Citation: TIAN Tao, QIAN Wei-Zhong, TANG Xiao-Ping, YUN Song, WEI Fei. Deactivation of Ag/ZSM-5 Catalyst in the Aromatization of Methanol[J]. Acta Physico-Chimica Sinica, ;2010, 26(12): 3305-3309. doi: 10.3866/PKU.WHXB20101228 shu

Deactivation of Ag/ZSM-5 Catalyst in the Aromatization of Methanol

TIAN Tao ^1,2 ,
QIAN Wei-Zhong ^1, ,
TANG Xiao-Ping ¹ ,
YUN Song ¹ ,
WEI Fei ¹

1.
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

Received Date: 6 August 2010
Available Online: 16 November 2010
Fund Project: 国家自然科学重点基金(20736004, 20736007) (20736004, 20736007)教育部新世纪优秀人才计划(NECT-07-0489)资助项目 (NECT-07-0489)

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.
- Methanol,
- Aromatization,
- Ag/ZSM-5,
- Deactivation,
- Regeneration
1. [1]
  
  1. Freeman, D.;Well, R. P. K.; Hutchings, G. J. Catal. Lett., 2002, 82(3-4): 217
2. [2]
  2. Haag,W. O.; La , R. M.; Rodewald, P. G. J. Mol. Catal., 1982, 17(2-3): 161
3. [3]
  3. Espinoza, R. L.; Mandersoot,W. G. B. J. Mol. Catal., 1984, 24(1): 127
4. [4]
  4. Stöcker, M. Microporous Mesoporous Mat. 1999, 29: 3
5. [5]
  5. Bjorgen, M.; Kolboe, S. Appl. Catal. A, 2002, 225: 285
6. [6]
  6. Yaragadda, P.; Lund, C. R. F.; Ruckenstein, E. Appl. Catal. A, 1989, 54: 139
7. [7]
  7. Chang, C. D.; Silvestri, A. J. J. Catal., 1977, 47: 249
8. [8]
  8. Kecskeméti, A.; Barthos, R.; Solymosi, F. J. Catal., 2008, 258: 111
9. [9]
  9. Moses, O. A.; Mervyn, A. L. Catal. Commun., 2003, 4: 71
10. [10]
  10. Jiang, Y. X. Guangxi Chem., 1994, 23(3): 40.
11. [11]
  [蒋月秀. 广西化工, 1994, 23(3): 40]
12. [12]
  11. Zaidi, H. A.; Pant, K. K. Catal. Today, 2004, 96: 155
13. [13]
  12. Choudhary, V. R. Zeolites, 1995, 15: 732
14. [14]
  13. Yoshilihiro, I.; Katsumi, N.; Yoshio, O. Microporous Mater., 1995, 4: 373
15. [15]
  14. Tian, T.; Qian,W. Z.; Sun, Y. J.; Cui, Y.; Lu, Y. Y.;Wei, F. Modern Chem. Ind., 2009, 29(1): 55.
16. [16]
  [田涛, 骞伟中, 孙玉建, 崔宇, 卢俨俨, 魏飞. 现代化工, 2009, 29(1): 55]
17. [17]
  15. Wang, X. X.; Chen, X. R.; Chen, C. L.; Xu, N. P. Petroleum Processing and Petrochemicals, 2006, 37(8): 7.
18. [18]
  [王星星, 陈晓蓉, 陈长林, 徐南平. 石油炼制与化工, 2006, 37(8): 7]
19. [19]
  16. Lu, X. D.; Li,W. B.; Yang, C. H.; Dou, X. Y.; Yang, D. Z. Chin. J. Catal., 1992, 13(1): 49.
20. [20]
  [卢学栋, 李文彬, 杨彩虹, 窦秀云, 杨定珠. 催化学报, 1992, 13(1): 49]
21. [21]
  17. Fang, L.; Li, Y. D. Catal. Today, 2009, 145(1-2): 101
22. [22]
  18. Xin, Q. Research methods on solid catalysts. Beijing: Science Press, 2004: 361-366.
23. [23]
  [辛勤. 固体催化剂研究方法. 北京: 科学出版社, 2004: 361-366]
24. [24]
  19. Datka, J.; Marschmeyer, S.; Neubarer, T. J. Phys. Chem., 1996, 100(34): 14451
25. [25]
  20. Sahasrabudhe, A.; Mitra, S.; Tripathi, A. K. Phys. Chem. Chem. Phys., 2003, 5: 3066
26. [26]
  21. Lu, J. M.;Wang, J. Q.; Li, Y. L.; Yin, D. H. Petrochem. Technol., 2004, 33(8): 717.
27. [27]
  [鲁金明, 王金渠, 栗艳玲, 殷德宏. 石油化工, 2004, 33(8): 717]
28. [28]
