1,8-辛二胺作为结构导向剂合成ZSM-11分子筛
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摘要
ZSM-11是重要的固体酸催化剂,在石油化工领域应用广泛,因此,ZSM-11的高效合成备受关注.采用1,8-辛二胺(DAOT)作为结构导向剂,用水热法在较宽范围内成功地合成了不含ZSM-5杂晶的ZSM-11分子筛.研究了水平转速、晶化温度、晶化时间以及硅铝比对ZSM-11分子筛制备的影响.在不同的合成条件下,得到了不同的晶体尺寸、形貌以及不同结晶度的ZSM-11分子筛.样品晶粒通过X射线衍射(XRD)和扫描电子显微镜(FESEM)进行表征.研究拓展了ZSM-11的高效合成方法,得到了ZSM-11分子筛的最佳合成条件为水平转速50r/min,160℃晶化48h.
ZSM-11 is an important solid acid catalyst and is widely used in petrochemical industry.Therefore,the high efficient synthesis of ZSM-11 is highly concerned.In this paper,ZSM-11 zeolites without ZSM-5 hybrid was successfully synthesized in a wide range by using 1,8-diaminooctane as Structure-directing agent(SDA).The effect of speed of horizontal rotation,crystallization temperature,crystallization time and Si/Al ratio on the preparation of the ZSM-11 zeolites were studied.ZSM-11 zeolites with different crystal sizes,morphologies and crystallinities were produced under different synthesis conditions.The crystallinity and morphology of the resulted ZSM-11 zeolites were characterized by X-ray diffraction(XRD)and field emission scanning electron microscopy(FESEM).This study extends efficient synthesis method of the ZSM-11 and gets the best synthetic conditions of ZSM-11 zeolites:horizontal speed of 50 r/min,160 ℃ crystallization 48 h.
ZSM-11 is an important solid acid catalyst and is widely used in petrochemical industry.Therefore,the high efficient synthesis of ZSM-11 is highly concerned.In this paper,ZSM-11 zeolites without ZSM-5 hybrid was successfully synthesized in a wide range by using 1,8-diaminooctane as Structure-directing agent(SDA).The effect of speed of horizontal rotation,crystallization temperature,crystallization time and Si/Al ratio on the preparation of the ZSM-11 zeolites were studied.ZSM-11 zeolites with different crystal sizes,morphologies and crystallinities were produced under different synthesis conditions.The crystallinity and morphology of the resulted ZSM-11 zeolites were characterized by X-ray diffraction(XRD)and field emission scanning electron microscopy(FESEM).This study extends efficient synthesis method of the ZSM-11 and gets the best synthetic conditions of ZSM-11 zeolites:horizontal speed of 50 r/min,160 ℃ crystallization 48 h.
引文
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[17]于庆君,李春义,山红红,等.纳米棒插接多级孔ZSM-11分子筛形貌影响因素研究[J].中国石油大学学报,2016,40(2):155-162.
[18]付文华,袁志庆,王仰东,等.协同导向法合成ZSM-5/ZSM-11共生分子筛[J].化学反应工程与工艺,2016,32(5):400-407.
[19]Conte M,Xu B,Davies T E,et al.Enhanced selectivity to propene in the methanol to hydrocarbons reaction by use of ZSM-5/11intergrowth zeolite[J].Microprous Mesoprous Mater,2012,164:207-213.
[20]Chen L,Zhu S.Y,Wang Y M,et al.One-step synthesis of hierarchical pentasil zeolite microspheres using diamine with linear carbon chain as single template[J].New J Chem,2010,34(10):2328-2334.
[2]Liu H,Liu S L,Xie S J,et al.Effect of Desilication on the Performance of Hierarchical ZSM-11Catalysts for Alkylation of Benzene with Dimethyl[J].Ether Catal Lett,2015,145(11):1972-1983.
[3]Huang H W,Meng X J,Chen C,et al.Effect of Phosphorus Addition on the Performance of Hierarchical ZSM-11Catalysts in Methanol to Propene Reaction[J].Catal Lett,2016,146(11):2357-2363.
