Register
ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2013,Vol.29>> Issue(07)>> 1550-1557     doi: 10.3866/PKU.WHXB201304283         中文摘要
CATALYSIS AND SURFACE SCIENCE
Properties and Roles of Adsorbed NH3 and NOx over Cu/SAPO-34 Zeolite Catalyst in NH3-SCR Process
SHI Lin1, YU Tie1, WANG Xin-Quan1, WANG Jun1, SHEN Mei-Qing1,2
1 Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2 State Key Laboratory of Engines, Tianjin University, Tianjin 300072, P. R. China
Full text: PDF (941KB) Export: BibTeX | EndNote (RIS)

To investigate the adsorption properties and roles of different feed gases in the selective catalytic reduction by ammonia (NH3-SCR), the adsorption sites, strength, and amount as well as reaction rates of NH3 and NOx (a mixture of NO and NO2) on exchanged Cu/SAPO-34 (chabazite zeolite) catalyst were studied. Transient response, temperature programmed desorption (TPD), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments were performed to characterize the catalyst. Transient response experiments showed that NH3 was adsorbed by the catalyst. TPD and DRIFTS indicated that NH3 can be adsorbed at both Br?nsted and Lewis acid sites to form various NH3 adsorption species that show different SCR activities. The adsorption rate of NH3 by Cu2+ cations was the fastest and the adsorption bond strength of NH3-Cu2+ was the strongest between NH3 and the Cu/SAPO-34 catalyst. NOx can be oxidized and stored as nitrates and nitrites on the Cu catalyst. The intermediate species formed at Cu active sites during the NH3-SCR reaction are discussed, allowing SCR reaction mechanisms to be inferred.



Keywords: Ammonia selective catalytic reduction   NOx (NO and NO2)   Cu/SAPO-34   Diffuse reflectance infrared Fourier transform spectrum   Adsorption species  
Received: 2013-02-15 Accepted: 2013-04-27 Publication Date (Web): 2013-04-28
Corresponding Authors: SHEN Mei-Qing Email: mqshen@tju.edu.cn

Fund: The project was supported by the National High-Tech Research and Development Program of China (863) (2011AA03A405).

Cite this article: SHI Lin, YU Tie, WANG Xin-Quan, WANG Jun, SHEN Mei-Qing. Properties and Roles of Adsorbed NH3 and NOx over Cu/SAPO-34 Zeolite Catalyst in NH3-SCR Process[J]. Acta Phys. -Chim. Sin., 2013,29 (07): 1550-1557.    doi: 10.3866/PKU.WHXB201304283

