화학공학소재연구정보센터
홈 로그인 로그아웃 연락처 사이트맵
Journal of Industrial and Engineering Chemistry, Vol.102, 51-68, October, 2021
DOI10.1016/j.jiec.2021.06.030  Export Citation
HC-SCR system combining Ag/Al2O3 and Pd/Al2O3 catalysts with resistance to hydrothermal aging for simultaneous removal of NO, HC, and CO
Kyungseok Lee1, 2, and Byungchul Choi1, 3, †
  • 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
E-mail:
A combined Ag/Al2O3 and Pd/Al2O3 catalyst was investigated for the selective catalytic reduction (SCR) of NOx by H2-assisted C3H6 in the presence of excessive O2. The coexistent H2 significantly lowered the active temperature window of the de-NOx reaction because of the enhanced partial oxidation of C3H6 and NO oxidation to NO2. A low Ag loading of 1 wt% exhibited better de-NOx performance than that attained using 2 wt% Ag. Although Ag/Al2O3 exhibited a high resistance to hydrothermal aging, a high reaction temperature (>500 °C) was required to oxidize CO and C3H6 completely. In contrast to Ag/Al2O3, Pd/Al2O3 suppressed C3H6 and CO slip at relatively low temperatures, and a complete oxidation of C3H6 and CO was achieved at 195.275 °C and 240-275 °C, respectively, under varying SCR conditions and Pd contents (0.5-1.5 wt%); however, 30% de-NOx performance in a narrow temperature window of 210-240 °C was attained. The best configuration was found to be a sequential arrangement of 1Ag/Al2O3 followed by 1Pd/Al2O3, which enabled the reduction of NOx, C3H6, CO, and H2 over wide reaction temperatures, unlike the stand-alone configuration. In this configuration, the reacted NOx was reduced to N2 with negligible formation of by-products, even after hydrothermal aging.
Keywords:H2-assisted C3H6-SCR;Hydrothermal aging;Combined SCR catalyst;Ag/Al2O3;Pd/Al2O3
  1. Granger P, Parvulescu VI, Chem. Rev., 111(5), 3155 (2011)
  2. Schmidt JE, Oord R, Guo W, Poplawsky JD, Weckhuysen BM, Nat. Commun., 8, 1666 (2017)
  3. Wang LF, Yin CY, Yang RT, Appl. Catal. A: Gen., 514, 35 (2016)
  4. Fang S, Takagaki A, Watanabe M, Ishihara T, Catal. Sci. Technol., 10, 2513 (2020)
  5. Ayhan V, Ece YM, Appl. Energy, 260 (2020)
  6. Li C, Wang Y, Jia B, Roskilly AP, Appl. Therm. Eng., 150, 904 (2019)
  7. Castro N, Toledo M, Amador G, Appl. Therm. Eng., 156, 660 (2019)
  8. Shinabuth D, Nagasawa T, Sato S, Kosaka H, Int. J. Automot. Eng., 11, 159 (2020)
  9. Alghamdi N, Cano JR, Anjum DH, Im HG, Kalamaras C, Gascon J, Sarathy SM, SAE Technical Paper 2020-01-2173 (2020).
  10. Olabi AG, Maizak D, Wilberforce T, Sci. Total Environ., 748 (2020)
  11. Choi B, Lee KS, Chem. Eng. J., 240, 476 (2014)
  12. Martinez-Munuera JC, Gimenez-Manogil J, Castoldi L, Lietti L, Garcia-Garcia A, Appl. Surf. Sci., 529 (2020)
  13. Liu K, Yu Q, Liu J, Wang K, Han Z, Xuan Y, Qin Q, New J. Chem., 41, 13993 (2017)
  14. Oton LF, Oliveira AC, de Araujo JCS, Araujo RS, de Sousa FF, Saraiva GD, Lang R, Otubo L, Duarte GCD, Campos A, Adv. Powder Technol., 31(1), 464 (2020)
  15. Duan KJ, Wang ZH, Hardacre C, Liu ZM, Chansai S, Stere C, Catal. Today, 332, 69 (2019)
  16. Samojeden B, Crzybek T, Energy, 116, 1484 (2016)
  17. Li Q, Hou Y, Xiang N, Liu Y, Huang Z, Sci. Total Environ., 740 (2020)
  18. Lee K, Kosaka H, Sato S, Yokoi T, Choi B, Chem. Eng. Sci., 203, 28 (2019)
  19. Lee KS, Kosaka H, Sato S, Yokoi T, Choi BC, Kim DS, J. Ind. Eng. Chem., 72, 73 (2019)
  20. Jung Y, Shin YJ, Pyo YD, Cho CP, Jang J, Kim G, Chem. Eng. J., 236, 853 (2017)
  21. Shibata G, Eijima W, Koiwai R, Shimizu K, Nakasaka Y, Kobashi Y, Kubota Y, Ogura M, Kusaka J, Catal. Today, 332, 59 (2019)
  22. Resitoglu IA, Keskin A, Int. J. Hydrog. Energy, 42(36), 23389 (2017)
  23. Wang X, Wen W, Mi J, Li X, Wang R, Appl. Catal. B: Environ., 176-177, 454 (2015)
  24. Beale AM, Gao F, Lezcano-Gonzalez I, Peden CHF, Szanyi J, Chem. Soc. Rev., 44, 7371 (2015)
  25. Zhang RD, Liu N, Lei ZG, Chen BH, Chem. Rev., 116(6), 3658 (2016)
  26. Choi B, Lee K, Son G, Int. J. Automot. Technol., 21, 1597 (2020)
  27. Held W, Konig A, Richter T, Puppe L, Catalytic NOx Reduction in Net Oxidizing Exhaust Gas SAE Technical Paper 900496, p.13 (1990).
