Four ZSM-5 zeolite catalysts with different Si/Al ratios for the catalytic cracking of C4 fractions to produce ethylene and propylene were prepared in this study.First,the adsorption isotherms of pure n-butane and but...Four ZSM-5 zeolite catalysts with different Si/Al ratios for the catalytic cracking of C4 fractions to produce ethylene and propylene were prepared in this study.First,the adsorption isotherms of pure n-butane and butene-1 and their mixtures on these catalysts at 300K and p=0—100kPa were measured using the intelligent gra- vimetric analyzer.The experimental results indicate that the presence of Al can significantly affect the adsorption of butene-1 than that of n-butane on ZSM-5 zeolites.Then,the double Langmuir(DL)model was applied to study the pure gas adsorption on ZSM-5 zeolites for pure n-butane and butene-1.By combining the DL model with the ideal adsorbed solution theory(IAST),the IAST-DL model was applied to model the butene-1(1)/n-butane(2)binary mixture adsorption on ZSM-5 zeolites with different Si/Al ratios.The calculated results are in good agreement with the experimental data,indicating that the IAST-DL model is effective for the present systems.Finally,the adsorp- tion over a wide range of variables was predicted at low pressure and 300K by the model proposed.It is found that the selectivity of butene-1 over n-butane increases linearly with the decrease of Si/Al ratio.A correlation between the selectivity and Si/Al ratio of the sample was proposed at 300K and p=0.08MPa.展开更多
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...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。展开更多
基金Supported by the National Natural Science Foundation of China (Nos.20236010,20476004) and China Petroleum & Chemical Corporation (No.X504023).
文摘Four ZSM-5 zeolite catalysts with different Si/Al ratios for the catalytic cracking of C4 fractions to produce ethylene and propylene were prepared in this study.First,the adsorption isotherms of pure n-butane and butene-1 and their mixtures on these catalysts at 300K and p=0—100kPa were measured using the intelligent gra- vimetric analyzer.The experimental results indicate that the presence of Al can significantly affect the adsorption of butene-1 than that of n-butane on ZSM-5 zeolites.Then,the double Langmuir(DL)model was applied to study the pure gas adsorption on ZSM-5 zeolites for pure n-butane and butene-1.By combining the DL model with the ideal adsorbed solution theory(IAST),the IAST-DL model was applied to model the butene-1(1)/n-butane(2)binary mixture adsorption on ZSM-5 zeolites with different Si/Al ratios.The calculated results are in good agreement with the experimental data,indicating that the IAST-DL model is effective for the present systems.Finally,the adsorp- tion over a wide range of variables was predicted at low pressure and 300K by the model proposed.It is found that the selectivity of butene-1 over n-butane increases linearly with the decrease of Si/Al ratio.A correlation between the selectivity and Si/Al ratio of the sample was proposed at 300K and p=0.08MPa.
文摘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。