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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

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【作者】 张娇玉朱生华唐瑞源郑延成李克华

【Author】 ZHANG Jiaoyu;ZHU Shenghua;TANG Ruiyuan;ZHENG Yancheng;LI Kehua;College of Chemistry and Environmental Engineering, Yangtze University;Research Center of Petroleum Processing & Petrochemicals, Xi’an Shiyou University;

【机构】 长江大学化学与环境工程学院西安石油大学石油炼化工程技术研究中心

【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%.

【基金】 重质油国家重点实验室开放课题项目(SKLOP201901001);湖北省教育厅指导性项目(B2020040);省部共建煤炭高效利用与绿色化工国家重点实验室开放课题(2021-K44)
  • 【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
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