Citation: SHI Lin, YU Tie, WANG Xin-Quan, WANG Jun, SHEN Mei-Qing. Properties and Roles of Adsorbed NH₃ and NO_x over Cu/SAPO-34 Zeolite Catalyst in NH₃-SCR Process[J]. Acta Physico-Chimica Sinica, ;2013, 29(07): 1550-1557. doi: 10.3866/PKU.WHXB201304283 shu

Properties and Roles of Adsorbed NH₃ and NO_x over Cu/SAPO-34 Zeolite Catalyst in NH₃-SCR Process

SHI Lin ¹ ,
YU Tie ¹ ,
WANG Xin-Quan ¹ ,
WANG Jun ¹ ,
SHEN Mei-Qing ^1,2,

1.
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

Received Date: 15 February 2013
Available Online: 28 April 2013
Fund Project: 国家高技术研究发展计划项目(863) (2011AA03A405)资助 (863) (2011AA03A405)

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 NO_x (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. NO_x 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.
- Ammonia selective catalytic reduction,
- NO_x (NO and NO₂),
- Cu/SAPO-34,
- Diffuse reflectance infrared Fourier transform spectrum,
- Adsorption species
1. [1]
  
  (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. [2]
  (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. [3]
  (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. [4]
  (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. [5]
  (5) Liu, C. C.; Teng, H. Appl. Catal. B: Environ. 2005, 58, 69.doi: 10.1016/j.apcatb.2004.12.002
6. [6]
  (6) Sjövall, H.; Blint, R. J.; Olsson, L. Appl. Catal. B: Environ.2009, 92, 138. doi: 10.1016/j.apcatb.2009.07.020
7. [7]
  (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. [8]
  (8) Centi, G.; Perathoner, S. Appl. Catal. A: Gen. 1995, 132, 179.doi: 10.1016/0926-860X(95)00154-9
9. [9]
  (9) Seyedeyn-Azad, F.; Zhang, D. K. Catal. Today 2001, 68, 161.doi: 10.1016/S0920-5861(01)00308-X
10. [10]
  (10) Kagawa, S.; Yokoo, S.; Iwamoto, M. J. Chem. Soc. Chem. Commun. 1978, 23, 1058.
11. [11]
  (11) Li, Y.; Hall,W. K. J. Phys. Chem. 1990, 94, 6145. doi: 10.1021/j100379a001
12. [12]
  (12) Dltri, J. L.; Sachtler,W. M. H. Catal. Lett. 1992, 15, 289.doi: 10.1007/BF00765273
13. [13]
  (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. [14]
  (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. [15]
  (15) Ishihara, T.; Kagawa, M.; Hadama, F.; Takita, Y. J. Catal. 1997,169, 93. doi: 10.1006/jcat.1997.1681
16. [16]
  (16) Pastore, H. O.; Coluccia, S.; Marchese, L. A. Rev. Mater. Res.2005, 35, 351. doi: 10.1146/annurev.matsci.35.103103.120732
17. [17]
  (17) Deka, U.; Lezcano- nzalez, 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. [18]
  (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. [19]
  (19) Wang, L.; Li,W.; Qi, G. S.;Weng, D. J. Catal. 2012, 289, 21.doi: 10.1016/j.jcat.2012.01.012
20. [20]
  (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. [21]
  (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. [22]
  (22) Onida, B.; Gabelica, Z.; Lourenco, J.; Garrone, E. J. Phys. Chem. 1996, 100, 11072. doi: 10.1021/jp9600874
23. [23]
  (23) Sun, Q.; Gao, Z. X.;Wen, B.; Sachtler,W. M. H. Catal. Lett.2002, 78, 1. doi: 10.1023/A:1014981206924
24. [24]
