无有机胺醇水体系低硅铝比ZSM-5沸石的一步合成  

One-step synthesis of ZSM-5 zeolites with low silica-alumina ratio in organic amine-free alcohol-water system

作　　者：张国林 郝文明 秦波 杜艳泽 马静红[1] 李瑞丰[1] ZHANG Guolin;HAO Wenming;QIN Bo;DU Yanze;MA Jinghong;LI Ruifeng(College of Chemical Engineering and Technology,Taiyuan University of Technology,Taiyuan 030024,China;Sinopec(Dalian)Research Institute of Petroleum and Petrochemicals Co.,Ltd.,Dalian 116045,China)

机构地区：[1]太原理工大学化学工程与技术学院,山西太原030024 [2]中石化(大连)石油化工研究院有限公司,辽宁大连116045

出　　处：《石油化工》2024年第9期1251-1258,共8页Petrochemical Technology

基　　金：国家自然科学基金企业创新发展联合基金重点支持项目(U21B20100)。

摘　　要：研究了无有机胺醇水体系低硅铝比ZSM-5沸石的绿色合成方法。在无有机胺模板剂和不加晶种的醇水体系中,一步合成了形貌均一的小晶粒聚集体低硅铝比ZSM-5沸石,考察了合成体系中各配料的含量以及晶化温度对合成低硅铝比ZSM-5沸石的影响。利用XRD、FTIR、SEM、N_(2)吸附-脱附、^(27)Al MAS NMR和^(29)Si MAS NMR等方法对合成的ZSM-5沸石进行表征。实验结果表明,当n(Si)∶n(Al)=20,n(Na_(2)O)∶n(SiO_(2))=0.071,n(C_(2)H_(5)OH)∶n(SiO_(2))=1.77,晶化温度为160℃时,可合成具有高结晶度的纯相ZSM-5沸石。^(27)Al MAS NMR表征结果显示,合成的ZSM-5沸石主要含有骨架四配位铝,无非骨架铝。合成的ZSM-5沸石的比表面积和微孔孔体积分别为384 m^(2)/g和0.14 cm^(3)/g,总酸量达到789μmol/g,骨架n(Si)∶n(Al)=14.4。The green synthesis of ZSM-5 zeolite with low silica-alumina ratio in an organic aminefree alcohol-water system was investigated.In the alcohol-water system without an organic amine templating agent and addition of crystal seed,ZSM-5 zeolites with low silica-alumina ratio and small grain aggregates of uniform morphology were synthesized in one step,and the effects of the amount of each ingredient in the synthesis system and the crystallization temperature on the synthesis of ZSM-5 zeolites with low silica-alumina ratio were investigated.The synthesized ZSM-5 zeolites were characterized using XRD,FTIR,SEM,N_(2) adsorption-desorption,^(27)Al MAS NMR,and ^(29)Si MAS NMR.The experimental results show that the ZSM-5 pure-phase zeolite with high crystallinity could be synthesized when n(Si)∶n(Al)=20,n(Na_(2)O)∶n(SiO_(2))=0.071,and n(C_(2)H_(5)OH)∶n(SiO_(2))=1.77 at the crystallization temperature of 160℃.^(27)Al MAS NMR result shows that the synthesized ZSM-5 zeolite mainly contains skeletal tetra-coordinated aluminum and no non-skeletal aluminum.The specific surface area and microporous pore volume of the synthesized ZSM-5 zeolite are 384 m^(2)/g and 0.14 cm^(3)/g,respectively,and the total acid amount reaches 789μmol/g,with n(Si)∶n(Al)=14.4.

关 键 词：无有机胺体系 低硅铝比ZSM-5沸石 水热合成 

分 类 号：TQ426.65[化学工程]