催化学报

催化学报 ›› 2011, Vol. 32 ›› Issue (7): 1280-1286.DOI: 10.3724/SP.J.1088.2011.10235

• 研究论文 • 上一篇    下一篇

改性纳米 HZSM-5 催化剂上甲苯与甲醇的烷基化反应

张志萍, 赵 岩, 吴宏宇, 谭伟, 王祥生, 郭新闻*   

  1. 大连理工大学化工学院催化化学与工程系, 精细化工国家重点实验室, 辽宁大连 116024
  • 收稿日期:2011-02-24 修回日期:2011-05-11 出版日期:2011-07-18 发布日期:2014-11-28

Shape-Selective Alkylation of Toluene with Methanol over Modified Nano-scale HZSM-5 Zeolite

ZHANG Zhiping, ZHAO Yan, WU Hongyu, TAN Wei, WANG Xiangsheng, GUO Xinwen*   

  1. State Key Laboratory of Fine Chemicals, Department of Catalysis Chemistry and Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China
  • Received:2011-02-24 Revised:2011-05-11 Online:2011-07-18 Published:2014-11-28

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摘要： 以 Si, P, Mg 复合改性的纳米 HZSM-5 为催化剂, 进行了甲苯与甲醇的烷基化反应; 并采用 X 射线衍射, NH3 程序升温脱附, 红外和低温 N2 吸附等方法研究了改性前后催化剂酸性质和孔结构的变化. 在小型固定床反应器上, 考察了载气量、反应温度和重时空速等反应条件对烷基化反应性能的影响. 在 2 h–1, 460 oC, 甲苯/甲醇比, 水/烃比和 N2/烃摩尔比均为 8 的优化条件下, 单程连续运转 500 h, 甲苯转化率可维持在 10% 左右, 对二甲苯选择性高于 97%, 催化剂表现出良好的稳定性.

Abstract: Shape-selective alkylation of toluene (T) with methanol (M) was performed over Si-P-Mg-modified nano-scale HZSM-5 zeolite. The change of acidity and pore structure of the catalyst was studied by X-ray diffraction, NH3 temperature-programmed desorption, Fourier transform infrared spectroscopy, and N2 adsorption．The effects of temperature, space velocity (WHSV), and flow rate of N2 carrier gas on the reaction were investigated in a continuous flow fixed-bed reactor. Under the optimized conditions (2 h–1, 460 oC, n(T)/n(M) = n(H2O)/n(HC) = n(N2)/n(HC) = 8, where HC represents toluene and methanol), during 500 h on stream over the Si-P-Mg modified nano-scale HZSM-5 catalyst, the toluene conversion of about 10% and the selectivity to p-xylene of more than 97% were maintained, indicating that the catalyst exhibits high selectivity and good stability.

Key words: nano-scale HZSM-5 zeolite, silicon-phosphorus-magnesium modification, toluene, methanol, alkylation, p-xylene