摘要
Crystalline phase is the key factor for catalyst activity. The zirconium modified PCs/γ-Al_2O_3 samples were prepared through a simple step incipient-wetness impregnation method. The raw materials and samples were characterized by thermogravimetric-differential analysis(TG-DTA), X-ray diffraction(XRD), Fourier transform infrared spectroscopy(FT-IR), temperature-programmed desorption of ammonia and carbon dioxide(NH_3-and CO_2-TPD). The effects of calcination temperature and zirconium content on structure, chemical transformation,and acidity-basicity were investigated. Calcination temperature exhibited the major effect on the crystalline phase of samples. The new phase of Al0.1Zr_(0.9)O_(1.95) was exhibited which was above 650 ℃. In addition, zirconium content was influenced by the acidic and basic properties of the surface. The acidity and basicity of the Zr PCs/γ-Al_2O_3 sample increased with the increasing of zirconium content.
Crystalline phase is the key factor for catalyst activity. The zirconium modified PCs/γ-Al_2O_3 samples were prepared through a simple step incipient-wetness impregnation method. The raw materials and samples were characterized by thermogravimetric-differential analysis(TG-DTA), X-ray diffraction(XRD), Fourier transform infrared spectroscopy(FT-IR), temperature-programmed desorption of ammonia and carbon dioxide(NH_3-and CO_2-TPD). The effects of calcination temperature and zirconium content on structure, chemical transformation,and acidity-basicity were investigated. Calcination temperature exhibited the major effect on the crystalline phase of samples. The new phase of Al0.1Zr_(0.9)O_(1.95) was exhibited which was above 650 ℃. In addition, zirconium content was influenced by the acidic and basic properties of the surface. The acidity and basicity of the Zr PCs/γ-Al_2O_3 sample increased with the increasing of zirconium content.
引文
[1]G.Zhang,H.Zhang,D.Yang,C.LI,Z.Peng,S.Zhang,Catalysts,kinetics and process optimization for the synthesis of methyl acrylate over Cs-P/γ-Al2O3,Catal.Sci.Technol.6(2016)6417–6430.
[2]C.Sararuk,D.Yang,G.Zhang,C.Li,S.Zhang,One-step aldol condensation of ethyl acetate with formaldehyde over Ce and P modified cesium supported alumina catalyst,J.Ind.Eng.Chem.46(2017)342–349.
[3]H.Amani,Z.Ahmad,B.H.Hameed,Highly active alumina-supported Cs–Zr mixed oxide catalysts for low-temperature transesterification of waste cooking oil,Appl.Catal.A Gen.487(2014)16–25.
[4]B.Li,R.Yan,L.Wang,Y.Diao,Z.Li,S.Zhang,Synthesis of methyl methacrylate by aldol condensation of methyl propionate with formaldehyde over acid–base bifunctional catalysts,Catal.Lett.143(2013)829–838.
[5]R.Liu,T.Wang,C.Liu,Y.Jin,Highly selective and stable Cs PW/Nb2O5catalysts for dehydration of glycerol to acrolein,Chin.J.Catal.34(2013)2174–2182.
[6]A.Hamza,N.Nagaraju,Amorphous metal-aluminophosphate catalysts for aldol condensation of n-heptanal and benzaldehyde to jasminaldehyde,Chin.J.Catal.36(2015)209–215.
[7]Y.Wei,Y.Li,Y.Tan,J.Zhou,Z.Wu,Y.Liu,A facile route for one-pot synthesis of short-channeled bimetallic Zr–Al–SBA-15,Mater.Lett.141(2015)145–148.
[8]L.E.Davies,N.A.Bonini,S.Locatelli,E.E.Gonzo,Characterization and catalytic activity of zirconium dioxide prepared by sol–gel,Lat.Am.Appl.Res.35(2005)23–28.