(1) Busca, G.; Lietti, L.; Ramis, G.; Berti, F. Appl. Catal. B: Environ. 1998, 18, 1. doi: 10.1016/S0926-3373(98)00040-X
(2) Qi, G. S.; Yang, R. T.; Chang, R. Appl. Catal. B: Environ. 2004,51, 93. doi: 10.1016/j.apcatb.2004.01.023
(3) Si, Z. C.;Weng, D.;Wu, X. D.; Li, J.; Li, G. J. Catal. 2010, 271,43. doi: 10.1016/j.jcat.2010.01.025
(4) Lobree, L. J.; Hwang, I. C.; Reimer, J. A.; Bell, A. T. J. Catal.1999, 186, 242. doi: 10.1006/jcat.1999.2548
(5) Liu, C. C.; Teng, H. Appl. Catal. B: Environ. 2005, 58, 69.doi: 10.1016/j.apcatb.2004.12.002
(6) Sjövall, H.; Blint, R. J.; Olsson, L. Appl. Catal. B: Environ.2009, 92, 138. doi: 10.1016/j.apcatb.2009.07.020
(7) Praliaud, H.; Mikhailenko, S.; Chajar, Z.; Primet, M. Appl. Catal. B: Environ. 1998, 16, 359. doi: 10.1016/S0926-3373(97)00093-3
(8) Centi, G.; Perathoner, S. Appl. Catal. A: Gen. 1995, 132, 179.doi: 10.1016/0926-860X(95)00154-9
(9) Seyedeyn-Azad, F.; Zhang, D. K. Catal. Today 2001, 68, 161.doi: 10.1016/S0920-5861(01)00308-X
(10) Kagawa, S.; Yokoo, S.; Iwamoto, M. J. Chem. Soc. Chem. Commun. 1978, 23, 1058.
(11) Li, Y.; Hall,W. K. J. Phys. Chem. 1990, 94, 6145. doi: 10.1021/j100379a001
(12) Dltri, J. L.; Sachtler,W. M. H. Catal. Lett. 1992, 15, 289.doi: 10.1007/BF00765273
(13) Kwak, J. H.; Tonkyn, R. G.; Kim, D. H.; Szanyi, J.; Peden, C.H. F. J. Catal. 2010, 275, 187. doi: 10.1016/j.jcat.2010.07.031
(14) Fickel, D.W.; D'Addio, E.; Lauterbach, J. A.; Lobo, R. F. Appl. Catal. B: Environ. 2011, 102, 441. doi: 10.1016/j.apcatb.2010.12.022
(15) Ishihara, T.; Kagawa, M.; Hadama, F.; Takita, Y. J. Catal. 1997,169, 93. doi: 10.1006/jcat.1997.1681
(16) Pastore, H. O.; Coluccia, S.; Marchese, L. A. Rev. Mater. Res.2005, 35, 351. doi: 10.1146/annurev.matsci.35.103103.120732
(17) Deka, U.; Lezcano-Gonzalez, I.;Warrender, S. J.; Picone, A. L.;Wright, P. A.;Weckhuysen, B. M.; Beale, A. M. Microporous Mesoporous Mat. 2013, 166, 144. doi: 10.1016/j.micromeso.2012.04.056
(18) Xue, J. J.;Wang, X. Q.; Qi, G. S.;Wang, J.; Shen, M. Q.; Li,W.J. Catal. 2013, 297, 56. doi: 10.1016/j.jcat.2012.09.020
(19) Wang, L.; Li,W.; Qi, G. S.;Weng, D. J. Catal. 2012, 289, 21.doi: 10.1016/j.jcat.2012.01.012
(20) Wang, J.; Yu, T.;Wang, X. Q.; Qi, G. S.; Xue, J. J.; Shen, M. Q.;Li,W. Appl. Catal. B: Environ. 2012, 127, 137. doi: 10.1016/j.apcatb.2012.08.016
(21) Martins, G. V. A.; Berlier, G.; Bisio, C.; Coluccia, S.; Pastore,H. O.; Marchese, L. J. Phys. Chem. C 2008, 112, 7193.doi: 10.1021/jp710613q
(22) Onida, B.; Gabelica, Z.; Lourenco, J.; Garrone, E. J. Phys. Chem. 1996, 100, 11072. doi: 10.1021/jp9600874
(23) Sun, Q.; Gao, Z. X.;Wen, B.; Sachtler,W. M. H. Catal. Lett.2002, 78, 1. doi: 10.1023/A:1014981206924
(24) Hadjiivanov, K.; Klissurski, D.; Ramis G.; Busca, G. Appl. Catal. B: Environ. 1996, 7, 251. doi: 10.1016/0926-3373(95)00034-8
(25) Centi, G.; Perathoner, S.; Biglino D.; Giamello, E. J. Catal.1995, 152, 75. doi: 10.1006/jcat.1995.1062
(26) Valyon, J.; Onyestyak, G.; Rees, L. V. C. J. Phys. Chem. B1998, 102, 8994. doi: 10.1021/jp981872e
(27) Qi, G. S.; Gatt, J. E.; Yang, R. T. J. Catal. 2004, 226, 120.doi: 10.1016/j.jcat.2004.05.023
(28) Jentys, A.;Warecka, G.; Lercher, J. A. J. Mol. Catal. A: Chem.1989, 51, 309. doi: 10.1016/0304-5102(89)80010-0
(29) Centi, G.; Perathoner, S. Catal. Today 1996, 29, 117.doi: 10.1016/0920-5861(95)00289-8
(30) Hadjiivanov, K.; Klissurski, D.; Ramis, G.; Busca, G. Appl. Catal. B: Environ. 1996, 7, 251. doi: 10.1016/0926-3373(95)00034-8
(31) Adelman, B. J.; Beutel, T.; Lei, G. D.; Sachtler,W. M. H.J. Catal. 1996, 158, 327. doi: 10.1006/jcat.1996.0031
(32) Poignant, F.; Freysz, J. L.; Daturi, M.; Saussey, J. Catal. Today2001, 70, 197. doi: 10.1016/S0920-5861(01)00418-7
(33) Sjövall, H.; Fridell, E.; Blint, R. J.; Olsson, L. Top Catal. 2007,42, 113. doi: 10.1007/s11244-007-0162-6
(34) Qi, G. S.; Yang, R. T. J. Phys. Chem. B 2004, 108, 15738.doi: 10.1021/jp048431h
(35) Trovarelli, A. Catal. Rev.-Sci. Eng. 1996, 38, 439. doi: 10.1080/01614949608006464
(36) Centi, G.; Perathoner, S. Catal. Today 1996, 29, 117.doi: 10.1016/0920-5861(95)00289-8
(37) Konduru, M. V.; Chuang, S. S. C. J. Catal. 2000, 196, 271.doi: 10.1006/jcat.2000.3046
(38) Sjövall, H.; Blint, R. J.; Olsson, L. J. Phys. Chem. C 2009, 113,1393. doi: 10.1021/jp802449s
(39) Lin, T.; Li,W.; Gong, M. C.; Yu, Y.; Du, B.; Chen, Y. Q. Acta Phys. -Chim. Sin. 2007, 23, 1851. [林涛, 李伟, 龚茂初,喻瑶, 杜波, 陈耀强. 物理化学学报, 2007, 23, 1851.]doi: 10.1016/S1872-1508(07)60089-8
(40) Korhonen, S. T.; Fickel, D.W.; Lobo, R. F.;Weckhuysenb, B.M.; Beale, A. M. Chem. Commun. 2010, 47, 800
(41) Brandenberger, S.; Kröcher, O.; Tissler A.; Althoff, R. Catal. Res. 2008, 50, 492. doi: 10.1080/01614940802480122

Copyright © 2006-2016 Editorial office of Acta Physico-Chimica Sinica
Address: College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P.R.China
Service Tel: +8610-62751724 Fax: +8610-62756388 Email:whxb@pku.edu.cn
^ Top