Citation: LUO Hong-Cheng, HUANG Bi-Chun, FU Ming-Li, WU Jun-Liang, YE Dai-Qi. SO₂ Deactivation Mechanism of MnO_x/MWCNTs Catalyst for Low-Temperature Selective Catalytic Reduction of NOx by Ammonia[J]. Acta Physico-Chimica Sinica doi: 10.3866/PKU.WHXB201207062 shu

SO₂ Deactivation Mechanism of MnO_x/MWCNTs Catalyst for Low-Temperature Selective Catalytic Reduction of NOx by Ammonia

LUO Hong-Cheng ¹ ,
HUANG Bi-Chun ^1,2, ,
FU Ming-Li ^1,2 ,
WU Jun-Liang ^1,2 ,
YE Dai-Qi ^1,2

1.
1. College of Environmental Science and Engineering, South China University of Technology, Guangzhou 510006, P. R. China;
2. Key Laboratory of the Ministry of Education for Pollution Control and Ecosystem Restoration in Industry Clusters, South China University of Technology, Guangzhou 510006, P. R. China

Received Date: 18 June 2012
Available Online: 6 July 2012
Fund Project: 国家自然科学基金(209077034)资助项目 (209077034)

Manganese oxides supported on multi-walled carbon nanotubes (MnO_x/MWCNTs) catalysts were prepared by pore volume impregnation using MWCNTs as the catalyst support which was pretreated by concentrated nitric acid and oxygen dielectric barrier discharge plasma. The catalysts were characterized by thermogravimetric analysis (TGA), scanning electron microscopy (SEM), X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction/desorption (TPR/ TPD), and Fourier transform infrared (FTIR) spectroscopy. The effect of SO₂ on the activity of the catalysts for low-temperature selective catalytic reduction (SCR) of NOx by ammonia and the SO₂ poisoning mechanism were investigated. The results showed that SO₂ had an obvious poisoning effect on the SCR activity of MnO_x/MWCNTs at low temperature. The activity decreased more rapidly as reaction temperature and SO₂ concentration increased. The observed deactivation was attributed to the sulfation of the active center atoms. Formation of ammonium sulfate on the catalyst surface and the inhibiting effect of SO₂ on NO adsorption also resulted in the deactivation of the catalysts to some extent.
- Multi-walled carbon nanotubes,
- Selective catalytic reduction,
- Sulfur dioxide,
- Poisoning mechanism
1. [1]
  