  28. Iwamoto M, Yahiro H, Yuu Y, Shundo S, Mizuno N, Shokubai, 32, 430 (1990)
  29. Iwamoto M, Yahiro H, Tanda K, Mizuno N, Mine Y, Kagawa S, J. Phys. Chem., 95, 3727 (1991)
  30. Burch R, Breen JP, Meunier FC, Appl. Catal. B: Environ., 39(4), 283 (2002)
  31. Ayodhya AS, Narayanappa KG, Environ. Sci. Pollut. Res., 25, 35034 (2018)
  32. Resitoglu IA, Keskin A, Ozarslan H, Bulut H, Int. J. Environ. Sci. Technol., 16, 6959 (2019)
  33. Cheng X, Bi XT, Particuology, 16, 1 (2014)
  34. Kim SS, Choi SH, Lee SM, Hong SC, J. Ind. Eng. Chem., 18(1), 272 (2012)
  35. Hamill C, Burch R, Goguet A, Rooney D, Driss H, Petrov L, Daous M, Appl. Catal. B: Environ., 147, 864 (2014)
  36. More PM, Dongare MK, Umbarkar SB, Granger P, Dujardin C, Catal. Today, 306, 23 (2018)
  37. Xu J, Qin Y, Wang H, Guo F, Xie J, New J. Chem., 44, 817 (2020)
  38. Lee KS, Choi BC, Lee CB, Oh KC, J. Ind. Eng. Chem., 90, 132 (2020)
  39. More PM, J. Environ. Manage., 188, 43 (2017)
  40. Zhang ZS, Crocker M, Chen BB, Wang XK, Bai ZF, Shi C, Catal. Today, 258, 386 (2015)
  41. Satokawa S, Chem. Lett., 29(3), 294 (2000)
  42. Satokawa S, Shibata J, Shimizu K, Atsushi S, Hattori T, Appl. Catal. B: Environ., 42(2), 179 (2003)
  43. Satokawa S, Shibata J, Shimizu KI, Satsuma A, Hattori T, Kojima T, Chem. Eng. Sci., 62(18-20), 5335 (2007)
  44. Shimizu KI, Satsuma A, J. Phys. Chem. C, 111, 2259 (2007)
  45. Yu Y, He H, Zhang X, Deng H, Catal. Sci. Technol., 4, 1239 (2014)
  46. Deng H, Yu Y, He H, J. Phys. Chem. C, 119, 3132 (2015)
  47. Chaieb T, Delannoy L, Costentin G, Louis C, Casale S, Chantry RL, Li ZY, Thomas C, Appl. Catal. B: Environ., 156-157, 192 (2014)
  48. Lee KS, Choi BC, Kim CH, Lee CB, Oh KC, J. Ind. Eng. Chem., 93, 461 (2021)
  49. Moulijn JA, van Diepen AE, Kapteijn F, Appl. Catal. A: Gen., 212(1-2), 3 (2001)
  50. Wang HL, Luo ST, Li XH, Liu W, Wu XD, Weng D, Liu S, Catal. Today, 332, 189 (2019)
  51. Houel V, James D, Millington P, Pollington S, Poulston S, Rajaram R, Torbati R, J. Catal., 230(1), 150 (2005)
  52. Breen JP, Burch R, Hardacre C, Hill CJ, Krutzsch B, Bandl-Konrad B, Jobson E, Cider L, Blakeman PG, Peace LJ, Twigg MV, Preis M, Gottschling M, Appl. Catal. B: Environ., 70(1-4), 36 (2007)
  53. Petitto C, Mutin PH, Delahay G, Top. Catal., 56, 34 (2013)
  54. Lucci F, Della Torre A, Montenegro G, Eggenschwiler PD, Chem. Eng. J., 264, 514 (2015)
  55. Zhou H, Su YX, Liao WY, Deng WY, Zhong FC, Appl. Catal. A: Gen., 505, 402 (2015)
  56. Wang F, Ma J, Xin S, Wang Q, Xu J, Zhang C, He H, Zeng XC, Nat. Commun., 11, 529 (2020)
  57. Korhonen ST, Beale AM, Newton MA, Weckhuysen BM, J. Phys. Chem. C, 115, 885 (2011)
  58. Strom L, Carlsson PA, Skoglundh M, Harelind H, Appl. Catal. B: Environ., 181, 403 (2016)
