采用水热合成法合成了金属原子(Zn,Ni,Fe,Al,Cu,Ce)掺杂的MCM-41介孔分子筛(简称T-MCM-41),并将其应用于邻苯二甲酸二(2-乙基已)酯(DOP)的合成反应,研究了不同原子的掺杂对T-McM-41的结构,比表面积和孔径、酸性及催化性能的影响.结果表明,所制备的T-McM-41仍然具有六方有序排列结构,比表匝f积较高(550-900 m2/g)、孔径大(3 nm左右),杂原子的引入使T-MCM-41产生了酸中心,从而使其对DOP的合成具有很好的催化活性和选择性.用T-MCM-41(T=Zn,Fe,Al,Cu)催化DOP的合成反应,在5 h的反应时间内苯酐的转化率可以达到95.5%以上,DOP的选择性可达到96.5%以上.T-MCM-41催化剂具有很好的稳定性,Al-MCM-41在重复使用5次后仍具有较好的催化活性.
参考文献
| [1] | J.S.Beck,J.C.Vartuli,W.J.Roth,M.E.Leonowicz,C.T.Kresge,K.D.Schmitt,C.T-W.Chu,D.H.Olson,E.W.Sheppard,S.B.McCullen,J.B.Higgins,J.L.Schlenkert,A new family of mesoporous molecular sieves prepared with liquid crystal templates,Journal of the American Chemical Society,114,10834(1992) |
| [2] | ZHANG Jianguo,JIANG Qingzhe,ZHENG Chengguo,SONG Zhaozheng,KE Ming,Synthesis method and its influence factors of Si-MCM-41,Journal of China University of Petroleum (Natural Science Edition),32(1),113(2008)(张建国,蒋庆哲,郑成国,宋昭峥,柯明,Si-MCM-41的合成及其影响因素,中国石油大学学报(自然科学版),32(1),113(2008)) |
| [3] | MENG Huadong,ZHANG Juntao,DING Liqin,LIANG Shengrong,WANG Xiaoquan,Synthesis and characterization of mesoporons molecular sieve AI-MCM-41,Journal of Xi'an Shiyou University (Natural Science Edition),22(3),104(2007)(孟华东,张君涛,丁丽芹,梁生荣,王小泉,Al-MCM-41介孔分子筛的合成与表征,西安石油大学学报(自然科学版),22(3),104(2007)) |
| [4] | Y.R.Wang,N.C.Lang,A.Tuel,Nature and acidity of aluminum species in Ai MCM--41 with a high aluminum content (Si/A1=1.25),Microporous and Mesoporous Materials,93,46(2006) |
| [5] | QIAO Kui,ZHANG Fumin,PAN Duoli,ZHANG Niaofei,JIAN Panming,Synthesis,characterization and catalyti oxidation performance of high Ti-contalning Ti-MCM-41 molecular sieves,Chinese Journal of Inorgnic Chemistry,24(5),748(2008)(乔亏,张富民,潘多丽,张鸟飞,营盘铭,高钛Ti-MCM-41分子筛的合成、表征与催化氧化性能考察,无机化学学报,24(5),748(2008)) |
| [6] | S.Udayakumar,A.Pandurangan,P.K.Sinha,Paraselective ethylation of phenol with diethyl carbonate over mesoporous A1-MCM-41 molecular sieves,Applied Catalysis A:General,272,267(2004) |
| [7] | M.J.B.Souza,A.S.Araujo,A.M.G.Pedrcea,B.A.Marinkovic,P.M.Jardim,E.M.Jr.,Textural features of highly ordered AI-MCM-41 molecular sieve studied by X-ray diffraction,nitrogen adsorption and transmission electron microscopy,Materials Letters,60,2682(2006) |
| [8] | C.Blanco,C.Pesquera,F.Gonz 6 lez,Synthesis and characterization of MCM-41 with different Si/Al molar ratios and different silicon sources.Studies in Surface Science and Catalysis,154,432(2004) |
| [9] | R.Wojcieszak,S.Monteverdi,M.Mercy,I.Nowak,M.Ziolek,M.M.Bettahar,Nickel containing MCM-41 and Al MCM-41 mesoporous molecular sieves:characteristics and activity in the hydrogenation of benzene,Applied Catalysis A:General,268,241(2004) |
| [10] | V.Parvuleecu,B.L.Su,Iron,cobalt or nickel substituted MCM-41 molecular sieves for oxidation of hydrocarbons,Catalysis Today,60,315(2001) |
| [11] | R.R.Sever,R.Alcala,J.A.Dumesic,T.W.Root,Vaporphase silylation of MCM-41 and Ti-MCM-41,Microporous and Mesoporous Materials,66(1),53(2003) |
| [12] | CUI Rong,LIU Xiaoqin,SHAN Jiahui,Preparation of Ce-MCM-41 adsorbent and its performance in model gasofine desulfurization,Natural Gas Chemical Engineering,33(2),11(2008)(崔榕,刘晓勤,单佳慧,Ce-MCM-41分子筛吸附剂的制备及其在模拟汽油脱硫中的性能,天然气化工,33(2),11(2008)) |