[9]R.Si,Y.-W.Zhang,C.-X.Xiao,S.-J.Li,B.-X.Lin,Y.Kou,C.-H.Yan,Non-template hydrothermal route derived mesoporous Ce0.2Zr0.8O2nanosized powders with blue-shifted UV absorption and high CO conversion activity,Phys.Chem.Chem.Phys.6(2004)1056–1063.
[10]G.Zhang,Z.Peng,C.Li,A study of thermal behavior of cesium phosphate,J.Therm.Anal.Calorim.124(2016)1063–1070.
[11]M.Laspéras,H.Cambon,D.Brunel,I.Rodriguez,P.Geneste,Cesium oxide encapsulation in faujasite zeolites effect of framework composition on the nature and basicity of intrazeolitic species,Microporous Mater.7(1996)61–72.
[12]S.Yuvaraj,L.Fan-Yuan,C.Tsong-Huei,Y.Chuin-Tih,Thermal decomposition of metal nitrates in air and hydrogen environments,J.Phys.Chem.B 107(2003)1044–1047.
[13]N.Gorodylova,P.?ulcová,M.Bosacka,E.Filipek,DTA-TG and XRD study on the reaction between Zr OCl2·8H2O and(NH4)2HPO4for synthesis of Zr P2O7,J.Therm.Anal.Calorim.118(2014)1095–1100.
[14]A.Keshavaraja,N.E.Jacob,A.V.Ramaswamy,Thermal decomposition of coprecipitated oxide hydrates of zirconium and manganese,Thermochim.Acta 254(1995)267–275.
[15]M.Lasperas,I.Rodriguez,D.Brunel,H.Cambon,P.Geneste,Effect of the framework composition on the nature and the basicity of intrazeolitic cesium oxides.Correlation activity/basicity,Stud.Surf.Sci.Catal.97(1995)319–326.
[16]S.Damyanova,P.Grange,B.Delmon,Surface characterization of zirconia-coated alumina and silica carriers,J.Catal.168(1997)421–430.
[17]G.Li,W.Li,M.Zhang,K.Tao,Characterization and catalytic application of homogeneous nano-composite oxides Zr O2–Al2O3,Catal.Today 93(2004)595–601.
[18]T.Klimova,M.L.Rojas,P.Castillo,R.Cuevas,J.Ramírez,Characterization of Al2O3-Zr O2mixed oxide catalytic supports prepared by the sol–gel method,Microporous Mesoporous Mater.20(1998)293–306.
[19]V.S.De Portilla,The nature of hydrogen bonds and water in legrandite by IR spectroscopy,Am.Mineral.61(1976)95–99.
[20]M.Dixit,M.Mishra,P.A.Joshi,D.O.Shah,Physico-chemical and catalytic properties of Mg–Al hydrotalcite and Mg–Al mixed oxide supported copper catalysts,J.Ind.Eng.Chem.19(2013)458–468.
[21]H.Song,Y.Sun,X.Jia,Hydrothermal synthesis of iron phosphate microspheres constructed by mesoporous polyhedral nanocrystals,Mater.Charact.107(2015)182–188.
[22]J.Yan,C.Zhang,C.Ning,Y.Tang,Y.Zhang,L.Chen,S.Gao,Z.Wang,W.Zhang,Vapor phase condensation of methyl acetate with formaldehyde to preparing methyl acrylate over cesium supported SBA-15 catalyst,J.Ind.Eng.Chem.25(2015)344–351.
[23]D.Sarkar,D.Mohapatra,S.Ray,S.Bhattacharyya,S.Adak,N.Mitra,Synthesis and characterization of sol–gel derived Zr O2doped Al2O3nanopowder,Ceram.Int.33(2007)1275–1282.
[24]A.R.Hajipour,H.Karimi,Synthesis and characterization of hexagonal zirconium phosphate nanoparticles,Mater.Lett.116(2014)356–358.
[25]Y.Li,J.Feng,D.Li,Preparation and characterization of spherical mesoporous Zr O2-Al2O3composites with high thermal stability,Sci.China Chem.54(2011)1032–1038.