通过采用高温带压磷酸二氢铵溶液对β分子筛进行磷改性得到改性β分子筛催化剂,考察其在苯与乙烯高空速烷基化反应中的催化活性,并对其结晶度、元素组成、酸量、酸类型及骨架结构等物化性质进行表征。结果表明:经磷改性后,β分子筛催化...通过采用高温带压磷酸二氢铵溶液对β分子筛进行磷改性得到改性β分子筛催化剂,考察其在苯与乙烯高空速烷基化反应中的催化活性,并对其结晶度、元素组成、酸量、酸类型及骨架结构等物化性质进行表征。结果表明:经磷改性后,β分子筛催化剂的总酸量和B酸、L酸中心浓度均有明显提高,且磷元素的引入使改性β分子筛催化剂在31P MASNMR和27 Al MASNMR表征谱图中,在化学位移为-30.908和41.392处均有一强吸收峰,证明β分子筛的骨架结构中有P(4Al)和Al(4P)四配位结构出现,稳定了骨架铝,提高了催化剂的活性稳定性。当P2O5在催化剂中的质量分数为2%时,该催化剂在苯与乙烯高空速烷基化反应中的活性稳定性最佳。展开更多
对常温和高温条件下的磷改性β分子筛进行热重、核磁共振和酸性分析,并考察其在苯与乙烯烷基化反应中的反应性能。结果表明:β分子筛高温条件下引入铵根离子后,其DTG曲线在220~230℃之间有一明显的失重峰出现,即铵根离子进入分子筛内部;...对常温和高温条件下的磷改性β分子筛进行热重、核磁共振和酸性分析,并考察其在苯与乙烯烷基化反应中的反应性能。结果表明:β分子筛高温条件下引入铵根离子后,其DTG曲线在220~230℃之间有一明显的失重峰出现,即铵根离子进入分子筛内部;其^(31)P MAS NMR和^(27)Al MAS NMR表征中在化学位移为-30.908和41.392处均有一强吸收峰,即β分子筛的骨架结构中有P(4Al)和Al(4P)四配位结构出现;其NH_3-TPD酸性增强,酸量增加。评价结果表明β分子筛高温条件下引入铵根离子后,其烷基化反应性能明显提高。展开更多
Zeolite beta with a low SiO2/Al2O3 ratio was synthesizcd by a novel two-step process. The synthesized sample was characterized with XRD, SEM, FTIR, and N2 adsorption-desorption and solid-state MAS NMR. The results sho...Zeolite beta with a low SiO2/Al2O3 ratio was synthesizcd by a novel two-step process. The synthesized sample was characterized with XRD, SEM, FTIR, and N2 adsorption-desorption and solid-state MAS NMR. The results showed that aluminium species were inserted into the framework of zeolite beta. The BET surface area, volume, and particle size of the zeolite beta sample decreased with decreasing SiO2/Al2O3 ratio. Our process was proved an efficient route to synthesize zeolitc beta with a low SiO2/Al2O3 ratio.展开更多
Well-crystallized zeolite beta was synthesized by using acid-leached metakaolin as the silica-alumina source and tetraethylammonium hydroxide structure-directing agent.The influence of the composition of the reaction ...Well-crystallized zeolite beta was synthesized by using acid-leached metakaolin as the silica-alumina source and tetraethylammonium hydroxide structure-directing agent.The influence of the composition of the reaction mixture on product crystallinity was investigated,and the crystallization process was studied by examining solid samples obtained at different synthesis times.Results showed that the acid-leached metakaolin was fully converted into soluble aluminum and silicon species,which is crucial for the formation of well-crystallized zeolite beta.At the beginning of the crystallization process,these soluble aluminum and silicon species formed a aluminum-rich intermediate structure with layer morphology.With the crystallization proceeding,more silicon species were incorporated into the zeolite beta framework and the layered structure was changed into spherical particles of zeolite beta with high SiO 2 /Al 2 O 3 ratio and crystallinity.展开更多
