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作 者:余道轲 符美丽 袁亚辉[1] 宋一兵[1] 陈佳阳[1] 方奕文[1]
出 处:《燃料化学学报》2016年第11期1363-1369,共7页Journal of Fuel Chemistry and Technology
基 金:The project was supported by the National Fund Cultivation Project(NFC 15001);the Science and Technology Plan Project of Guangdong Province(2013B030600001);the Subject and Specialty Construction Special Fund of Guangdong Provincial Higher Education Institution(2012CXZD0024,2013KJCX0081)~~
摘 要:多级孔结构ZSM-5分子筛的合成过程复杂。利用双模板剂,通过优化晶化条件(如晶化时间与晶化温度)和Si/Al物质的量比等一步水热晶化合成了具有多级孔结构的ZSM-5分子筛,并采用XRD、N_2吸附-脱附、吡啶红外吸脱附、SEM和TEM等方法对样品的晶体结构、孔道结构、表面酸性和形貌等进行了表征。结果表明,一步法合成多级孔结构ZSM-5分子筛的适宜条件是:晶化温度160-180℃,晶化时间24-96 h,反应物组成为SiO_2/Al_2O_3/Na_2O/CTAB/TPABr/H_2O=1/x/0.4/0.05/0.12/280,(x:50-240)。其中,晶化温度160℃、晶化时间48 h和以Si/Al物质的量比50的凝胶合成的样品具有有序的介孔(平均尺寸3.60 nm)结构、较高的结晶度和较强的酸性。Generally,the process for synthesis of hierarchical-structured ZSM-5 zeolite is complex. Here,the polygonal threedimensional ZSM-5 zeolite with hierarchical structure was hydrothermally synthesized by one-step synthesis method with dual templates. The effects of crystallization conditions and synthesis gel compositions, including crystallization temperature,crystallization time,Si/Al molar ratio,on the products were investigated for optimizing synthesis conditions. The X-ray diffraction( XRD),N_2 adsorption-desorption experiment,Pyridine adsorption FT-IR( Py-FTIR),scanning electron microscopy( SEM) and transmission electron microscope( TEM) were used to characterize the crystalline structure,pore structure,surface acidity and crystal morphology of products. It was shown that the hierarchical-structured ZSM-5 zeolite can be synthesized under the following conditions: crystallization temperature of 160-180 ℃,crystallization time of 24-96 h,the SiO_2/Al_2O_3/Na_2O/CTAB/TPABr/H2 O ratio of 1/x/0.4/0.05/0.12/280,( x: 50-240). The sample crystallized at 160℃ for 48 h with a synthesis gel having a Si/Al molar ratio of 50 had uniform cylindrical crystal morphology,high crystallinity and ordered mesoporous structure with a pore diameter of 3.60 nm. It contains both strong Brnsted and Lewis acid sites at 300 ℃,which contribute to its catalytic properties.
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