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1、第*期作者等:文章题目·9·Ce改性硅钨酸催化制备月桂酸单甘酯朱广琪1,李佳敏1,张晓芳1,韩晓祥1*,唐秀娟2,王奎武1,王彦波1*(1.浙江工商大学应用化学系,浙江杭州310018;2.浙江工商大学环境科学与工程学院浙江杭州310018)摘要:采用离子交换法合成多种稀土改性硅钨酸催化剂MxH4–3xSiW12O40(M=La,Ce,Pr,Nd,Sm;x=1/3,2/3,1,4/3),并利用FTIR,XRD,TGA-DTG,固体核磁共振结合探针分子技术(31P-TMPOMAS-NMR)对CexH4–3xSiW12O40催化剂结构、稳定性及酸
2、性进行了表征;结果表明,Ce1/3H3SiW12O40催化剂在月桂酸单甘酯制备中显示出最好的催化性能。稀土Ce有效结合到硅钨酸上,制备的催化剂保持了完整的Keggin结构。与纯硅钨酸相比,CexH4–3xSiW12O40的酸强度有所减弱,但由于该类催化剂较强的Brønsted酸性及Brønsted-Lewis酸性位间的协同效应,使CexH4–3xSiW12O40在月桂酸单甘酯的制备中具有良好的催化性能。以Ce1/3H3SiW12O40为催化剂,在甘油/月桂酸物质的量比为4/1,催化剂用量为月桂酸质量的4%,反应温度423K,反应时间120mi
3、n下,月桂酸单甘酯产率为78.4%;动力学研究表明,该反应活化能为42.37kJ/mol;Ce1/3H3SiW12O40催化剂经5次回收利用,月桂酸单甘酯的产率为71.4%,具有较好的重复使用性能。关键词:稀土;硅钨酸;酯化反应;月桂酸单甘酯;催化技术中图分类号:O643.32文献标识码:A文章编号:CatalyticPropertiesofCeExchangedTungstosilicicAcidontheEsterificationtoGlycerolMonolaurateZHUGuang-qi1,LIJia-min1,ZHANGXiao
4、-fang1,HANXiao-xiang1*,TANGXiu-juan2,WANGKui-wu1,WANGYan-bo1*(1.DepartmentofAppliedChemistry,ZhejiangGongshangUniversity,Hangzhou310018,Zhejiang,China;2.CollegeofEnvironmentalScienceandEngineering,ZhejiangGongshangUniversity,Hangzhou310018,Zhejiang,China)Abstract:Aseriesofr
5、areearthmodifiedtungstosilicicacidcatalystsMxH4-3xSiW12O40(M=La,Ce,Pr,Nd,Sm;x=1/3,2/3,1,4/3)werepreparedbyionexchangemethod.Thestructure,stabilityandacidityofthecatalysts(CexH4-3xSiW12O40)werecharacterizedbydifferentanalyticalandspectroscopictechniquessuchasFT-IR,XRD,TGA-DT
6、Gand31PMAS-NMR,andtheircatalyticpropertieswereinvestigatedontheesterificationoflauricacid(LA)andglycerol(GL)toglycerolmonolaurate(GML).ResultsshowedthatCe1/3H3.0SiW12O40catalysthadthebestcatalyticactivityinthesynthesisofGML.Therareearthmetalcation(Ce)hadbeeneffectivelycombi
7、nedtotungstosilicicacid,andthecatalystsmaintainedthecompleteKegginstructure.Comparedwithtungstosilicicacid,theacidityofCexH4-3xSiW12O40catalystsdecreased,butthecatalystshadgoodcatalyticperformanceduringtheesterificationforstrongBrønstedacidityandBrønsted-Lewisacidsynergy.Th
8、eCe1/3H3.0SiW12O40wasutilizedtooptimizethereactionconditionswith第*期作者等:文章题目·9·78.4