  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.
29. [29]
  [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]
30. [30]
  23. Lucas, A.; Canizares, P.; Durhn, A. Appl. Catal. A, 1997, 154: 221
1. [1]
  Yunhao Zhang , Yinuo Wang , Siran Wang , Dazhen Xu . Progress in Selective Construction of Functional Aromatics from Nitrogenous Cycloalkanes. University Chemistry, 2024, 39(11): 136-145. doi: 10.3866/PKU.DXHX202401083
2. [2]
  Xingyang LI , Tianju LIU , Yang GAO , Dandan ZHANG , Yong ZHOU , Meng PAN . A superior methanol-to-propylene catalyst: Construction via synergistic regulation of pore structure and acidic property of high-silica ZSM-5 zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1279-1289. doi: 10.11862/CJIC.20240026
3. [3]
  Hengyi ZHU , Liyun JU , Haoyue ZHANG , Jiaxin DU , Yutong XIE , Li SONG , Yachao JIN , Mingdao ZHANG . Efficient regeneration of waste LiNi_0.5Co_0.2Mn_0.3O₂ cathode toward high-performance Li-ion battery. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 625-638. doi: 10.11862/CJIC.20240358
4. [4]
  Xinyu You , Xin Zhang , Shican Jiang , Yiru Ye , Lin Gu , Hexun Zhou , Pandong Ma , Jamal Ftouni , Abhishek Dutta Chowdhury . Efficacy of Ca/ZSM-5 zeolites derived from precipitated calcium carbonate in the methanol-to-olefin process. Chinese Journal of Structural Chemistry, 2024, 43(4): 100265-100265. doi: 10.1016/j.cjsc.2024.100265
5. [5]
  Shanyuan Bi , Jin Zhang , Dengchao Peng , Danhong Cheng , Jianping Zhang , Lupeng Han , Dengsong Zhang . Improved N₂ selectivity for low-temperature NO_x reduction over etched ZSM-5 supported MnCe oxide catalysts. Chinese Chemical Letters, 2025, 36(5): 110295-. doi: 10.1016/j.cclet.2024.110295
6. [6]
  Lisha LEI , Wei YONG , Yiting CHENG , Yibo WANG , Wenchao HUANG , Junhuan ZHAO , Zhongjie ZHAI , Yangbin DING . Application of regenerated cellulose and reduced graphene oxide film in synergistic power generation from moisture electricity generation and Mg-air batteries. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1151-1161. doi: 10.11862/CJIC.20240202
7. [7]
  Kai CHEN , Fengshun WU , Shun XIAO , Jinbao ZHANG , Lihua ZHU . PtRu/nitrogen-doped carbon for electrocatalytic methanol oxidation and hydrogen evolution by water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1357-1367. doi: 10.11862/CJIC.20230350
8. [8]
  Yongmei Liu , Lisen Sun , Zhen Huang , Tao Tu . Curriculum-Based Ideological and Political Design for the Experiment of Methanol Oxidation to Formaldehyde Catalyzed by Electrolytic Silver. University Chemistry, 2024, 39(2): 67-71. doi: 10.3866/PKU.DXHX202308020
9. [9]
  Ling Liu , Haibin Wang , Genrong Qiang . Curriculum Ideological and Political Design for the Comprehensive Preparation Experiment of Ethyl Benzoate Synthesized from Benzyl Alcohol. University Chemistry, 2024, 39(2): 94-98. doi: 10.3866/PKU.DXHX202304080