  (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. [25]
  (25) Centi, G.; Perathoner, S.; Biglino D.; Giamello, E. J. Catal.1995, 152, 75. doi: 10.1006/jcat.1995.1062
26. [26]
  (26) Valyon, J.; Onyestyak, G.; Rees, L. V. C. J. Phys. Chem. B1998, 102, 8994. doi: 10.1021/jp981872e
27. [27]
  (27) Qi, G. S.; Gatt, J. E.; Yang, R. T. J. Catal. 2004, 226, 120.doi: 10.1016/j.jcat.2004.05.023
28. [28]
  (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. [29]
  (29) Centi, G.; Perathoner, S. Catal. Today 1996, 29, 117.doi: 10.1016/0920-5861(95)00289-8
30. [30]
  (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. [31]
  (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. [32]
  (32) Poignant, F.; Freysz, J. L.; Daturi, M.; Saussey, J. Catal. Today2001, 70, 197. doi: 10.1016/S0920-5861(01)00418-7
33. [33]
  (33) Sjövall, H.; Fridell, E.; Blint, R. J.; Olsson, L. Top Catal. 2007,42, 113. doi: 10.1007/s11244-007-0162-6
34. [34]
  (34) Qi, G. S.; Yang, R. T. J. Phys. Chem. B 2004, 108, 15738.doi: 10.1021/jp048431h
35. [35]
  (35) Trovarelli, A. Catal. Rev.-Sci. Eng. 1996, 38, 439. doi: 10.1080/01614949608006464
36. [36]
  (36) Centi, G.; Perathoner, S. Catal. Today 1996, 29, 117.doi: 10.1016/0920-5861(95)00289-8
37. [37]
  (37) Konduru, M. V.; Chuang, S. S. C. J. Catal. 2000, 196, 271.doi: 10.1006/jcat.2000.3046
38. [38]
  (38) Sjövall, H.; Blint, R. J.; Olsson, L. J. Phys. Chem. C 2009, 113,1393. doi: 10.1021/jp802449s
39. [39]
  (39) Lin, T.; Li,W.; ng, 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. [40]
  (40) Korhonen, S. T.; Fickel, D.W.; Lobo, R. F.;Weckhuysenb, B.M.; Beale, A. M. Chem. Commun. 2010, 47, 800
41. [41]
  (41) Brandenberger, S.; Kröcher, O.; Tissler A.; Althoff, R. Catal. Res. 2008, 50, 492. doi: 10.1080/01614940802480122
1. [1]
  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, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
2. [2]
  Linhui Liu , Wuwan Xiong , Mingli Fu , Junliang Wu , Zhenguo Li , Daiqi Ye , Peirong Chen . Efficient NO_x abatement by passive adsorption over a Pd-SAPO-34 catalyst prepared by solid-state ion exchange. Chinese Chemical Letters, 2024, 35(4): 108870-. doi: 10.1016/j.cclet.2023.108870
3. [3]
  Haojie Duan , Hejingying Niu , Lina Gan , Xiaodi Duan , Shuo Shi , Li Li . Reinterpret the heterogeneous reaction of α-Fe₂O₃ and NO₂ with 2D-COS: The role of SDS, UV and SO₂. Chinese Chemical Letters, 2024, 35(6): 109038-. doi: 10.1016/j.cclet.2023.109038
4. [4]
  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, 2024, 39(5): 251-257. doi: 10.3866/PKU.DXHX202311084
5. [5]
  Shihui Shi , Haoyu Li , Shaojie Han , Yifan Yao , Siqi Liu . Regioselectively Synthesis of Halogenated Arenes via Self-Assembly and Synergistic Catalysis Strategy. University Chemistry, 2024, 39(5): 336-344. doi: 10.3866/PKU.DXHX202312002
6. [6]
  Tong Zhou , Xue Liu , Liang Zhao , Mingtao Qiao , Wanying Lei . Efficient Photocatalytic H₂O₂ Production and Cr(VI) Reduction over a Hierarchical Ti₃C₂/In₄SnS₈ Schottky Junction. Acta Physico-Chimica Sinica, 2024, 40(10): 2309020-. doi: 10.3866/PKU.WHXB202309020
