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时间:2020-03-26
《制备方法对ZnO-ZrO2催化剂上乙醇转化制异丁烯反应的影响.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、第32卷第8期无机化学学报Vo1.32No.82016年8月CHINESEJOURNALOFINORGANICCHEMISTRY1391.1397制备方法对ZnO.ZrO2催化剂上乙醇转化制异丁烯反应的影响刘田薛芳琦乐英红华伟明高滋(复旦大学化学系,上海市分子催化和功能材料重点实验室,上海200433)摘要:采用恒pH值共沉淀法和非恒pH值共沉淀法制备了ZnO—ZrO混合氧化物催化剂,考察了制备方法对乙醇转化制异丁烯反应的影响,并用低温N吸附、X射线衍射、扫描电子显微镜、透射电子显微镜、X射线光电子能谱、拉曼光谱、紫外一可见漫反射光谱、NH程序升温脱附和CO程序
2、升温脱附对催化剂进行了表征。研究结果表明,相比于非恒pH值共沉淀法制备的ZnO—ZrO,恒pH值共沉淀法制备的ZnO.ZrO,具有较高的比表面积,更多的酸量和碱量,从而表现出更好的乙醇转化制异丁烯催化性能。在450℃和乙醇质量空速O.2h的反应条件下,两种催化剂的乙醇转化率均为100%,恒pH值共沉淀法制备的催化剂的异丁烯得率为54.9%,明显高于非恒pH值共沉淀法制备的催化剂(45.7%),并且稳定性也是前者明显高于后者。关键词:混合氧化物;制备方法;乙醇;异丁烯;酸碱性中图分类号:0614.241;0614.41+2文献标识码:A文章编号:1001—4861
3、(2016)08。1391.07DoI:10.11862/CJIC.2016.177InfluenceofPreparativeMethodonZnO-ZrO2CatalystforEthanolConversiontoIsobuteneLIUTianXUEFang—QiYUEYing—HongHUAWei—MingGAOZi∞KeyLaboratoryofMolecularCatalysisandInnovativeMaterials,DepartmentofChemistry,FudanUniversity,Shanghai200433,China)Abst
4、ract:ZnO—ZrO2mixedoxidecatalystswerepreparedusingeitheraconstantorvariablepHvalueCO.precipitationmethod.TheobtainedcatalystsampleswerecharacterizedusingN2adsorption,X-raydiffraction,scanningelectronmicroscopy,transmissionelectronmicroscopy,X—rayphotoelectronspectroscopy,Ramanspectros
5、copy,uhraviolet—visiblediffusereflectance,NH3temperature-programmeddesorptionandCO2temperature—programmeddesorption.ComparedtotheZnO—Zr02mixedoxidepreparedusingthevariablepHvaluemethod,thecorrespondingmixedoxidepreparedusingtheconstantpHvaluemethodhadahighersurfaceareaandahighernumbe
6、rofacidsitesandbasicsites,thusexhibitingasuperiorcatalyticperformance.Whenthereactiontemperaturewas450℃andtheweighthourlyspacevelocityofethanolwas0.2h~.theconversionofethanolforbothcatalystswas100%.TheZnO—ZrO2catalystpreparedusingtheconstantpHvaluemethodgave54.9%yieldofisobutene.whic
7、hwasobviouslygreaterthantheyieldobtainedusingthecorrespondingcatalystpreparedusingthevariablepHvaluemethod(45.7%).Moreover,theformercatalystexhibitedobviouslyhigherstabilitythanthelatteronefortheisobuteneproductionfromethanolconversion.Keywords:mixedoxide;preparativemethod;ethanol;is
8、obutene;acid
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