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改性纳米ZSM-5分子筛催化甲醇制对二甲苯的反应性能
Study on Catalytic Performance of Methanol to p-Xylene over Modified Nano-sized ZSM-5 Zeolites
【摘要】 通过水热合成的方法合成纳米ZSM-5分子筛,并采用等体积浸渍法制备ZnO,MgO和P2O5复合改性分子筛,用于催化甲醇高选择性制对二甲苯反应中。采用XRD、SEM、氮气吸附-脱附以及NH3-TPD等手段对催化剂进行表征分析,并在固定床微型反应装置上进行甲醇直接制对二甲苯(MTPX)反应性能评价。结果表明:相比于常规微米ZSM-5分子筛,纳米分子筛具有大量晶间介孔,提高总芳烃选择性;Zn改性减少强酸量,增加中强酸酸量,有利于芳烃产物的生成;分子筛上进一步引入适量的MgO和P2O5可以有效覆盖分子筛的部分孔口和外表面的酸性位,对孔道扩散限制产生影响,对位选择性提高至81.1%,对二甲苯选择性提高至23.3%。
【Abstract】 Nano ZSM-5 zeolites was synthesized by hydrothermal synthesis method, and the compositely modified nano ZSM-5zeolites by ZnO,MgO,and P2O5 was prepared by equal volume impregnation method, which was used to catalyze the highly selective reaction of preparing p-xylene using methanol.The synthesized modified nano-sized ZSM-5 zeolites was characterized by XRD,SEM,N2 adsorption-desorption and NH3-TPD.Furthermore, the catalytic performance of different ZSM-5 zeolites for using methanol to prepare p-xylene was investigated.The results indicated that, nano-sized samples exhibited higher aromatic selectivity than micro-sized ZSM-5,owing to the more inter-mesopores.The introduction of Zn could increase the medium acid sites, which enhanced the aromatic production.The modification of Mg and P could optimise both the acidic properties and shape selectivity, which is beneficial to the formation of p-xylene.The modified nano-sized ZSM-5 zeolite gave the p-xylene selectivity of 23.3%,with the para-selectivity of 81.1%.
【Key words】 nano-sized ZSM-5 zeolites; composite modification; p-xylene; methanol; shape selectivity;
- 【文献出处】 西安石油大学学报(自然科学版) ,Journal of Xi’an Shiyou University(Natural Science Edition) , 编辑部邮箱 ,2024年05期
- 【分类号】O643.36;TQ241.13
- 【下载频次】77