  59. Duan K, Liu Z, Li J, Yuan L, Hu H, Woo SI, Catal. Commun., 57, 19 (2014)
  60. Zhang X, Qu Z, Yu F, Wang Y, J. Catal., 297, 364 (2013)
  61. Morgan K, Goguet A, Hardacre C, ACS Catal., 5, 3430 (2015)
  62. Huang Z, Ban T, Zhang Y, Wang L, Guo S, Chang CR, Jing G, Appl. Catal. B: Environ., 283 (2021)
  63. Wagstaffe M, Hussain H, Acres MJ, Jones R, Syres KL, Thomas AG, J. Phys. Chem. C, 121, 21383 (2017)
  64. Barrera A, Tzompantzi F, Campa-Molina J, Casillas JE, Perez-Hernandez R, Ulloa-Godinez S, Velasquez C, Arenas-Alatorre J, RSC Adv., 8, 3108 (2018)
  65. Leelavathi A, Udaya T, Rao B, Pradeep T, Nanoscale Res. Lett., 6, 123 (2011)
  66. Jing X, Wang H, Chen H, Huang J, Li Q, Sun D, RSC Adv., 4, 27597 (2014)
  67. Jin GJ, Lu GZ, Guo YL, Guo Y, Wang JS, Liu XH, Catal. Lett., 87(3-4), 249 (2003)
  68. Beketov G, Heinrichs B, Pirard JP, Chenakin S, Kruse N, Appl. Surf. Sci., 287, 293 (2013)
  69. Chen XY, Cheng YS, Seo CY, Schwank JW, McCabe RW, Appl. Catal. B: Environ., 163, 499 (2015)
  70. Busca G, Catal. Today, 226, 2 (2014)
  71. Wang Y, Qu Z, Xu J, Huang B, Appl. Catal. A: Gen., 602 (2020)
  72. Prins R, J. Catal., 392, 336 (2020)
  73. Zeng J, Zheng YQ, Rycenga M, Tao J, Li ZY, Zhang QA, Zhu YM, Xia YN, J. Am. Chem. Soc., 132(25), 8552 (2010)
  74. Zhang J, Li Y, Zhang Y, Chen M, Wang L, Zhang C, He H, Sci. Rep., 5, 12950 (2015)
  75. Li L, Zhang N, Huang X, Liu Y, Li Y, Zhang G, Song L, He H, ACS Catal., 8, 3222 (2018)
  76. Albiter E, Valenzuela MA, Alfaro S, Valverde-Aguilar G, Martinez-Pallares FM, J. Saudi Chem. Soc., 19, 563 (2015)
  77. Xu GY, Ma JZ, Wang L, Xie W, Liu JJ, Yu YB, He H, Appl. Catal. B: Environ., 244, 909 (2019)
  78. Kim MK, Kim PS, Baik JH, Nam IS, Cho BK, Oh SH, Appl. Catal. B: Environ., 105(1-2), 1 (2011)
  79. Cant NW, Liu IOY, Catal. Toady, 63, 133 (2000)
  80. Li L, Zhang F, Guan N, Schreier E, Richter M, Catal. Commun., 9, 1827 (2008)
  81. Duan K, Liu Z, Yuan L, Chin. Sci. Bull., 59, 3973 (2014)
  82. Duan K, Chen B, Zhu T, Liu Z, Appl. Catal. B: Environ., 176-177, 6189 (2015)
  83. Hu Z, Yang RT, Ind. Eng. Chem. Res., 58(24), 10140 (2019)
  84. Hernandez-Teran ME, Fuentes GA, Fuel, 138, 91 (2014)
  85. Kim MY, Choi JS, Crocker M, Catal. Today, 231, 90 (2014)
  86. Gunnarsson F, Pihl JA, Toops TJ, Skoglundh M, Harelind H, Appl. Catal. B: Environ., 202, 42 (2017)
  87. Tamm S, Catal. Lett., 143(9), 957 (2013)
  88. Yeom YH, Wen B, Sachtler WMH, Weitz E, J. Phys. Chem. B, 108(17), 5386 (2004)
  89. Strom L, Carlsson PA, Skoglundh M, Harelind H, Catalysts, 8, 38 (2018)
  90. Xu G, Ma J, Wang L, Lv Z, Wang S, Yu Y, He H, ACS Catal., 9, 10489 (2019)
  91. Barreau M, Tarot ML, Duprez D, Courtois X, Can F, Appl. Catal. B: Environ., 220, 19 (2018)