  (1) Busca, G.; Lietti, L.; Ramis, G.; Berti, F. Appl. Catal. B 1998,18, 1. doi: 10.1016/S0926-3373(98)00040-X
2. [2]
  (2) Notoya, F.; Su, C.; Sasaoka, E. Ind. Eng. Chem. Res. 2001, 40,3732. doi: 10.1021/ie000972f
3. [3]
  (3) Huang, J. H.; Tong, Z. Q.; Huang, Y.; Zhang, J. F. Appl. Catal. B2008, 78, 309. doi: 10.1016/j.apcatb.2007.09.031
4. [4]
  (4) Lin, T.; Zhang, Q. L.; Li,W.; ng, M. C.; Xing, Y. X.; Chen, Y.Q. Acta Phys. -Chim. Sin. 2008, 24, 1127. [林涛, 张秋林,李伟, 龚茂初, 幸怡汛, 陈耀强. 物理化学学报, 2008, 24,1127.] doi: 10.1016/S1872-1508(08)60046-7
5. [5]
  (5) Qi, G.; Yang, R. T. Appl. Catal. B 2003, 44, 217. doi: 10.1016/S0926-3373(03)00100-0
6. [6]
  (6) Smirniotis, P. G.; Pena, D. A.; Uphade, B. S. Angew. Chem. Int. Edit. 2001, 40, 2479. doi: 10.1002/1521-3773(20010702)40:13<2479::AID-ANIE2479>3.0.CO;2-7
7. [7]
  (7) Wang, L. S.; Huang, B. C.; Su, Y. X.; Zhou, G. Y.;Wang, K. L.;Luo, H. C.; Ye, D. Q. J. Chem. Eng. 2012, 192, 232. doi: 10.1016/j.cej.2012.04.012
8. [8]
  (8) Kijlstra,W. S.; Biervliet, M.; Poels, E. K.; Bliek, A. Appl. Catal. B 1998, 16, 327. doi: 10.1016/S0926-3373(97)00089-1
9. [9]
  (9) Xie, G. Y.; Liu, Z. Y.; Zhu, Z. P.; Liu, Q. Y.; Ge, J.; Huang, Z. G.J. Catal. 2004, 224, 36. doi: 10.1016/j.jcat.2004.02.015
10. [10]
  (10) Shen, B. X.; Liu, T. Acta Phys. -Chim. Sin. 2010, 26, 3009. [沈伯雄, 刘亭. 物理化学学报, 2010, 26, 3009.] doi: 10.3866/PKU.WHXB20101120
11. [11]
  (11) Jiang, B. Q.;Wu, Z. B.; Liu, Y.; Lee, S. C.; Ho,W. K. J. Phys. Chem. C 2010, 114, 4961. doi: 10.1021/jp907783g
12. [12]
  (12) Forzatti, P.; Lietti, L. Catal. Taday 1999, 62, 51.
13. [13]
  (13) Svachula, J.; Ferlazzo, N.; Forzatti, P.; Tronconi, E.; Bregani, F.Ind. Eng. Chem. Res. 1993, 32, 826. doi: 10.1021/ie00017a009
14. [14]
  (14) Cao, Z. L.;Wang, Z. Y. Inorganic Chemistry Formula Manual;Hunan Science and Technology Press: Changsha, 1972; p 171.[曹忠良, 王珍云. 无机化学方程式手册. 长沙: 湖南科学技术出版社, 1972: 171.]
15. [15]
  (15) Venezia, A. M.; Carlo, G. D.; Pantaleo, G.; Liotta, L. F.; Melaet,G.; Kruse, N. Appl. Catal. B 2009, 88, 430. doi: 10.1016/j.apcatb.2008.10.023
16. [16]
  (16) Reddy, B. M.; Sreekanth, P. M.; Yamada, Y.; Xu, Q.; Kobayashi,T. Appl. Catal. A 2002, 228, 269. doi: 10.1016/S0926-860X(01)00982-6
17. [17]
  (17) Román, E.; de Se via, J. L.; Martín-Ga , J. A.; Comtet, G.;Hellner, L. Vacuum 1997, 48, 597. doi: 10.1016/S0042-207X(97)00074-2
18. [18]
  (18) Romano, E. J.; Schulz, K. H. Appl. Surf. Sci. 2004, 246, 262.
19. [19]
  (19) Liu, J.; Zhao, Z.;Wang, J. Q.; Xu, C. M.; Duan, A. J.; Jiang, G.Y.; Yang, Q. Appl. Catal. B 2008, 84, 185. doi: 10.1016/j.apcatb.2008.03.017
20. [20]
  (20) Macleod, N.; Cropley, R.; Lambert, R. M. Catal. Lett. 2003, 86,69. doi: 10.1023/A:1022611109139
21. [21]
  (21) Jin, R. B.; Liu, Y.;Wu, Z. B.;Wang, H. Q.; Gu, T. T. Catal. Today 2010, 153, 84. doi: 10.1016/j.cattod.2010.01.039
22. [22]
  (22) Takagi, M.; Kawai, T.; Soma, M.; Onishi, T.; Tamaru, K.J. Phys. Chem. 1976, 80, 430. doi: 10.1021/j100545a019
23. [23]
  (23) Lin, S. D.; Gluhoi, A. C.; Nieuwenhuys, B. E. Catal. Today2004, 90, 3. doi: 10.1016/j.cattod.2004.04.047
