured by different types of catalyst,temperature,time,etc.The PN-1∶1displayed extremely high catalytic activity,the yield ofγ-undecalactone reaching 85%.
引文
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[2]B Vigneron.Preparation 4-Alkyl-γ-Lactones Optiquemet actives[J].Tetrahedron Leters,1980,21:173-175.
[3]蔡宝国,孙晔,金东元,等.γ-十一内酯合成工艺的研究[J].香料香精化妆品,2003,2:4-6.
[4]W J Wang,M H Qiao,H X Li,et al.Amorphous NiP/SiO2aerogel:its preparation,its high thermal stability and its activity during theselective hydrogenation of cyclopentadiene to cyclopentene[J].Applied Catalysis A-General,1998,166:243-247.
[5]S Yoshida,H Yamashita,T Funabiki,et al.Catalysis by amorphous metal alloys[J].Journal of the Chemical Society,Faraday Transactions,1984,180:1 435-1 446.
[6]C L Fernando,G Q Santiago,A Claudia,et al.Gas phase hydrogenation of p-chloronitrobenzene over Pd-Ni/Al2O3[J].Applied Catalysis A-General,2014,473:41-50.
[7]N S Babu,N Lingaiah,P S S Prasad.Characterization and reactivity of Al2O3supported Pd-Ni bimetallic catalysts for hydrodechlorinationof chlorobenzene[J].Applied Catalysis B-Environmental,2012,111-112:309-316.
[8]H Yang,D Shi,S F Ji,et al.NanosizedPd assembled on superparamagnetic core-shellmicrospheres:Synthesis,characterization and recyclablecatalytic properties for the Heck reaction[J].Chinese Chemical Letters,2014,25:1 265-1 270.
[9]S J SardharBasha,P Vijayan,C Suresh,et al.Effect of order of impregnation of Mo and Ni on the hydrodenitrogenation activity of NiO-MoO3/AlMCM-41catalyst[J].Industrial&Engineering Chemistry Research,2009,48:2 774-2 780.
[10]A B Jaap,V Tom,R G L Bob,et al.Envisaging the physicochemical processes during the preparation of supported catalysts:raman microscopy on the impregnation of Mo onto Al2O3extrudates[J].Journal of the American Chemical Society,2004,126:14 548-14 556.
[11]Y Qiu,L Xin,W Z Li.Electrocatalytic oxygen evolution over supported small amorphous Ni-Fe nanoparticles in alkaline electrolyte[J].Langmuir,2014,30:7 893-7 901.
[12]X Q Pan,Y B Zhang,Z Z Miao,et al.A novel PdNi/Al2O3catalyst prepared by galvanic deposition for low temperature methane combustion[J].Journal of Energy Chemistry,2013,22:610-616.
[13]C L Fernando,G Q Santiago,A Claudia,et al.Gas phase hydrogenation of p-chloronitrobenzene over Pd-Ni/Al2O3[J].Applied Catalysis A-General,2014,473:41-50.
[14]X Q Pan,Y B Zhang,B Zhang,et al.Influence of electronic effect on methane catalytic combustion over PdNi/Al2O3[J].Chemical Research in Chinese Universities,2013,29:952-955.
[15]P Lu,T Teranishi,K Asakura,et al.Polymer-protected Ni/Pd bimetallic nano-clusters:preparation,characterization and catalysis for hydrogenation of nitrobenzene[J].The Journai of Physical Chemistry B,1999,103:9 673-9 682.
[16]P K Cheekatamarla,A M Lane.Efficient bimetallic catalysts for hydrogen generation from diesel fuel[J].International Journal of Hydrogen Energy,2005,30:1 277-1 285.