高等学校化学学报 ›› 2021, Vol. 42 ›› Issue (1): 227-238.doi: 10.7503/cjcu20200413

• 研究论文 • 上一篇    下一篇

ZSM-5分子筛酸位分布及其甲醇制烯烃催化性能的定向管理与调控

郭淑佳1,2,王森1,张莉1,2,秦张峰1,王鹏飞1,董梅1,王建国1,2,樊卫斌1   

  1. 1.中国科学院山西煤炭化学研究所, 煤转化国家重点实验室, 太原 030001
    2.中国科学院大学, 北京 100049
  • 收稿日期:2020-07-01 出版日期:2021-01-10 发布日期:2021-01-12
  • 基金资助:
    国家自然科学基金(批准号(U1910203);21802157, 21991092, 21991090)、 山西省自然科学基金(201901D211581);山西省优秀博士生奖励资助项目(BK2018001);中国科学院山西煤炭化学研究所煤转化国家重点实验室自主课题(2020BWZ004)

Regulating the Acid Sites Distribution in ZSM-5 Zeolite and Its Catalytic Performance in the Conversion of Methanol to Olefins

GUO Shujia1,2, WANG Sen1(), ZHANG Li1,2, QIN Zhangfeng1(), WANG Pengfei1, DONG Mei1, WANG Jianguo1,2, FAN Weibin1()   

  1. 1.State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China
    2.University of the Chinese Academy of Sciences,Beijing 100049,China
  • Received:2020-07-01 Online:2021-01-10 Published:2021-01-12
  • Contact: WANG Sen,QIN Zhangfeng,FAN Weibin E-mail:wangsen@sxicc.ac.cn;qzhf@sxicc.ac.cn;fanwb@sxicc.ac.cn
  • Supported by:
    This paper is supported by the National Natural Science Foundation of China(U1910203);the Natural Science Foundation of Shanxi Province, China(201901D211581);the Excellent Doctoral Student Award and Subsidy Program of Shanxi Province, China(BK2018001);the Autonomous Research Project of State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy Sciences(2020BWZ004)

摘要:

ZSM-5分子筛在甲醇制烯烃(MTO)过程中的催化性能和反应机理与其孔道中酸位点分布位置紧密相关. 本文证明在水热合成过程中加入适量的钠离子(Na+)可以增加ZSM-5分子筛交叉腔酸位点比例; 从而促进高级甲基苯的生成并加速芳烃循环, 有利于乙烯生成. 相反, 在合成过程中不添加钠离子, 所制备的ZSM-5分子筛直孔道和正弦孔道酸位点比例明显提高, 有利于促进烯烃循环并提高丙烯和C3+烯烃选择性.

关键词: 甲醇制烯烃, ZSM-5分子筛, 酸位分布, 管理与调控

Abstract:

The catalytic performance and reaction mechanism of ZSM-5 zeolite in the conversion of methanol to olefins(MTO) is closely related to the distribution of acid sites in framework. In this work, it was demonstrated that adding proper content of Na+ ions during synthesis can increase the proportion of acid sites in the intersection cavity of ZSM-5; the concentration of acid sites in the intersection cavity can promote the formation of higher polymethylbenzene(polyMBs) and the propagation of aromatic cycle, forming more ethene. In contrast, in the Na+ ions free synthesis system, more acid sites are distributed in the sinusoidal and straight channels of ZSM-5, which is more encouraging for the alkene cycle and conduces to producing more propene and higher alkenes(C3+).

Key words: Methanol to olefins, ZSM-5 zeolite, Acid sites distribution, Regulation

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