WANG Chen, CHEN Zexiang, WANG Jianqiang, SHEN Meiqing, WANG Jun. Comparison study of Na poisoning effect on copper-based chabazite micropore catalysts for NH3-SCR reaction[J]. CIESC Journal, 2020, 71(12): 5551-5560 DOI: 10.11949/0438-1157.20200408.
WANG Chen, CHEN Zexiang, WANG Jianqiang, SHEN Meiqing, WANG Jun. Comparison study of Na poisoning effect on copper-based chabazite micropore catalysts for NH3-SCR reaction[J]. CIESC Journal, 2020, 71(12): 5551-5560 DOI: 10.11949/0438-1157.20200408.DOI:
Comparison study of Na poisoning effect on copper-based chabazite micropore catalysts for NH3-SCR reaction
Using wet impregnation method to mimic alkali metal poison of ammonia-selective catalytic reduction (NH
3
-SCR) catalysts
Cu-based micropore zeolites Cu/SSZ-13 and Cu/SAPO-34 with different Na contents(mass fraction) were prepared
and the Na poisoning mechanism on them was studied. The results show that the externally introduced Na ions can severely affect the NH
3
-SCR catalytic activity of the two catalysts
resulting in the collapse of the crystal structure of the catalyst
the decrease of acidity and the reduction of active species. In detail
when Na content was less than 1.82%
Cu/SAPO-34 has higher resistance of Na ions than Cu/SZZ-13; while when Na
>
3.48%
Cu/SAPO-34 catalysts almost deactivated thoroughly. By structural characterization (BET
XRD and SEM) and acidity characterization (DRIFTS
NH
3
-TPD and H
2
-TPR)
it was found that with Na poisoning deeper and deeper
Cu/SSZ-13 took a gradual style of the structural destruction
but Cu/SAPO-34 adopted a sudden way. Studies on the mechanism of Na poisoning show that the decrease of acid sites is the main reason for the decrease of SCR activity of Cu/SSZ-13
and th
e structural collapse is the main reason for the decrease of SCR activity of Cu/SAPO-34.
关键词
Keywords
references
杨光. 世界上第一辆汽油车奔弛1号[J]. 时代汽车, 2013, (12): 92-93.
Yang G. The first car in the world: Benz patent motor[J]. Auto Time, 2013, (12): 92-93.
Li Y Y. Research on total amount of vehicular emission in Beijing-Tianjin-Hebei (BTH) region and its abatement control strategy[D]. Tianjin: Tianjin University of Technology, 2015.
王小霞. 道路机动车尾气污染物排放量的预测与控制措施研究[D]. 西安: 长安大学, 2012.
Wang X X. Study on prediction and control measures of motor vehicle pollutant emission[D].Xian: Changan University, 2012.
李玉辉.机动车污染及防治对策[J ] . 环境科学与技术, 2000, 2 : 37-38.
Li Y H. Motor vehicle pollution and its prevention and control countermeasures[J ] . Environmental Science and Technology, 2000, 2 : 37-38.
Ministry of Ecology and Environment of the Peoples Republic of China. China Mobile Source Environmental Management Annual Report(2019)[R]. Beijing: Ministry of Ecology and Environment of the Peoples Republic of China, 2019.
Busca G, Lietti L, Ramis G, et al. Chemical and mechanistic aspects of the selective catalytic reduction of NO x by ammonia over oxide catalysts: a review [J ] . Applied Catalysis B: Environmental, 1998, 18 (1): 1-36.
Su L, Zhou L B, Jiang D M, et al. Recent development of aftertreatment of diesel emissions[J]. Internal Combustion Engines, 2003, (1): 1-8.
Forzatti P, Lietti L, Nova I, et al. Diesel NO x aftertreatment catalytic technologies: analogies in LNT and SCR catalytic chemistry[J ] . Catalysis Today, 2010, 151 (3/4): 202-211.
Girard J, Cavataio G, Snow R, et al. Combined Fe-Cu SCR systems with optimized ammonia to NO x ratio for diesel NO x control[J ] . SAE International Journal of Fuels and Lubricants, 2009, 1 (1): 603-610.
Arous W, Tounsi H, Djemel S, et al. Selective catalytic reduction of nitric oxide with ammonia on copper (Ⅱ) ion-exchanged offretite[J ] . Catalysis Communications, 2005, 6 (4): 281-285.
Sjvall H, Olsson L, Fridell E, et al. Selective catalytic reduction of NO x with NH3 over Cu-ZSM-5: the effect of changing the gas composition[J ] . Applied Catalysis B: Environmental, 2006, 64 (3/4): 180-188.
Delahay G, Kieger S, Tanchoux N, et al. Kinetics of the selective catalytic reduction of NO by NH3 on a Cu-faujasite catalyst[J ] . Applied Catalysis B: Environmental, 2004, 52 (4): 251-257.
Baik J H, Yim S D, Nam I, et al. Modeling of monolith reactor washcoated with CuZSM5 catalyst for removing NO from diesel engine by urea[J ] . Industrial & Engineering Chemistry Research, 2006, 45 (15): 5258-5267.
Han B, Lei Z G, Liu Q, et al. Influence of alkali metal compound on low-temperature NH3-SCR of NO over V2O5/AC catalyst[J ] .CIESC Journal, 2013, 64 (8): 2867-2874.
