NOx abatement and N2O formation over urea-SCR systems with zeolite supported Fe and Cu catalysts in a nonroad diesel engine

被引:61
|
作者
Shin, Youngjin [1 ]
Jung, Yongjin [1 ]
Cho, Chong Pyo [1 ]
Pyo, Young Dug [1 ]
Jang, Jinyoung [1 ]
Kim, Gangchul [1 ]
Kim, Tae Min [2 ]
机构
[1] Korea Inst Energy Res, Energy Efficiency Technol & Mat Sci Div, 152 Gajeong Ro, Daejeon 34129, South Korea
[2] E&D Co Ltd, R&D Ctr, 14 Gasan Digital 2 Ro, Seoul 08592, South Korea
关键词
Nitrogen oxides (NOx); Nitrous oxide (N2O); Selective catalytic reduction (SCR); Urea; Zeolite; Greenhouse gases (GHG); REDUCTION; EMISSIONS; AMMONIA; NH3-SCR; CHEMISTRY; MECHANISM;
D O I
10.1016/j.cej.2019.122751
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
NO and NO2 emissions over urea-based selective catalytic reduction (SCR) systems were investigated in a nonroad diesel engine. For catalysts of the SCR systems, two types of metal ion-exchanged zeolites were used; one is Fe, the other Cu. The Fe/zeolite was composed of Fe only, however, the Cu/zeolite consisted of Cu (80%) and Fe (20%). Nitrogen oxides (NOx) conversion efficiency of the Fe/ and Cu/zeolite catalysts remained greater than 80% in the temperature range of approximately 300 and 450 degrees C. The Cu/zeolite catalyst retained high efficiency above approximately 450 degrees C, however, the Fe/zeolite exhibited a drastic decrease resulting from the deterioration of NO conversion efficiency due to the ammonia storage capability of Fe/zeolite, which was inferior to that of Cu/zeolite. It was also found that NO was oxidized to NO2 in the diesel oxidation catalyst and diesel particulate filter, and NO2/NOx ratio at the SCR inlet consistently maintained thermodynamic equilibrium irrespective of the SCR catalyst. The ratio was higher than 50% between 200 and 410 degrees C. N2O emission that forms in SCR systems through side reactions during NOx reduction was also studied because N2O is a greenhouse gas with approximately 300 times greater global warming potential than carbon dioxide. The ratio of N2O at the SCR outlet to NOx at the SCR inlet for both catalysts was higher between 200 and 410 degrees C than at other temperatures, which implies that N2O formation is considerably involved in the NO2/NOx ratio. The Cu/zeolite catalyst in the urea-SCR system exhibited higher NO and NO2 conversion efficiencies while maintaining a lower amount of N2O formation compared to the Fe/zeolite catalyst.
引用
收藏
页数:11
相关论文
共 50 条
  • [41] Pathways for N2 and N2O Formation during the Reduction of NOx over Pt Ba/Al2O3 LNT Catalysts Investigated by Labeling Isotopic Experiments
    Lietti, L.
    Artioli, N.
    Righini, L.
    Castoldi, L.
    Forzatti, P.
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2012, 51 (22) : 7597 - 7605
  • [42] Experimental Investigation on N2O Formation during the Selective Catalytic Reduction of NOx with NH3 over Cu-SSZ-13
    Liu, Biao
    Yao, Dongwei
    Wu, Feng
    Wei, Lai
    Li, Xingwen
    Wang, Xinlei
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2019, 58 (45) : 20516 - 20527
  • [43] The effect of ammonia gas and UWS injection on the N2O formation in diesel engine after-treatment systems under steady and transient conditions
    Raza, Hassan
    Oh, Kwang-Chul
    Kim, Hongsuk
    FUEL, 2022, 330
  • [44] Direct methanol production from mixed methane/H2O/N2O feedstocks over Cu-Fe/Al2O3 catalysts
    Dasireddy, Venkata D. B. C.
    Likozar, Blaz
    FUEL, 2021, 301
  • [45] Catalytic decomposition of N2O over Co-M (M=La, Ce, Fe, Mn, Cu, Cr) composite oxide catalysts
    Xue Li
    He Hong
    ACTA PHYSICO-CHIMICA SINICA, 2007, 23 (05) : 664 - 670
  • [46] In situ IR comparative study on N2O formation pathways over different valence states manganese oxides catalysts during NH3–SCR of NO
    College of Materials Science and Engineering, Chongqing University, Chongqing
    400044, China
    不详
    400044, China
    不详
    不详
    Chem. Eng. J., 2020,
  • [47] NO/NO2/N2O-NH3 SCR reactions over a commercial Fe-zeolite catalyst for diesel exhaust aftertreatment: Intrinsic kinetics and monolith converter modelling
    Colombo, Massimo
    Nova, Isabella
    Tronconi, Enrico
    Schmeisser, Volker
    Bandl-Konrad, Brigitte
    Zimmermann, Lisa
    APPLIED CATALYSIS B-ENVIRONMENTAL, 2012, 111 : 106 - 118
  • [48] FORMATION OF METHYLFORMATE DURING HYDROGENATION OF CO2 OVER CU/ZNO/AL2O3 AND K-FE/L ZEOLITE CATALYSTS
    PARK, SE
    SHIM, EK
    LEE, KW
    KIM, PS
    ZEOLITES AND RELATED MICROPOROUS MATERIALS: STATE OF THE ART 1994, 1994, 84 : 1595 - 1602
  • [49] Formation of Surface Oxygen Species and the Conversion of Methane to Value-Added Products with N2O as Oxidant over Fe-Ferrierite Catalysts
    Zhao, Guangyu
    Adesina, Adesoji
    Kennedy, Eric
    Stockenhuber, Michael
    ACS CATALYSIS, 2020, 10 (02): : 1406 - 1416
  • [50] Formation of reactive oxygen by N2O decomposition over binuclear cationic sites of Fe-ferrierite zeolite: Periodic DFT plus U study
    Avdeev, Vasilii I.
    Bedilo, Alexander F.
    CHEMICAL PHYSICS LETTERS, 2018, 695 : 222 - 227