[4]Ji Y W,Birmingham J,Deimund M A,et al.Steam-dealuminated,OSDA-free RHO and KFI-type zeolites as catalysts for the methanolto-olefins reaction[J].Microprous Mesoprous.Mater,2016,232:126-137.
[5]Meng X J,Huang H W,Zhang Q,et al.Conversion of methanol into light olefins over ZSM-11catalyst in a circulating fluidized-bed unit[J].Korean J Chem Eng,2016,33(3):831-837.
[6]Anunziata O A,Cussa J.Applying response surface design to the optimization of methane activation with ethane over Zn-H-ZSM-11zeolite[J].Chem Eur J,2008,138(1/2/3):510-516.
[7]Wang X,Chen H B,Meng F J,et al.CTAB resulted direct synthesis and properties of hierarchical ZSM-11/5composite zeolite in the absence of template[J].Microprous Mesoprous Mater,2017,243:271-280.
[8]Otomo R,Müller U,Feyen M,et al.Development of post-synthetic method for tuning Al content of OSDA-free Beta as catalyst for conversion of methanol to olefins[J].Catal Sci Technol,2016,6(3):713-721.
[9]Fyfe C A,Lin Z S,Tong C,et al.efficient syntheses of zeolite ZSM-11(MEL)at temperatures below 100℃using very dense gels[J].Microprous Mesoprous Mater,2012,150(1):7-13.
[10]Makowski W,Majda D.Equilibrated thermodesorption studies of adsorption of n-exae and n-heptane on zeolites Y,ZSM-5and ZSM-11[J].Appl Surf Sci,2005,252(3):707-715.
[11]Wei Z H,Zhu K K,Xing L Y,et al.Steam-assisted transformation of natural kaolin to hierarchical ZSM-11using tetrabutylphosphonium hydroxide as structure-directing agent:synthesis,structural characterization and catalytic performance in the methanol-to-aromatics reaction[J].RSC Adv,2017,7(39):24015-24021.
[12]Marguta R,Khatib S J,Guil J M,et al.Molecular simulation and adsorption studies of n-hexane in ZSM-11zeolites[J].Microprous Mesoprous Mater,2011,142(1):258-267.
[13]Yu Q J,Cui C Y,Zhang Q,et al.Hierarchical ZSM-11with intergrowth structures:Synthesis,characterization and catalytic properties[J].J Energ Chem,2013,22(5):761-768.
[14]Dyballa M,Becker P,Trefz D,et al.Parameters influencing the selectivity to propene in the MTO conversion on 10-ring zeolites:directly synthesized zeolites ZSM-5,ZSM-11,and ZSM-22[J].Appl Catal A Gen,2016,510:233-243.
[15]Dey K P,Ghosh S,Naskar M K.A facile synthesis of ZSM-11zeolite particles using rice husk ash as silica source[J].Mater Lett,2012,87:87-89.
[16]Yu Q J,Meng X J,Liu J W,et al.A fast organic template-free,ZSM-11seed-assisted synthesis of ZSM-5with good performance in methanol-to-olefin[J].Microprous Mesoprous Mater,2013,181:192-200.
[17]于庆君,李春义,山红红,等.纳米棒插接多级孔ZSM-11分子筛形貌影响因素研究[J].中国石油大学学报,2016,40(2):155-162.
[18]付文华,袁志庆,王仰东,等.协同导向法合成ZSM-5/ZSM-11共生分子筛[J].化学反应工程与工艺,2016,32(5):400-407.
[19]Conte M,Xu B,Davies T E,et al.Enhanced selectivity to propene in the methanol to hydrocarbons reaction by use of ZSM-5/11intergrowth zeolite[J].Microprous Mesoprous Mater,2012,164:207-213.
[20]Chen L,Zhu S.Y,Wang Y M,et al.One-step synthesis of hierarchical pentasil zeolite microspheres using diamine with linear carbon chain as single template[J].New J Chem,2010,34(10):2328-2334.
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