Study on attrition of spherical-shaped Mo/HZSM-5 catalyst for methane dehydro-aromatization in a gas-solid fluidized bed

doi:10.1016/j.cjche.2021.03.025

中国化学工程学报 ›› 2021, Vol. 38 ›› Issue (10): 172-183.DOI: 10.1016/j.cjche.2021.03.025

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

Study on attrition of spherical-shaped Mo/HZSM-5 catalyst for methane dehydro-aromatization in a gas-solid fluidized bed

Xinzhuang Zhang^1,2,3,4,5,6, Yunda Han^1,3,4,5,6, Dapeng Li⁷, Zhanguo Zhang⁸, Xiaoxun Ma^1,3,4,5,6,9

1. School of Chemical Engineering, Northwest University, Xi’an 710069, China;
2. Research Institute of Shaanxi Yanchang Petroleum (Group) Co., Ltd., Xi’an 710065, China;
3. Chemical Engineering Research Center of the Ministry of Education (MOE) for Advanced Use Technology of Shanbei Energy, Xi’an 710069, China;
4. Shaanxi Research Center of Engineering Technology for Clean Coal Conversion, Xi’an 710069, China;
5. Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Xi’an 710069, China;
6. International Scientific and Technological Cooperation Base of the Ministry of Science and Technology (MOST) for Clean Utilization of Hydrocarbon Resources, Xi’an 710069, China;
7. Hydrocarbon High-efficiency Utilization Technology Research Center of Shaanxi Yanchang Petroleum (Group) Co., Ltd., Xi’an 710065, China;
8. Key Laboratory on Resources Chemicals and Materials, Shenyang University of Chemical Technology, Shenyang 110142, China;
9. Longdong University, Xifeng District, Qingyang 745000, China

收稿日期:2020-12-17 修回日期:2021-03-17 出版日期:2021-10-28 发布日期:2021-12-02
通讯作者: Xiaoxun Ma
基金资助:
This work was supported by Hydrocarbon High-efficiency Utilization Technology Research Center of Shaanxi Yanchang Petroleum (Group) Co., Ltd., China (Contract No. HCRC-C13-010), and the National Natural Science Foundation of China (No. 21536009). The authors also would like to acknowledge Northwest University and Shaanxi Yanchang Petroleum (Group) Co., Ltd. for affording the opportunity to participate in relevant research projects, and appreciate Jialiang Gao and Gen Zhang for their help in SEM analysis of catalysts, Baoqiang Wu for his help in TGA of catalysts.

Study on attrition of spherical-shaped Mo/HZSM-5 catalyst for methane dehydro-aromatization in a gas-solid fluidized bed

Xinzhuang Zhang^1,2,3,4,5,6, Yunda Han^1,3,4,5,6, Dapeng Li⁷, Zhanguo Zhang⁸, Xiaoxun Ma^1,3,4,5,6,9

1. School of Chemical Engineering, Northwest University, Xi’an 710069, China;
2. Research Institute of Shaanxi Yanchang Petroleum (Group) Co., Ltd., Xi’an 710065, China;
3. Chemical Engineering Research Center of the Ministry of Education (MOE) for Advanced Use Technology of Shanbei Energy, Xi’an 710069, China;
4. Shaanxi Research Center of Engineering Technology for Clean Coal Conversion, Xi’an 710069, China;
5. Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Xi’an 710069, China;
6. International Scientific and Technological Cooperation Base of the Ministry of Science and Technology (MOST) for Clean Utilization of Hydrocarbon Resources, Xi’an 710069, China;
7. Hydrocarbon High-efficiency Utilization Technology Research Center of Shaanxi Yanchang Petroleum (Group) Co., Ltd., Xi’an 710065, China;
8. Key Laboratory on Resources Chemicals and Materials, Shenyang University of Chemical Technology, Shenyang 110142, China;
9. Longdong University, Xifeng District, Qingyang 745000, China

Received:2020-12-17 Revised:2021-03-17 Online:2021-10-28 Published:2021-12-02
Contact: Xiaoxun Ma
Supported by:
This work was supported by Hydrocarbon High-efficiency Utilization Technology Research Center of Shaanxi Yanchang Petroleum (Group) Co., Ltd., China (Contract No. HCRC-C13-010), and the National Natural Science Foundation of China (No. 21536009). The authors also would like to acknowledge Northwest University and Shaanxi Yanchang Petroleum (Group) Co., Ltd. for affording the opportunity to participate in relevant research projects, and appreciate Jialiang Gao and Gen Zhang for their help in SEM analysis of catalysts, Baoqiang Wu for his help in TGA of catalysts.

