Please wait a minute...
Acta Physico-Chimica Sinica  2010, Vol. 26 Issue (12): 3305-3309    DOI: 10.3866/PKU.WHXB20101228
CATALYSIS AND SURFACE STRUCTURE     
Deactivation of Ag/ZSM-5 Catalyst in the Aromatization of Methanol
TIAN Tao1,2, QIAN Wei-Zhong1, TANG Xiao-Ping1, YUN Song1, WEI Fei1
1. Beijing Key Laboratory of Green Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, P. R. China;

2. Economics & Development Research Institute, SINOPEC, Beijing 100029, P. R. China
Download:   PDF(1204KB) Export: BibTeX | EndNote (RIS)      

Abstract  

The deactivation and regeneration properties of the methanol aromatization catalyst, Ag/ ZSM-5, were investigated by a continuous reaction-catalyst regeneration experiment over four cycles. The activity of the catalyst decreased gradually over the long reaction and was only partly recovered after coke burning. Characterization of the regenerated catalyst by X-ray diffraction (XRD) and transmission electron microscope (TEM) revealed that the ZSM-5 framework remained unchanged and that the sintering of the Ag nanoparticles was not serious. Analyses by Fourier transform Infrared spectroscopy (FTIR) and ammonia-temperature programmed desorption (NH3-TPD) experiment confirmed that the hydrothermal de-alumination of the catalyst by water in large amounts at 475 °C during aromatization resulted in a significant loss of Brønsted acidity. Consequently, an irreversible decrease in the aromatization ability of the catalyst was apparent.



Key wordsMethanol      Aromatization      Ag/ZSM-5      Deactivation      Regeneration     
Received: 06 August 2010      Published: 16 November 2010
MSC2000:  O643  
Fund:  

The project was supported by the National Natural Science Foundation of China (20736004, 20736007) and Program for New Century Excellent Talents in Universities of the Ministry of Education of China (NECT-07-0489).

Corresponding Authors: QIAN Wei-Zhong     E-mail: qianwz@mail.tsinghua.edu.cn
Cite this article:

TIAN Tao, QIAN Wei-Zhong, TANG Xiao-Ping, YUN Song, WEI Fei. Deactivation of Ag/ZSM-5 Catalyst in the Aromatization of Methanol. Acta Physico-Chimica Sinica, 2010, 26(12): 3305-3309.

URL:

http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/10.3866/PKU.WHXB20101228     OR     http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/Y2010/V26/I12/3305

