화학공학소재연구정보센터
홈 로그인 로그아웃 연락처 사이트맵
Journal of Industrial and Engineering Chemistry, Vol.90, 132-144, October, 2020
DOI10.1016/j.jiec.2020.07.005  Export Citation
Effects of SiO2/Al2O3 ratio, reaction atmosphere and metal additive on de-NOx performance of HC-SCR over Cu-based ZSM-5
Kyungseok Lee1, 2, Byungchul Choi1, 3, †, Chunbeom Lee4, and Kwangchul Oh4
  • 1Automotive Research Center, Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju 61186, Republic of Korea
  • 2University Industry Liaison of Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju 61186, Republic of Korea
  • 3School of Mechanical Engineering, Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju 61186, Republic of Korea
  • 4Korea Automotive Technology Institute, 303, Pungse-myeon, Dongnam-gu, Cheonan-si, Chungnam 31214, Republic of Korea
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This study aims to investigate the catalytic performance of 2Cu/ZSM-5 with different SiO2/Al2O3 ratios (30, 75, and 90) for selective catalytic reduction (SCR) of NOx by C3H6. The coexistent CO and H2 in the C3H6-SCR process were also evaluated to further improve the de-NOx performance. The SiO2/Al2O3 ratios and coexistent CO and H2 significantly affected the de-NOx performance and its operating temperature window. The addition of 1 wt.% metal additives (Pt, Ce, Sn, and Mn) to 2Cu/ZSM-5 exhibited a distinct improvement in catalytic performance. Among the metal-additive catalysts, 2Cu1Sn/ZSM-5 demonstrated favorable NOx conversion in the H2- or CO-C3H6-SCR process owing to the enhancement of partial oxidation of C3H6 by H2. This resulted in improved low-temperature catalytic performance, without any accompanying side reactions that produce NH3, N2O, and HNCO.
Keywords:HC-SCR;De-NOx;Cu/ZSM-5;SiO2/Al2O3ratio;Additives
  1. Coula MA, Charisiou ND, Papageridis KN, Delimitis A, Papista E, et al., J. Environ. Chem. Eng., 4, 1629 (2016)
  2. Castoldi L, Righini L, Matarrese R, Lietti L, Forzatti P, J. Catal., 328, 270 (2015)
  3. Worton DR, Sturges WT, Reeves CE, Newland MJ, Penkett SA, Atlas E, et al., Atmos. Environ., 54, 592 (2012)
  4. Piumetti M, Bensaid S, Fino D, Russo N, Catal. Struct. React., 1, 155 (2015)
  5. Boningari T, Smirniotis PG, Curr. Opin. Chem. Eng., 13, 133 (2016)
  6. Zhang RD, Liu N, Lei ZG, Chen BH, Chem. Rev., 116(6), 3658 (2016)
  7. Chen C, Yao A, Yao C, Wang H, Liu M, Li Z, Chem. Eng. Sci., 211, 115320 (2020)
  8. Iwamoto M, Furukawa H, Mine Y, Uemura F, Mikuriya SH, Kagawa S, Chem. Commun., 16, 1272 (1986)
  9. Garin F, Appl. Catal. A: Gen., 222(1-2), 183 (2001)
  10. Damma D, Boningari T, Ettireddy PR, Reddy BM, Smirniotis PG, Ind. Eng. Chem. Res., 57(49), 16615 (2018)
  11. Choi B, Lee KS, Chem. Eng. J., 240, 476 (2014)
  12. Say Z, Tohumeken M, Ozensoy E, Catal. Today, 267, 167 (2016)
  13. Cha J, Lee J, Chon MS, Atmos. Environ., 196, 133 (2019)
  14. Lefort I, Herreros JM, Tsolakis A, Environ. Sci. Technol., 48, 2361 (2014)
  15. Xu JN, Lu GZ, Guo Y, Guo YL, Gong XQ, Appl. Catal. A: Gen., 535, 1 (2017)
  16. Vaclavik M, Koci P, Novak V, Thompsett D, Chem. Eng. J., 329, 128 (2017)
  17. Lambert CK, React. Chem. Eng., 4, 969 (2019)
  18. Girard J, Montreuil C, Kim J, Cavataio G, Lambert C, SAE Int. J. Fuels Lubric., 488 (2009).
  19. Zhan R. Li W, Eakle ST, Weber P, Mixing and Distribution to Enhance SCR Performance, SAE Technical Paper 2010-01-1185 (2010).