10. [10]
  Wanmin Cheng , Juan Du , Peiwen Liu , Yiyun Jiang , Hong Jiang . Photoinitiated Grignard Reagent Synthesis and Experimental Improvement in Triphenylmethanol Preparation. University Chemistry, 2024, 39(5): 238-242. doi: 10.3866/PKU.DXHX202311066
11. [11]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028
12. [12]
  Xue Liu , Lipeng Wang , Luling Li , Kai Wang , Wenju Liu , Biao Hu , Daofan Cao , Fenghao Jiang , Junguo Li , Ke Liu . Cu基和Pt基甲醇水蒸气重整制氢催化剂研究进展. Acta Physico-Chimica Sinica, 2025, 41(5): 100049-. doi: 10.1016/j.actphy.2025.100049
13. [13]
  Guangming YIN , Huaiyao WANG , Jianhua ZHENG , Xinyue DONG , Jian LI , Yi'nan SUN , Yiming GAO , Bingbing WANG . Preparation and photocatalytic degradation performance of Ag/protonated g-C₃N₄ nanorod materials. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1491-1500. doi: 10.11862/CJIC.20240086
14. [14]
  Jian Jin , Jing Cheng , Xueping Yang . Integration Practice of Organic Chemistry Experiment and Safety Education: Taking the Synthesis of Triphenylmethanol as an Example. University Chemistry, 2024, 39(3): 345-350. doi: 10.3866/PKU.DXHX202309010
15. [15]
  Feng Han , Fuxian Wan , Ying Li , Congcong Zhang , Yuanhong Zhang , Chengxia Miao . Comprehensive Organic Chemistry Experiment: Phosphotungstic Acid-Catalyzed Direct Conversion of Triphenylmethanol for the Synthesis of Oxime Ethers. University Chemistry, 2025, 40(3): 342-348. doi: 10.12461/PKU.DXHX202405181
16. [16]
  Kexin Dong , Chuqi Shen , Ruyu Yan , Yanping Liu , Chunqiang Zhuang , Shijie Li . Integration of Plasmonic Effect and S-Scheme Heterojunction into Ag/Ag₃PO₄/C₃N₅ Photocatalyst for Boosted Photocatalytic Levofloxacin Degradation. Acta Physico-Chimica Sinica, 2024, 40(10): 2310013-. doi: 10.3866/PKU.WHXB202310013
17. [17]
  Yanxi LIU , Mengjia XU , Haonan CHEN , Quan LIU , Yuming ZHANG . A fluorescent-colorimetric probe for peroxynitrite-anion-imaging in living cells. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1112-1122. doi: 10.11862/CJIC.20240423
18. [18]
  Mingjie Lei , Wenting Hu , Kexin Lin , Xiujuan Sun , Haoshen Zhang , Ye Qian , Tongyue Kang , Xiulin Wu , Hailong Liao , Yuan Pan , Yuwei Zhang , Diye Wei , Ping Gao . Co/Mn/Mo掺杂加速NiSe₂重构以提高其电催化尿素氧化性能. Acta Physico-Chimica Sinica, 2025, 41(8): 100083-. doi: 10.1016/j.actphy.2025.100083
19. [19]
  Rui Gao , Ying Zhou , Yifan Hu , Siyuan Chen , Shouhong Xu , Qianfu Luo , Wenqing Zhang . Design, Synthesis and Performance Experiment of Novel Photoswitchable Hybrid Tetraarylethenes. University Chemistry, 2024, 39(5): 125-133. doi: 10.3866/PKU.DXHX202310050
20. [20]
  Nan Xiao , Fang Sun . 二芳基硫醚化合物的构建及应用. University Chemistry, 2025, 40(6): 360-363. doi: 10.12461/PKU.DXHX202407099

Get Citation

PDF

XML

Metrics

PDF Downloads(1339)
Abstract views(3089)
HTML views(6)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142