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, 2024, 39(8): 324-330. doi: 10.3866/PKU.DXHX202401063
8. [8]
  Xinyu Yin , Haiyang Shi , Yu Wang , Xuefei Wang , Ping Wang , Huogen Yu . Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production. Acta Physico-Chimica Sinica, 2024, 40(10): 2312007-. doi: 10.3866/PKU.WHXB202312007
9. [9]
  Yi YANG , Shuang WANG , Wendan WANG , Limiao CHEN . Photocatalytic CO₂ reduction performance of Z-scheme Ag-Cu₂O/BiVO₄ photocatalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 895-906. doi: 10.11862/CJIC.20230434
10. [10]
  Xuejiao Wang , Suiying Dong , Kezhen Qi , Vadim Popkov , Xianglin Xiang . Photocatalytic CO₂ Reduction by Modified g-C₃N₄. Acta Physico-Chimica Sinica, 2024, 40(12): 2408005-. doi: 10.3866/PKU.WHXB202408005
11. [11]
  Heng Chen , Longhui Nie , Kai Xu , Yiqiong Yang , Caihong Fang . 两步焙烧法制备大比表面积和结晶性增强超薄g-C₃N₄纳米片及其高效光催化产H₂O₂. Acta Physico-Chimica Sinica, 2024, 40(11): 2406019-. doi: 10.3866/PKU.WHXB202406019
12. [12]
  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
13. [13]
  Ping ZHANG , Chenchen ZHAO , Xiaoyun CUI , Bing XIE , Yihan LIU , Haiyu LIN , Jiale ZHANG , Yu'nan CHEN . Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1965-1974. doi: 10.11862/CJIC.20240014
14. [14]
  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, 2024, 40(4): 713-724. doi: 10.11862/CJIC.20230355
15. [15]
  Xilin Zhao , Xingyu Tu , Zongxuan Li , Rui Dong , Bo Jiang , Zhiwei Miao . Research Progress in Enantioselective Synthesis of Axial Chiral Compounds. University Chemistry, 2024, 39(11): 158-173. doi: 10.12461/PKU.DXHX202403106
16. [16]
  Peng ZHOU , Xiao CAI , Qingxiang MA , Xu LIU . Effects of Cu doping on the structure and optical properties of Au₁₁(dppf)₄Cl₂ nanocluster. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1254-1260. doi: 10.11862/CJIC.20240047
17. [17]
  Min WANG , Dehua XIN , Yaning SHI , Wenyao ZHU , Yuanqun ZHANG , Wei ZHANG . Construction and full-spectrum catalytic performance of multilevel Ag/Bi/nitrogen vacancy g-C₃N₄/Ti₃C₂T_x Schottky junction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1123-1134. doi: 10.11862/CJIC.20230477
18. [18]
  Fei Xie , Chengcheng Yuan , Haiyan Tan , Alireza Z. Moshfegh , Bicheng Zhu , Jiaguo Yu . d带中心调控过渡金属单原子负载COF吸附O₂的理论计算研究. Acta Physico-Chimica Sinica, 2024, 40(11): 2407013-. doi: 10.3866/PKU.WHXB202407013
19. [19]
  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, 2024, 40(6): 1095-1104. doi: 10.11862/CJIC.20240002
20. [20]
  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, 2024, 40(8): 1501-1510. doi: 10.11862/CJIC.20240078

Get Citation

PDF

XML

Metrics

PDF Downloads(1020)
Abstract views(1146)
HTML views(28)

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

Properties and Roles of Adsorbed NH3 and NOx over Cu/SAPO-34 Zeolite Catalyst in NH3-SCR Process

Metrics

通讯作者: 陈斌, bchen63@163.com

Properties and Roles of Adsorbed NH₃ and NO_x over Cu/SAPO-34 Zeolite Catalyst in NH₃-SCR Process