SCI和EI收录∣中国化工学会会刊

›› 2016, Vol. 24 ›› Issue (12): 1735-1741.DOI: 10.1016/j.cjche.2016.09.008

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

Catalytic kinetics of dimethyl ether one-step synthesis over CeO2-CaO-Pd/HZSM-5 catalyst in sulfur-containing syngas process

Ruizhi Chu1,2, Wenxin Hou1, Xianliang Meng1,2, Tingting Xu1, Zhenyong Miao1, Guoguang Wu1, Lei Bai3   

  1. 1 School of Chemical Engineering and Technology, China University of Mining & Technology, Xuzhou 221116, China;
    2 High-Tech Research Institute of China University of Mining and Technology, Lianyungang 222000, China;
    3 Department of Chemical and Biomedical Engineering, West Virginia University, Morgantown 26506, USA
  • 收稿日期:2016-08-01 修回日期:2016-09-07 出版日期:2016-12-28 发布日期:2017-01-04
  • 通讯作者: Xianliang Meng,E-mail address:hwxcumt@163.com
  • 基金资助:
    Supported by the National Natural Science Foundation of China (51204179, 51204182, 51674256) and The Natural Science Foundation of Jiangsu Province, China (BK20141242).

Catalytic kinetics of dimethyl ether one-step synthesis over CeO2-CaO-Pd/HZSM-5 catalyst in sulfur-containing syngas process

Ruizhi Chu1,2, Wenxin Hou1, Xianliang Meng1,2, Tingting Xu1, Zhenyong Miao1, Guoguang Wu1, Lei Bai3   

  1. 1 School of Chemical Engineering and Technology, China University of Mining & Technology, Xuzhou 221116, China;
    2 High-Tech Research Institute of China University of Mining and Technology, Lianyungang 222000, China;
    3 Department of Chemical and Biomedical Engineering, West Virginia University, Morgantown 26506, USA
  • Received:2016-08-01 Revised:2016-09-07 Online:2016-12-28 Published:2017-01-04
  • Supported by:
    Supported by the National Natural Science Foundation of China (51204179, 51204182, 51674256) and The Natural Science Foundation of Jiangsu Province, China (BK20141242).

摘要: CeO2-CaO-Pd/HZSM-5 catalyst was prepared for the dimethyl ether (DME) one-step synthesis in a continuous fixed-bed micro-reactor from the sulfur-containing syngas. The catalytic stability over hybrid catalyst of CeO2-CaO-Pd/HZSM-5 was investigated to ensure that the kinetics experimental results were not significantly influenced by induction period and catalytic deactivation. A large number of kinetic data points (40 sets) were obtained over a range of temperature (240-300℃), pressure (3-4 MPa), gas hourly space velocity (GHSV) (2000-3000 L·kg-1·h-1) and H2/CO mole ratio (2-3). Kinetic model for the methanol synthesis reaction and the dehydration of methanol were obtained separately according to reaction mechanism and Langmuir-Hinshelwood mechanism. Regression parameters were investigated by the method combining the simplex method and Runge-Kutta method. The model calculations were in appropriate accordance with the experimental data.

关键词: CeO2-CaO-Pd/HZSM-5 catalyst, DME, One-step synthesis, Catalytic kinetics, Sulfur-containing syngas

Abstract: CeO2-CaO-Pd/HZSM-5 catalyst was prepared for the dimethyl ether (DME) one-step synthesis in a continuous fixed-bed micro-reactor from the sulfur-containing syngas. The catalytic stability over hybrid catalyst of CeO2-CaO-Pd/HZSM-5 was investigated to ensure that the kinetics experimental results were not significantly influenced by induction period and catalytic deactivation. A large number of kinetic data points (40 sets) were obtained over a range of temperature (240-300℃), pressure (3-4 MPa), gas hourly space velocity (GHSV) (2000-3000 L·kg-1·h-1) and H2/CO mole ratio (2-3). Kinetic model for the methanol synthesis reaction and the dehydration of methanol were obtained separately according to reaction mechanism and Langmuir-Hinshelwood mechanism. Regression parameters were investigated by the method combining the simplex method and Runge-Kutta method. The model calculations were in appropriate accordance with the experimental data.

Key words: CeO2-CaO-Pd/HZSM-5 catalyst, DME, One-step synthesis, Catalytic kinetics, Sulfur-containing syngas