摘要/Abstract

摘要： As a potential methane efficient conversion process, non-oxidative aromatization of methane in fluidized bed requires a catalyst with good attrition resistance, especially in the states of high temperature, long-time rapid movement and chemical reaction. Existing evaluation methods for attrition resistance, such as ASTM D5757 and Jet Cup test, are targeted for fresh catalysts at ambient temperature, which cannot well reflect the real process. In this study, spherical-shaped Mo/HZSM-5 catalyst prepared by dipping and spray drying was placed in a self-made apparatus for attrition testing, in which the catalyst attrition under different system temperatures, running time and process factors was investigated with percent mass loss (PML), particle size-mass distribution (PSMD) and scanning electron microscope (SEM). Carbon deposition on the catalyst before and after activation, aromatization and regeneration was analyzed by thermogravimetry (TG), and the attrited catalysts were evaluated for methane dehydro-aromatization (MDA). The results show that the surface abrasion and body breakage of catalyst particles occur continuously, with the increase of system temperature and running time, and make the PML rise gradually. The process factors of activation, aromatization and regeneration can cause the catalyst attrition and carbon deposits, which broaden the PSMD in varying degrees, and the carbon-substances on catalysts greatly improve their attrition resistance at high temperature. Catalyst attrition has a certain influence on its catalytic performance, and the main reasons point to particle breakage and fine powder escape.

关键词: Attrition, Mo/HZSM-5, Fluidized-bed, Catalyst activation, Methane dehydro-aromatization

Abstract: As a potential methane efficient conversion process, non-oxidative aromatization of methane in fluidized bed requires a catalyst with good attrition resistance, especially in the states of high temperature, long-time rapid movement and chemical reaction. Existing evaluation methods for attrition resistance, such as ASTM D5757 and Jet Cup test, are targeted for fresh catalysts at ambient temperature, which cannot well reflect the real process. In this study, spherical-shaped Mo/HZSM-5 catalyst prepared by dipping and spray drying was placed in a self-made apparatus for attrition testing, in which the catalyst attrition under different system temperatures, running time and process factors was investigated with percent mass loss (PML), particle size-mass distribution (PSMD) and scanning electron microscope (SEM). Carbon deposition on the catalyst before and after activation, aromatization and regeneration was analyzed by thermogravimetry (TG), and the attrited catalysts were evaluated for methane dehydro-aromatization (MDA). The results show that the surface abrasion and body breakage of catalyst particles occur continuously, with the increase of system temperature and running time, and make the PML rise gradually. The process factors of activation, aromatization and regeneration can cause the catalyst attrition and carbon deposits, which broaden the PSMD in varying degrees, and the carbon-substances on catalysts greatly improve their attrition resistance at high temperature. Catalyst attrition has a certain influence on its catalytic performance, and the main reasons point to particle breakage and fine powder escape.

Key words: Attrition, Mo/HZSM-5, Fluidized-bed, Catalyst activation, Methane dehydro-aromatization

Xinzhuang Zhang, Yunda Han, Dapeng Li, Zhanguo Zhang, Xiaoxun Ma. Study on attrition of spherical-shaped Mo/HZSM-5 catalyst for methane dehydro-aromatization in a gas-solid fluidized bed[J]. 中国化学工程学报, 2021, 38(10): 172-183.

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Study on attrition of spherical-shaped Mo/HZSM-5 catalyst for methane dehydro-aromatization in a gas-solid fluidized bed

Study on attrition of spherical-shaped Mo/HZSM-5 catalyst for methane dehydro-aromatization in a gas-solid fluidized bed

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