24. [24]
  (24) Yang, S. X.; Li, X.; Zhu,W. P.;Wang, J. B.; Descorme, C.Carbon 2008, 46, 445. doi: 10.1016/j.carbon.2007.12.006
25. [25]
  (25) Lambia, M. A.; Ramis, G.; Busca, G. Appl. Catal. B 2000, 27,145. doi: 10.1016/S0926-3373(00)00150-8
26. [26]
  (26) Wang,W. H.; Huang, B. C.;Wang, L. S.; Ye, D. Q. Surf. Coat. Technol. 2011, 205, 4896. doi: 10.1016/j.surfcoat.2011.04.100
27. [27]
  (27) Luo, J.; Tong, Z. Q.; Huang, Y.; Xia, B.; Luo, H. Acta. Sci. Circumst. 2010, 30, 1023. [罗晶, 童志权, 黄妍, 夏斌,罗河. 环境科学学报, 2010, 30, 1023.]
28. [28]
  (28) Hadjiivanov, K.; Avreyska, V.; Klissurski, D.; Marinova, T.Langmuir 2002, 18, 1619. doi: 10.1021/la0110895
29. [29]
  (29) Pirngruber, G. D.; Pieterse, J. A. Z. J. Catal. 2006, 237, 237.doi: 10.1016/j.jcat.2005.11.012
30. [30]
  (30) Zhang, X.; Ji, L. Y.; Zhang, S. C.; Yang,W. S. J. Power Sources2007, 173, 1017. doi: 10.1016/j.jpowsour.2007.08.083
31. [31]
  (31) Xu,W. Q.; Hong, H.; Yu, Y. B. J. Phys. Chem. C 2009, 113,4426. doi: 10.1021/jp8088148
1. [1]
  Xiufang Wang , Donglin Zhao , Kehua Zhang , Xiaojie Song . “Preparation of Carbon Nanotube/SnS₂ Photoanode Materials”: A Comprehensive University Chemistry Experiment. University Chemistry, doi: 10.3866/PKU.DXHX202308025
2. [2]
  Hailang JIA , Hongcheng LI , Pengcheng JI , Yang TENG , Mingyun GUAN . Preparation and performance of N-doped carbon nanotubes composite Co₃O₄ as oxygen reduction reaction electrocatalysts. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20230402
3. [3]
  Zhiquan Zhang , Baker Rhimi , Zheyang Liu , Min Zhou , Guowei Deng , Wei Wei , Liang Mao , Huaming Li , Zhifeng Jiang . Insights into the Development of Copper-based Photocatalysts for CO₂ Conversion. Acta Physico-Chimica Sinica, doi: 10.3866/PKU.WHXB202406029
4. [4]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20230385
5. [5]
  Haihua Yang , Minjie Zhou , Binhong He , Wenyuan Xu , Bing Chen , Enxiang Liang . Synthesis and Electrocatalytic Performance of Iron Phosphide@Carbon Nanotubes as Cathode Material for Zinc-Air Battery: a Comprehensive Undergraduate Chemical Experiment. University Chemistry, doi: 10.12461/PKU.DXHX202405100
6. [6]
  Shihui Shi , Haoyu Li , Shaojie Han , Yifan Yao , Siqi Liu . Regioselectively Synthesis of Halogenated Arenes via Self-Assembly and Synergistic Catalysis Strategy. University Chemistry, doi: 10.3866/PKU.DXHX202312002
7. [7]
  Yinuo Wang , Siran Wang , Yilong Zhao , Dazhen Xu . Selective Synthesis of Diarylmethyl Anilines and Triarylmethanes via Multicomponent Reactions: Introduce a Comprehensive Experiment of Organic Chemistry. University Chemistry, doi: 10.3866/PKU.DXHX202401063
8. [8]
  Linbao Zhang , Weisi Guo , Shuwen Wang , Ran Song , Ming Li . Electrochemical Oxidation of Sulfides to Sulfoxides. University Chemistry, doi: 10.3866/PKU.DXHX202401009
9. [9]
  Xiaoning TANG , Shu XIA , Jie LEI , Xingfu YANG , Qiuyang LUO , Junnan LIU , An XUE . Fluorine-doped MnO₂ with oxygen vacancy for stabilizing Zn-ion batteries. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240149
10. [10]