  20. Gao F, Washton NM, Wang YL, Kollar M, Szanyi J, Peden CHF, J. Catal., 331, 25 (2015)
  21. Beale AM, Gao F, Lezcano-Gonzalez I, Peden CHF, Szanyi J, Chem. Soc. Rev., 44, 7371 (2015)
  22. Jung Y, Pyo YD, Jang J, Kim GC, Cho CP, Yang CH, Chem. Eng. J., 369, 1059 (2019)
  23. Lin F, Wang QL, Zhang JC, Jin J, Lu SY, Yan JH, Ind. Eng. Chem. Res., 58(51), 22763 (2019)
  24. Shin Y, Jung Y, Cho CP, Pyo YD, Jang J, Kim G, Kim TM, Chem. Eng. J., 381, 122751 (2020)
  25. Satokawa S, Chem. Lett., 29(3), 294 (2000)
  26. Wang X, Cen HY, Sachtler WMH, Appl. Catal. B: Environ., 26, L227 (2000)
  27. Kim MH, Nam IS, Korean J. Chem. Eng., 18(5), 725 (2001)
  28. Lonyi F, Solt HE, Valyon J, Boix A, Gutierrez LB, J. Mol. Catal. A-Chem., 345(1-2), 75 (2011)
  29. Chaieb T, Delannoy L, Louis C, Thomas C, Appl. Catal. B: Environ., 142-143, 780 (2013)
  30. Moreno-Gonzalez M, Palomares AE, Chiesa M, Boronat M, Giamello E, Blasco T, ACS Catal., 7, 3501 (2017)
  31. Xu J, Qin Y, Wang H, Guo F, Xie J, N. J. Chem., 44, 817 (2020)
  32. Di-Penta D, SAE Technical Paper 2011-01-1300 (2011).
  33. Torre UDL, Pereda-Ayo B, Gonzalez-Velasco JR, Chem. Eng. J., 207-208, 10 (2012)
  34. Liu Y, Zheng Y, Harold MP, Luss D, Top. Catal., 56, 104 (2013)
  35. You R, Meng M, Zhang J, Zheng LR, Hu TD, Li XG, Catal. Today, 327, 347 (2019)
  36. Held W, Konig A, Richter T, Puppe L, Catalytic NOx Reduction in Net Oxidizing Exhaust Gas, SAE Technical Paper 900496 (1990).
  37. Iwamoto M, Yahiro H, Tanda K, Stud. Surf. Sci. Catal., 44, 219 (1989)
  38. Iwamoto M, Yahiro H, Yuu Y, Shundo S, Mizuno N, Shokubai, 32, 430 (1990)
  39. Iwamoto M, Yahiro H, Tanda K, Mizuno N, Mine Y, Kagawa S, J. Phys. Chem., 95, 3727 (1991)
  40. Garrigos-Pastor G, Parres-Esclapez S, Bueno-Lopez A, Illan-Gomez MJ, de Lecea CSM, Appl. Catal. A: Gen., 354(1-2), 63 (2009)
  41. Martin JC, Suarez S, Yates M, Avila P, Chem. Eng. J., 150(1), 8 (2009)
  42. Heo I, Kim MK, Sung S, Nam IS, Cho BK, Olson KL, Li W, Environ. Sci. Technol., 47, 3657 (2013)
  43. More PM, J. Environ. Manage., 188, 43 (2017)
  44. Hirabayashi H, et al., SAE Technical Paper 2011-01-1277.
  45. Hayashizaki K, et al., SAE Technical Paper 2014-01-1501.
  46. Hino CSR Report, Environmental Technologies in Hino Motors’ Products, Urea-Free NOx and PM Post-Processing System for Light- and Medium-Duty Diesel Vehicles.
  47. Hayashizaki K, et al., SAE Technical Paper 2018-01-0345.
  48. Gawade P, Alexander AMC, Silver R, Ozkan US, Energy Fuels, 26(12), 7084 (2012)
  49. Cant NW, Liu IOY, Catal. Today, 63(2-4), 133 (2000)
  50. Shimizu KI, Sugino K, Kato K, Yokota S, Okumura K, Satsuma A, J. Phys. Chem. C, 111, 6481 (2007)
  51. Lobree LJ, Hwang IC, Reimer JA, Bell AT, Catal. Lett., 63(3-4), 233 (1999)
  52. Gu H, Chun KM, Song S, Int. J. Hydrog. Energy, 40(30), 9602 (2015)
  53. Lee KS, Kosaka H, Sato S, Yokoi T, Choi BC, Kim DS, J. Ind. Eng. Chem., 72, 73 (2019)
  54. Chansai S, Burch R, Hardacre C, Norton D, Bao X, Lewis L, Appl. Catal. B: Environ., 160-161, 356 (2014)
  55. Yu Y, Li Y, Zhang X, Deng H, He H, Li Y, Environ. Sci. Technol., 49, 481 (2015)
  56. Li L, Chen J, Zhang S, Zhang F, Guan N, Wang T, Liu S, Environ. Sci. Technol., 39, 2841 (2005)
  57. Lee K, et la., SAE Technical Paper 2015-01-2012 (2010).
  58. Lee K, Kosaka H, Sato S, Yokoi T, Choi B, Chem. Eng. Sci., 203, 28 (2019)
  59. Auerbach SM, Carrado KA, Dutta PK, Handbook of Zeolite Science and Technology, CRC Press, p. 1 2003, doi:http://dx.doi.org/10.1201/9780203911167.