Mesoporous aluminosilicate with cubic ordered structure was synthesized by two-step crystallization, which showed stronger acid sites and more effective activity for catalytic alkylation of 2, 4-ditert-butylphenol wit...Mesoporous aluminosilicate with cubic ordered structure was synthesized by two-step crystallization, which showed stronger acid sites and more effective activity for catalytic alkylation of 2, 4-ditert-butylphenol with tert-butanol than conventional H-AlMCM-48 materials.展开更多
文摘通过采用高温带压磷酸二氢铵溶液对β分子筛进行磷改性得到改性β分子筛催化剂,考察其在苯与乙烯高空速烷基化反应中的催化活性,并对其结晶度、元素组成、酸量、酸类型及骨架结构等物化性质进行表征。结果表明:经磷改性后,β分子筛催化剂的总酸量和B酸、L酸中心浓度均有明显提高,且磷元素的引入使改性β分子筛催化剂在31P MASNMR和27 Al MASNMR表征谱图中,在化学位移为-30.908和41.392处均有一强吸收峰,证明β分子筛的骨架结构中有P(4Al)和Al(4P)四配位结构出现,稳定了骨架铝,提高了催化剂的活性稳定性。当P2O5在催化剂中的质量分数为2%时,该催化剂在苯与乙烯高空速烷基化反应中的活性稳定性最佳。
文摘对常温和高温条件下的磷改性β分子筛进行热重、核磁共振和酸性分析,并考察其在苯与乙烯烷基化反应中的反应性能。结果表明:β分子筛高温条件下引入铵根离子后,其DTG曲线在220~230℃之间有一明显的失重峰出现,即铵根离子进入分子筛内部;其^(31)P MAS NMR和^(27)Al MAS NMR表征中在化学位移为-30.908和41.392处均有一强吸收峰,即β分子筛的骨架结构中有P(4Al)和Al(4P)四配位结构出现;其NH_3-TPD酸性增强,酸量增加。评价结果表明β分子筛高温条件下引入铵根离子后,其烷基化反应性能明显提高。
文摘Zeolite beta with a low SiO2/Al2O3 ratio was synthesizcd by a novel two-step process. The synthesized sample was characterized with XRD, SEM, FTIR, and N2 adsorption-desorption and solid-state MAS NMR. The results showed that aluminium species were inserted into the framework of zeolite beta. The BET surface area, volume, and particle size of the zeolite beta sample decreased with decreasing SiO2/Al2O3 ratio. Our process was proved an efficient route to synthesize zeolitc beta with a low SiO2/Al2O3 ratio.
基金supported by Beijing Natural Science Foundation (Grant No.2093043)the National Natural Science Foundation of China (Grant No.20606038)
文摘Well-crystallized zeolite beta was synthesized by using acid-leached metakaolin as the silica-alumina source and tetraethylammonium hydroxide structure-directing agent.The influence of the composition of the reaction mixture on product crystallinity was investigated,and the crystallization process was studied by examining solid samples obtained at different synthesis times.Results showed that the acid-leached metakaolin was fully converted into soluble aluminum and silicon species,which is crucial for the formation of well-crystallized zeolite beta.At the beginning of the crystallization process,these soluble aluminum and silicon species formed a aluminum-rich intermediate structure with layer morphology.With the crystallization proceeding,more silicon species were incorporated into the zeolite beta framework and the layered structure was changed into spherical particles of zeolite beta with high SiO 2 /Al 2 O 3 ratio and crystallinity.
基金We thank financial support by the National Natural Science Foundation of China(grant 29973001).
文摘Mesoporous aluminosilicate with cubic ordered structure was synthesized by two-step crystallization, which showed stronger acid sites and more effective activity for catalytic alkylation of 2, 4-ditert-butylphenol with tert-butanol than conventional H-AlMCM-48 materials.