  Yuejiao An , Wenxuan Liu , Yanfeng Zhang , Jianjun Zhang , Zhansheng Lu . Revealing Photoinduced Charge Transfer Mechanism of SnO₂/BiOBr S-Scheme Heterostructure for CO₂ Photoreduction. Acta Physico-Chimica Sinica, doi: 10.3866/PKU.WHXB202407021
11. [11]
  Caixia Lin , Zhaojiang Shi , Yi Yu , Jianfeng Yan , Keyin Ye , Yaofeng Yuan . Ideological and Political Design for the Electrochemical Synthesis of Benzoxathiazine Dioxide Experiment. University Chemistry, doi: 10.3866/PKU.DXHX202309005
12. [12]
  Yunhao Zhang , Yinuo Wang , Siran Wang , Dazhen Xu . Progress in Selective Construction of Functional Aromatics from Nitrogenous Cycloalkanes. University Chemistry, doi: 10.3866/PKU.DXHX202401083
13. [13]
  Peiran ZHAO , Yuqian LIU , Cheng HE , Chunying DUAN . A functionalized Eu³⁺ metal-organic framework for selective fluorescent detection of pyrene. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20230355
14. [14]
  Xilin Zhao , Xingyu Tu , Zongxuan Li , Rui Dong , Bo Jiang , Zhiwei Miao . Research Progress in Enantioselective Synthesis of Axial Chiral Compounds. University Chemistry, doi: 10.12461/PKU.DXHX202403106
15. [15]
  Jiakun BAI , Ting XU , Lu ZHANG , Jiang PENG , Yuqiang LI , Junhui JIA . A red-emitting fluorescent probe with a large Stokes shift for selective detection of hypochlorous acid. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240002
16. [16]
  Heng Zhang . Determination of All Rate Constants in the Enzyme Catalyzed Reactions Based on Michaelis-Menten Mechanism. University Chemistry, doi: 10.3866/PKU.DXHX202310047
17. [17]
  Junjie Zhang , Yue Wang , Qiuhan Wu , Ruquan Shen , Han Liu , Xinhua Duan . Preparation and Selective Separation of Lightweight Magnetic Molecularly Imprinted Polymers for Trace Tetracycline Detection in Milk. University Chemistry, doi: 10.3866/PKU.DXHX202311084
18. [18]
  Zhuo WANG , Junshan ZHANG , Shaoyan YANG , Lingyan ZHOU , Yedi LI , Yuanpei LAN . Preparation and photocatalytic performance of CeO₂-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240067
19. [19]
  Yingchun ZHANG , Yiwei SHI , Ruijie YANG , Xin WANG , Zhiguo SONG , Min WANG . Dual ligands manganese complexes based on benzene sulfonic acid and 2, 2′-bipyridine: Structure and catalytic properties and mechanism in Mannich reaction. Chinese Journal of Inorganic Chemistry, doi: 10.11862/CJIC.20240078
20. [20]
  Jinyi Sun , Lin Ma , Yanjie Xi , Jing Wang . Preparation and Electrocatalytic Nitrogen Reduction Performance Study of Vanadium Nitride@Nitrogen-Doped Carbon Composite Nanomaterials: A Recommended Comprehensive Chemistry Experiment. University Chemistry, doi: 10.3866/PKU.DXHX202310094

Get Citation

PDF

XML

Metrics

PDF Downloads(805)
Abstract views(1749)
HTML views(17)

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

SO2 Deactivation Mechanism of MnOx/MWCNTs Catalyst for Low-Temperature Selective Catalytic Reduction of NOx by Ammonia

Metrics

通讯作者: 陈斌, bchen63@163.com

SO₂ Deactivation Mechanism of MnO_x/MWCNTs Catalyst for Low-Temperature Selective Catalytic Reduction of NOx by Ammonia