1. Freeman, D.;Well, R. P. K.; Hutchings, G. J. Catal. Lett., 2002, 82(3-4): 217
2. Haag,W. O.; Lago, R. M.; Rodewald, P. G. J. Mol. Catal., 1982, 17(2-3): 161
3. Espinoza, R. L.; Mandersoot,W. G. B. J. Mol. Catal., 1984, 24(1): 127
4. Stöcker, M. Microporous Mesoporous Mat. 1999, 29: 3
5. Bjorgen, M.; Kolboe, S. Appl. Catal. A, 2002, 225: 285
6. Yaragadda, P.; Lund, C. R. F.; Ruckenstein, E. Appl. Catal. A, 1989, 54: 139
7. Chang, C. D.; Silvestri, A. J. J. Catal., 1977, 47: 249
8. Kecskeméti, A.; Barthos, R.; Solymosi, F. J. Catal., 2008, 258: 111
9. Moses, O. A.; Mervyn, A. L. Catal. Commun., 2003, 4: 71
10. Jiang, Y. X. Guangxi Chem., 1994, 23(3): 40.
[蒋月秀. 广西化工, 1994, 23(3): 40]
11. Zaidi, H. A.; Pant, K. K. Catal. Today, 2004, 96: 155
12. Choudhary, V. R. Zeolites, 1995, 15: 732
13. Yoshilihiro, I.; Katsumi, N.; Yoshio, O. Microporous Mater., 1995, 4: 373
14. Tian, T.; Qian,W. Z.; Sun, Y. J.; Cui, Y.; Lu, Y. Y.;Wei, F. Modern Chem. Ind., 2009, 29(1): 55.
[田涛, 骞伟中, 孙玉建, 崔宇, 卢俨俨, 魏飞. 现代化工, 2009, 29(1): 55]
15. Wang, X. X.; Chen, X. R.; Chen, C. L.; Xu, N. P. Petroleum Processing and Petrochemicals, 2006, 37(8): 7.
[王星星, 陈晓蓉, 陈长林, 徐南平. 石油炼制与化工, 2006, 37(8): 7]
16. Lu, X. D.; Li,W. B.; Yang, C. H.; Dou, X. Y.; Yang, D. Z. Chin. J. Catal., 1992, 13(1): 49.
[卢学栋, 李文彬, 杨彩虹, 窦秀云, 杨定珠. 催化学报, 1992, 13(1): 49]
17. Fang, L.; Li, Y. D. Catal. Today, 2009, 145(1-2): 101
18. Xin, Q. Research methods on solid catalysts. Beijing: Science Press, 2004: 361-366.
[辛勤. 固体催化剂研究方法. 北京: 科学出版社, 2004: 361-366]
19. Datka, J.; Marschmeyer, S.; Neubarer, T. J. Phys. Chem., 1996, 100(34): 14451
20. Sahasrabudhe, A.; Mitra, S.; Tripathi, A. K. Phys. Chem. Chem. Phys., 2003, 5: 3066
21. Lu, J. M.;Wang, J. Q.; Li, Y. L.; Yin, D. H. Petrochem. Technol., 2004, 33(8): 717.
[鲁金明, 王金渠, 栗艳玲, 殷德宏. 石油化工, 2004, 33(8): 717]
22. Hou, H. D.; Huang, C. P.; Chen, B. H.; Li, Y. X.; He, J. J. Beijing Univ. Chem. Techn.(Natural Sci. Ed.), 2005, 32(4): 10.
[侯焕娣, 黄崇品, 陈标华, 李英霞, 贺杰. 北京化工大学学报: 自然科学 版, 2005, 32(4): 10]
23. Lucas, A.; Canizares, P.; Durhn, A. Appl. Catal. A, 1997, 154: 221