Williams A, Mccormick R, Lance M, et al. Effect of accelerated aging rate on the capture of fuel-borne metal impurities by emissions control devices [J ] . SAE International Journal of Fuels and Lubricants, 2014, 7 (2): 471-479.
Wang C, Wang C, Wang J, et al. Effects of Na+ on Cu/SAPO-34 for ammonia selective catalytic reduction [J ] . Journal of Environmental Sciences, 2018, 70 : 20-28.
Chen Z, Wang J, Wang J, et al. Disparate essences of residual, ion-exchanged, and impregnated Na ions on topology structure for Cu/SSZ-13 NH3 selective catalytic reduction catalysts [J ] . Industrial & Engineering Chemistry Research, 2019, 58 (45): 20610-20619.
Wang J, Zhao H, Haller G, et al. Recent advances in the selective catalytic reduction of NO x with NH3 on Cu-Chabazite catalysts [J ] . Applied Catalysis B: Environmental, 2017, 202 : 346-354.
Wang D, Jangjou Y, Liu Y, et al. A comparison of hydrothermal aging effects on NH3-SCR of NO x over Cu-SSZ-13 and Cu-SAPO-34 catalysts [J ] . Applied Catalysis B: Environmental, 2015, 165 : 438-445.
Su W, Li Z, Peng Y, et al. Correlation of the changes in the framework and active Cu sites for typical Cu/CHA zeolites (SSZ-13 and SAPO-34) during hydrothermal aging [J ] . Physical Chemistry Chemical Physics, 2015, 17 (43): 29142-29149.
Zones S. Zeolite SSZ-13 and its method of preparation: US 4544538A[P]. 1985-10-1.
Niu C, Shi X Y, Liu F D, et al. High hydrothermal stability of Cu-SAPO-34 catalysts for the NH3-SCR of NO x [J ] . Chemical Engineering Journal, 2016, 294 : 254-263.
Kim Y J, Lee J K, Min K M, et al. Hydrothermal stability of CuSSZ13 for reducing NO x by NH3[J ] . Journal of Catalysis, 2014, 311 : 447-457.
Zhang J M, Liu X Y, Li M, et al. Fast synthesis of submicron all-silica CHA zeolite particles using a seeding method[J ] . RSC Advances, 2015, 5 : 27087-27090.
Schmieg S, Oh S, Kim C, et al. Thermal durability of Cu-CHA NH3-SCR catalysts for diesel NO x reduction[J ] . Catalysis Today, 2012, 184 (1): 252-261.
Gedeon A. Zeolites and Related Materials: Trends, Targets and Challenges[M]. Massiani P, Babonneau F. 4th ed. UK: Elsevier, 2008: 265.
Kumar M, Luo H, Román-Leshkov Y, et al. SSZ-13 crystallization by particle attachment and deterministic pathways to crystal size control[J ] . Journal of the American Chemical Society, 2015, 137 (40): 13007-13017.
Ma L, Cheng Y S, Cavataio G, et al. Characterization of commercial Cu-SSZ-13 and Cu-SAPO-34 catalysts with hydrothermal treatment for NH3-SCR of NO x in diesel exhaust[J ] . Chemical Engineering Journal, 2013, 225 : 323-330.
Luo J Y, Kamasamudram K, Currier N, et al. NH3-TPD methodology for quantifying hydrothermal aging of Cu/SSZ-13 SCR catalysts[J ] . Chemical Engineering Science, 2018, 190 : 60-67.
Yu T, Wang J, Shen M Q, et al. NH3-SCR over Cu/SAPO-34 catalysts with various acid contents and low Cu loading[J ] . Catalysis Science & Technology, 2013, 3 : 3234-3241.
Ma L, Cheng Y, Cavataio G, et al. In situ DRIFTS and temperature-programmed technology study on NH3-SCR of NO x over Cu-SSZ-13 and Cu-SAPO-34 catalysts [J ] . Applied Catalysis B: Environmental, 2014, 156/157 : 428-437.
Luo J, Gao F, Kamasamudram K, et al. New insights into Cu/SSZ-13 SCR catalyst acidity(Ⅰ): Nature of acidi c sites probed by NH3 titration [J ] . Journal of Catalysis, 2017, 348 : 291-299.
Cui Y, Wang Y, Walter E D, et al. Influences of Na+ co-cation on the structure and performance of Cu/SSZ-13 selective catalytic reduction catalysts [J ] . Catalysis Today, 2020, 339 : 233-240.
Gao F, Walter E D, Karp E M, et al. Structure-activity relationships in NH3-SCR over Cu-SSZ-13 as probed by reaction kinetics and EPR studies [J ] . Journal of Catalysis, 2013, 300 : 20-29.
Deka U, Juhin A, Eilertsen E A, et al. Confirmation of isolated Cu2+ ions in SSZ-13 zeolite as active sites in NH3-selective catalytic reduction [J ] . The Journal of Physical Chemistry C, 2012, 116 (7): 4809-4918.
Wang C, Wang J, Wang J, et al. The role of impregnated sodium ions in Cu/SSZ-13 NH3-SCR catalysts [J ] . Catalysts, 2018, 8 (12): 593.
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