Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol

doi:10.1016/j.cjche.2023.06.008

中国化学工程学报 ›› 2023, Vol. 60 ›› Issue (8): 186-193.DOI: 10.1016/j.cjche.2023.06.008

• Full Length Article • 上一篇下一篇

Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol

Peipei Ai¹, Huiqing Jin¹, Jie Li², Xiaodong Wang¹, Wei Huang¹

1. State Key Laboratory of Clean and Efficient Coal Utilization, College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
2. CAS Key Laboratory of Nanophotonic Materials and Devices & Key Laboratory of Nanodevices and Applications, i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou 215123, China

收稿日期:2023-02-07 修回日期:2023-06-04 出版日期:2023-08-28 发布日期:2023-10-28
通讯作者: Xiaodong Wang,E-mail:wangxiaodong@tyut.edu.cn;Wei Huang,E-mail:huangwei@tyut.edu.cn
基金资助:
This work was financially supported by National Natural Science Foundation of China (22008166); Natural Science Foundation of Shanxi (201901D211047); and Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (2019L0185).

Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol

Peipei Ai¹, Huiqing Jin¹, Jie Li², Xiaodong Wang¹, Wei Huang¹

1. State Key Laboratory of Clean and Efficient Coal Utilization, College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
2. CAS Key Laboratory of Nanophotonic Materials and Devices & Key Laboratory of Nanodevices and Applications, i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou 215123, China

Received:2023-02-07 Revised:2023-06-04 Online:2023-08-28 Published:2023-10-28
Contact: Xiaodong Wang,E-mail:wangxiaodong@tyut.edu.cn;Wei Huang,E-mail:huangwei@tyut.edu.cn
Supported by:
This work was financially supported by National Natural Science Foundation of China (22008166); Natural Science Foundation of Shanxi (201901D211047); and Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (2019L0185).

摘要/Abstract

摘要： Dimethyl oxalate (DMO) hydrogenation is a crucial step in the coal to ethylene glycol (CTEG) process. Herein, Cu catalyst supported on fibrous mesoporous silica (Cu/FMS) was synthesized via liquid phase deposition technique and applied for the DMO hydrogenation to EG. The catalyst exhibited a remarkable EG selectivity of 96.95% and maintained its activity without deactivation for 1000 h. Fibers of FMS support and liquid phase deposition technology cooperated to give high dispersion of Cu species in the Cu/FMS catalyst, resulting in a high Cu surface area. The formation of Si—O—Cu during catalyst preparation process increased the Cu⁺/(Cu⁰ + Cu⁺) ratio and enhanced the thermal and valence stability of Cu species. The high Cu⁺ surface area and Cu stability (thermal and valence stability) of the Cu/FMS catalyst were key factors for achieving superior EG selectivity and ultra-high stability.

关键词: Stability, Cu⁺ surface area, Fibrous mesoporous silica, Catalyst, Hydrogenation

Abstract: Dimethyl oxalate (DMO) hydrogenation is a crucial step in the coal to ethylene glycol (CTEG) process. Herein, Cu catalyst supported on fibrous mesoporous silica (Cu/FMS) was synthesized via liquid phase deposition technique and applied for the DMO hydrogenation to EG. The catalyst exhibited a remarkable EG selectivity of 96.95% and maintained its activity without deactivation for 1000 h. Fibers of FMS support and liquid phase deposition technology cooperated to give high dispersion of Cu species in the Cu/FMS catalyst, resulting in a high Cu surface area. The formation of Si—O—Cu during catalyst preparation process increased the Cu⁺/(Cu⁰ + Cu⁺) ratio and enhanced the thermal and valence stability of Cu species. The high Cu⁺ surface area and Cu stability (thermal and valence stability) of the Cu/FMS catalyst were key factors for achieving superior EG selectivity and ultra-high stability.

Key words: Stability, Cu⁺ surface area, Fibrous mesoporous silica, Catalyst, Hydrogenation

Peipei Ai, Huiqing Jin, Jie Li, Xiaodong Wang, Wei Huang. Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol[J]. 中国化学工程学报, 2023, 60(8): 186-193.

Peipei Ai, Huiqing Jin, Jie Li, Xiaodong Wang, Wei Huang. Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol[J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 186-193.

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Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol

Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol

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