[1] YI Yanhui, WANG Xunxun, WANG Li, YAN Jinhui, ZHANG Jialiang, GUO Hongchen. Plasma-Triggered CH3OH/NH3 Coupling Reaction for Synthesis of Nitrile Compounds[J]. Acta Physico-Chimica Sinica, 2018, 34(3): 247-255.
[2] QIAN Hui-Hui, HAN Xiao, ZHAO Yan, SU Yu-Qin. Flexible Pd@PANI/rGO Paper Anode for Methanol Fuel Cells[J]. Acta Physico-Chimica Sinica, 2017, 33(9): 1822-1827.
[3] YANG Yi, LUO Lai-Ming, CHEN Di, LIU Hong-Ming, ZHANG Rong-Hua, DAI Zhong-Xu, ZHOU Xin-Wen. Synthesis and Electrocatalytic Properties of PtPd Nanocatalysts Supported on Graphene for Methanol Oxidation[J]. Acta Physico-Chimica Sinica, 2017, 33(8): 1628-1634.
[4] QIU Jian-Ping, TONG Yi-Wen, ZHAO De-Ming, HE Zhi-Qiao, CHEN Jian-Meng, SONG Shuang. Electrochemical Reduction of CO2 to Methanol at TiO2 Nanotube Electrodes[J]. Acta Physico-Chimica Sinica, 2017, 33(7): 1411-1420.
[5] WEI Chun-Lei, GAO Jie, WANG Kai, DONG Mei, FAN Wei-Bin, QIN Zhang-Feng, WANG Jian-Guo. Effect of Hydrogen pre-treatment on the catalytic properties of Zn/HZSM-5 zeolite for ethylene aromatization reaction[J]. Acta Physico-Chimica Sinica, 2017, 33(7): 1483-1491.
[6] ZHAN Lin-Jun, SUN Xiao-Yan, ZHOU Ying, ZHU Qiu-Lian, CHEN Yin-Fei, Lu Han-Feng. Deactivation Mechanism of CeO2-Based Mixed Oxide Catalysts Supported on SiO2[J]. Acta Physico-Chimica Sinica, 2017, 33(7): 1474-1482.
[7] HU Yi-Hao, SONG Tong-Yang, WANG Yue-Juan, HU Geng-Sheng, XIE Guan-Qun, LUO Meng-Fei. Gas Phase Dehydrochlorination of 1,1,2-Trichloroethane over Zn/SiO2 Catalysts: Acidity and Deactivation[J]. Acta Physico-Chimica Sinica, 2017, 33(5): 1017-1026.
[8] LI Ling-Ling, CHEN Ren, DAI Jian, SUN Ye, ZHANG Zuo-Liang, LI Xiao-Liang, NIE Xiao-Wa, SONG Chun-Shan, GUO Xin-Wen. Reaction Mechanism of Benzene Methylation with Methanol over H-ZSM-5 Catalyst[J]. Acta Physico-Chimica Sinica, 2017, 33(4): 769-779.
[9] LIU Zhao-Xin, LI Wei-Bin. Catalytic Activity and Deactivation of Toluene Combustion on Rod-Like Copper-Manganese Mixed Oxides[J]. Acta Physico-Chimica Sinica, 2016, 32(7): 1795-1800.
[10] YUAN Ping, WANG Hao, XUE Yan-Feng, LI Yan-Chun, WANG Kai, DONG Mei, FAN Wei-Bin, QIN Zhang-Feng, WANG Jian-Guo. Catalytic Properties of Different Crystal Sizes for ZSM-5 Zeolites on the Alkylation of Benzene with Methanol and Optimization of the Reaction Conditions[J]. Acta Physico-Chimica Sinica, 2016, 32(7): 1775-1784.
[11] HU Si, ZHANG Qing, GONG Yan-Jun, ZHANG Ying, WU Zhi-Jie, DOU Tao. Deactivation and Regeneration of HZSM-5 Zeolite in Methanol-to-Propylene Reaction[J]. Acta Physico-Chimica Sinica, 2016, 32(7): 1785-1794.
[12] TIAN Chun-Xia, YANG Jun-Shuai, LI Li, ZHANG Xiao-Hua, CHEN Jin-Hua. New Methanol-Tolerant Oxygen Reduction Electrocatalyst——Nitrogen-Doped Hollow Carbon Microspheres@Platinum Nanoparticles Hybrids[J]. Acta Physico-Chimica Sinica, 2016, 32(6): 1473-1481.
[13] ZHAO Jun-Feng, SUN Xiao-Li, HUANG Xu-Ri, LI Ji-Lai. A Theoretical Study on the Reactivity and Charge Effect of PtRu Clusters toward Methanol Activation[J]. Acta Physico-Chimica Sinica, 2016, 32(5): 1175-1182.
[14] LIU Jian-Hong, Lü Cun-Qin, JIN Chun, WANG Gui-Chang. First-Principles Study of Effect of CO to Oxidize Methanol to Formic Acid in Alkaline Media on PtAu(111) and Pt(111) Surfaces[J]. Acta Physico-Chimica Sinica, 2016, 32(4): 950-960.
[15] CHENG Xiao-Meng, LI Yu, CHEN Zong, LI Hong-Ping, ZHENG Xiao-Fang. A Comparative Study on theNMR Relaxation of Methanol in Sub-and Super-Critical Mixtures of CO2 and Methanol[J]. Acta Physico-Chimica Sinica, 2016, 32(11): 2671-2677.