| [13] | KONG Yah,XU Xinjie,WU Yong,ZHANG Rui,WANG Jun,Effect of promoters on the catalytic activity of MCM41 with high copper content in benzene hydroxylation,Chinese Journal of Catalysis,29(4),385(2008) |
| [14] | C.Mahendiran,P.Sangeetha,P.Vijayan,S.J.Sardhar Basha,K.Shanthi,Vapour phase oxidation of tetralin over Cr and Fe substituted MCM-41 molecular sieves,Journal of Molecular Catalysis A:Chemical,275,84(2007) |
| [15] | S.S.Bhoware,A.P.Singh,Characterization and catalytic activity of cobalt containing MCM-41 prepared by direct hydrothermal,grafting and immobilization methods,Journal of Molecular Catalysis A:Chemical,266,118(2007) |
| [16] | L.F.Chen,J.A.Wang,L.E.Norena,J.Aguilar,J.Navarrete,P.Salns,J.A.Montoya,P.Del Angel,Synthesis and physicochemical properties of Zr-MCM-41 mesoporons molecular sieves and Pt/H3PW12O40/Zr-MCM-41 catalysts,Journal of Solid State Chemistry,180,2958(2007) |
| [17] | JIANG Pingping,Lu Guanzhong,Development of solid catalyst in catalytic synthesis of DOP,Chemical Industry and Engineering Process,21(5),328(2002)(蒋平平,卢冠忠,固体酸催化合成邻苯二甲酸二辛酯,化工进展,21(5),328(2002)) |
| [18] | F.T.Sejidov,Y.Mansoori,N.Goodarzi,Esterification reaction using solid heterogeneous acid catalysts under solvent-less condition,Journal of Molecular Catalysis A:Chemical,240,186(2005) |
| [19] | M.Ziolek,I.Nowak,B.Kilos,I.Sobczak,P.Decyk,M.Trejda,J.C.Volta,Template synthesis and characterisation of MCM-41 mesoporous molecular sieves containing various transition metal elements-TME (Cu,Fe,Nb,V,Mo),Journal of Physics and Chemistry of Solids,65,571(2004) |
| [20] | S.Ajaikumar,A.Pandurangan,Esterifieation of alkyl acids with alkanols over MCM-41 molecular sieves:Influence of hydrophobic surface on condensation reaction,Journal of Molecular Catalysis A:Chemical,266,1(2007) |
| [21] | M.Bhagiyalakshmi,K.Shanmugapriya,M.Palanichamy,B.Arabindoo and V.Murugesan,Esterification of maleic anhydride with methanol over solid acid catalysts:a novel route for the production of heteroesters,Applied Catalysis A:General,267,77(2004) |
| [22] | DOU Maofeng,JIN Shengming,FUling,CHANG Yan,GUAN Haoyuan,YANG Min,Preparation and structure of mesoporous molecular sieves Ti-MCM-41,Journal of the Chinese Ceramic Society,36(1),65(2008)(豆茂峰,金胜明,付英,常燕,关豪元,杨敏,介孔分子筛Ti-McM-41的制备和结构,硅酸盐学报,36(1),65(2008)) |
| [23] | R.Luque,J.M.Campelo,D.Luna,J.M.Marinas,A.A.Romero,NH4F effect in post-synthesis treatment of Al-MCM-41 mesoporous materials,Microporous and Mesoporous Materials,84,11(2005) |
| [24] | HUANG Shiyong,WANG Haitao,SONG Yanfen,GAO Wenyi,FAN Lirong,LIAN Piyong,Synthesis of mesoporous MCM-41 molecular sieves containing heteroatoms and study of cyclohexane oxidation,Fine Chemicals,21(1),41(2004)(黄世勇,王海涛,宋艳芬,高文艺,樊丽荣,连丕勇,杂原子MCM-41分子筛的合成及对环己烷氧化的研究,精细化工,21(1),41(2004)) |
| [25] | LI Fuxiang,ZHANG Xiangdi,LI Ruifeng,XIE Kechang,Synthesis and characterization of mesoporous Zr-MCM-41,Journal of Fuel Chemidtry and Technology,32(4),471(2004)(李福祥,张香娣,李瑞丰,谢克昌,Zr-MCM-41的合成及其表征,燃料化学学报,32(4),471(2004)) |
| [26] | WU Shujie,HUANG Jiahui,WU Tonghao,SONG Ke,WANG Hongsu,XING Lihong,XU Haiyan,XU Ling,GUAN Jingqi,KAN Qiubin,Synthesis,characterization,and catalytic performance of mesoporous Al-SBA-15 for Tert-butylation of phenol,Chinese Journal of Catalysis,27(1),9(2006) |
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