SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2022, Vol. 41 ›› Issue (1): 350-357.DOI: 10.1016/j.cjche.2021.11.019

• Catalysis, Kinetics and Reaction Engineering • 上一篇    下一篇

Importance of metal location in M-H zeolite for synergistically catalyzing dimethyl ether carbonylation

Shiyue Li, Shouying Huang, Kai Cai, Ying Li, Jing Lv, Xinbin Ma   

  1. Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
  • 收稿日期:2021-07-14 修回日期:2021-10-30 出版日期:2022-01-28 发布日期:2022-02-25
  • 通讯作者: Shouying Huang,E-mail address:huangsy@tju.edu.cn;Jing Lv,E-mail address:muddylj@tju.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (21978209, 21325626), the Program of Introducing Talents of Discipline to Universities (BP0618007).

Importance of metal location in M-H zeolite for synergistically catalyzing dimethyl ether carbonylation

Shiyue Li, Shouying Huang, Kai Cai, Ying Li, Jing Lv, Xinbin Ma   

  1. Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
  • Received:2021-07-14 Revised:2021-10-30 Online:2022-01-28 Published:2022-02-25
  • Contact: Shouying Huang,E-mail address:huangsy@tju.edu.cn;Jing Lv,E-mail address:muddylj@tju.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21978209, 21325626), the Program of Introducing Talents of Discipline to Universities (BP0618007).

摘要: Mordenite (MOR) has shown great potential to catalyze dimethyl ether (DME) carbonylation to methyl acetate (MA) in industry. The synergy between metal species and Brønsted acid sites accelerates DME conversion. Here we designed and prepared two catalysts with different Ag locations by seed-directed growth method and two-step impregnation method (named as Ag@HMOR and Ag/HMOR-out, respectively), to explain the effect of Ag location on catalytic performance. The results of TEM, XPS, CO-IR and UV–Vis showed that Ag species mainly presented as Ag0 species over both Ag@HMOR and Ag/HMOR-out. Meanwhile, Ag0 species mainly located in the micropores of Ag@HMOR, while as for Ag/HMOR-out, Ag0 mainly existed on external surface. After comparing the performance of the catalysts with different Ag positions, we confirmed that the Ag0 species encapsulated in the channels of HMOR promoted the DME carbonylation, which revealed the importance of spatial adjacency on the acid-metal catalysts.

关键词: Dimethyl ether, Carbonylation, Silver modification, Metal location

Abstract: Mordenite (MOR) has shown great potential to catalyze dimethyl ether (DME) carbonylation to methyl acetate (MA) in industry. The synergy between metal species and Brønsted acid sites accelerates DME conversion. Here we designed and prepared two catalysts with different Ag locations by seed-directed growth method and two-step impregnation method (named as Ag@HMOR and Ag/HMOR-out, respectively), to explain the effect of Ag location on catalytic performance. The results of TEM, XPS, CO-IR and UV–Vis showed that Ag species mainly presented as Ag0 species over both Ag@HMOR and Ag/HMOR-out. Meanwhile, Ag0 species mainly located in the micropores of Ag@HMOR, while as for Ag/HMOR-out, Ag0 mainly existed on external surface. After comparing the performance of the catalysts with different Ag positions, we confirmed that the Ag0 species encapsulated in the channels of HMOR promoted the DME carbonylation, which revealed the importance of spatial adjacency on the acid-metal catalysts.

Key words: Dimethyl ether, Carbonylation, Silver modification, Metal location