SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2024, Vol. 66 ›› Issue (2): 216-223.DOI: 10.1016/j.cjche.2023.10.008

• Full Length Article • 上一篇    下一篇

Synthesis of mordenite by solvent-free method and its application in the dimethyl ether carbonylation reaction

Yinghui Liu1, Shaoduo Liu1,2, Xiaosheng Wang1, Hongjing Wang1, Ranjia Li1, Changchun Yu1, Chunming Xu1, Yuxiang Liu3, Zhengqiu Xie4, Yongqiang Wang4, Pan Tang4   

  1. 1. State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum-Beijing, Beijing 102249, China;
    2. Synfuels China Technology Co., Ltd, Beijing 101400, China;
    3. College of Chemical Engineering, Qingdao University of Science & Technology, Qingdao 266042, China;
    4. Yueyang Jucheng Chemical Co., Ltd, Yueyang 414009, China
  • 收稿日期:2023-07-05 修回日期:2023-10-14 出版日期:2024-02-28 发布日期:2024-04-20
  • 通讯作者: Xiaosheng Wang,E-mail:wxs880620@cup.edu.cn;Yuxiang Liu,E-mail:liuyx@qust.edu.cn
  • 基金资助:
    This work was supported by China National Natural Science Foundation (22008260 and 21908123).

Synthesis of mordenite by solvent-free method and its application in the dimethyl ether carbonylation reaction

Yinghui Liu1, Shaoduo Liu1,2, Xiaosheng Wang1, Hongjing Wang1, Ranjia Li1, Changchun Yu1, Chunming Xu1, Yuxiang Liu3, Zhengqiu Xie4, Yongqiang Wang4, Pan Tang4   

  1. 1. State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum-Beijing, Beijing 102249, China;
    2. Synfuels China Technology Co., Ltd, Beijing 101400, China;
    3. College of Chemical Engineering, Qingdao University of Science & Technology, Qingdao 266042, China;
    4. Yueyang Jucheng Chemical Co., Ltd, Yueyang 414009, China
  • Received:2023-07-05 Revised:2023-10-14 Online:2024-02-28 Published:2024-04-20
  • Contact: Xiaosheng Wang,E-mail:wxs880620@cup.edu.cn;Yuxiang Liu,E-mail:liuyx@qust.edu.cn
  • Supported by:
    This work was supported by China National Natural Science Foundation (22008260 and 21908123).

摘要: Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether (DME) carbonylation reaction. The influence of Si/Al ratio in the feedstock on the structure, porosity and acid sites were systematically investigated. The characterization results showed that with the increase of Si/Al ratio in the feedstock, part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased. The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio, and the amount of strong acid slightly increased. The Al atoms preferentially enter the strong acid sites in the 8 member ring (MR) channel during the crystallization process. The high Si/Al ratio sample had more acid sites located in the 8 MR channel, leading to more active sites for carbonylation reaction and higher catalytic performance. Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite (MOR) catalyst.

关键词: Carbonylation, Dimethyl ether, Solvent-free, Zeolite, Synthesis, Catalysis

Abstract: Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether (DME) carbonylation reaction. The influence of Si/Al ratio in the feedstock on the structure, porosity and acid sites were systematically investigated. The characterization results showed that with the increase of Si/Al ratio in the feedstock, part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased. The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio, and the amount of strong acid slightly increased. The Al atoms preferentially enter the strong acid sites in the 8 member ring (MR) channel during the crystallization process. The high Si/Al ratio sample had more acid sites located in the 8 MR channel, leading to more active sites for carbonylation reaction and higher catalytic performance. Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite (MOR) catalyst.

Key words: Carbonylation, Dimethyl ether, Solvent-free, Zeolite, Synthesis, Catalysis