  60. Loewenstein W, Am. Mineral., 39, 92 (1954)
  61. Gao Y, Zheng B, Wu G, Ma F, Liu C, RSC Adv., 87, 83581 (2016)
  62. Ismail MN, Goodrich TL, Ji Z, Ziemer KS, Warzywoda J, AS, Microporous Mesoporous Mater., 118, 245 (2009)
  63. Chen C, Yan X, Yoza BA, Zhou T, Li Y, Zhan Y, Wang Q, Li QX, Sci. Total Environ., 612, 1424 (2018)
  64. Dou BJ, Lv G, Wang C, Hao QL, Hui KS, Chem. Eng. J., 270, 549 (2015)
  65. Lai S, Meng D, Zhan W, Guo Y, Guo Y, Zhang Z, Lu G, RSC Adv., 5, 90235 (2015)
  66. Itho Y, Nishiyama S, Tsuruya S, Masai M, J. Phys. Chem., 98(3), 960 (1994)
  67. Spoto G, Zecchina A, Bordiga S, Ricchiardi G, Martra G, Leofanti G, Petrini G, Appl. Catal. B: Environ., 3(2-3), 151 (1994)
  68. Sultana A, Nanba T, Haneda M, Sasaki M, Hamada H, Appl. Catal. B: Environ., 101(1-2), 61 (2010)
  69. Praliaud H, Mikhailenko S, Chajar Z, Primet M, Appl. Catal. B: Environ., 16(4), 359 (1998)
  70. Korhonen ST, Fickel DW, Lobo RF, Weckhuysen BM, Beale AM, Chem. Commun., 2, 800 (2011)
  71. Fan C, Chen Z, Pang L, Ming SJ, Zhang XF, Albert KB, Liu P, Chen HP, Li T, Appl. Catal. A: Gen., 550, 256 (2018)
  72. Peng C, Yan R, Peng H, Mi Y, Liang J, Lu W, Wang X, Song G, Wu P, Liu F, J. Hazard. Mater., 385, 121593 (2020)
  73. Iwasaki M, Yamazaki K, Banno K, Shinjoh H, J. Catal., 2(260), 205 (2008)
  74. Han S, Ye O, Cheng S, Kang T, Dai H, Catal. Sci. Technol., 7, 703 (2017)
  75. Pang L, Fan C, Shao LN, Song KP, Yi JX, Cai X, Wang J, Kang M, Li T, Chem. Eng. J., 253, 394 (2014)
  76. Tian J, Peng H, Xu X, Liu W, Ma Y, Wang X, Yang X, Catal. Sci. Technol., 5, 2270 (2015)
  77. Ramirez-Garza RE, Rodriguez-Iznaga I, Simakov A, Farias MH, Castillon-Barraza FF, Mater. Res. Bull., 97, 369 (2081)
  78. Hernandez-Teran ME, Fuentes GA, Fuel, 138, 91 (2014)
  79. Goula MA, Charisiou ND, Papageridis KN, Delimitis A, Papista E, Pachatouridou E, Iliopoulou EF, Marnellos G, Konsolakis M, Yentekakis IV, J. Environ. Chem. Eng., 4, 1629 (2016)
  80. Xu GY, Ma JZ, He GZ, Yu YB, He H, Appl. Catal. B: Environ., 207, 60 (2017)
  81. Yang TT, Bi HT, Cheng XX, Appl. Catal. B: Environ., 102(1-2), 163 (2011)
  82. Zhang Z, Chen M, Jiang Z, Shangguan W, J. Environ. Sci., 22, 1441 (2010)
  83. Vaccaro AR, Mul G, Perez-Ramirez J, Moulijn JA, Appl. Catal. B: Environ., 46(4), 687 (2003)
  84. Mrad R, Aissat A, Cousin R, Courcot D, Siffert S, Appl. Catal. A: Gen., 504, 542 (2015)
  85. Pereda-Ayo B, De La Torre U, Illan-Gomez MJ, Bueno-Lopez A, Gonzalez-Velasco JR, Appl. Catal. B: Environ., 147, 420 (2014)
  86. Sun M, Wang S, Li Y, Wang Q, Xu H, Chen Y, J. Taiwan Inst. Chem. Eng., 78, 401 (2007)
  87. Xiong S, Peng Y, Wang D, Huang N, Zhang Q, Yang S, Chen J, Li J, Chem. Eng. J., 387, 124090 (2020)