Impact of mild hydrothermal aging on kinetics of NH 3, NO, SO 2 and CO oxidation reactions on Cu/SSZ-13 catalyst

被引:1
作者
Zheleznyak, Tetyana [1 ]
Koci, Petr [1 ]
Epling, William [2 ]
机构
[1] Univ Chem & Technol, Technicka 5, Prague 16628, Czech Republic
[2] Univ Virginia, 385 Mormick Rd, Charlottesville, VA 22903 USA
基金
美国国家科学基金会;
关键词
SCR; Catalyst; Aging; Kinetics; Exhaust gas aftertreatment; CU-CHA CATALYSTS; ACTIVE CU; LOW-TEMPERATURE; NH3-SCR; REDUCTION; SCR; SITES; IDENTIFICATION; CU-SSZ-13; AMMONIA;
D O I
10.1016/j.cej.2024.151194
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Cu/SSZ-13 is a catalyst commonly used for selective catalytic reduction (SCR) of nitrogen oxides (NO x ) in diesel engine exhaust. Standard configurations are based on SCR preceded by an oxidation catalyst, however, a close -coupled SCR configuration appears relevant for upcoming regulations addressing cold -start emissions. Two often discussed ion -exchanged Cu sites in Cu/SSZ-13 are denoted ZCuOH and Z 2 Cu, where Z represents an Al atom in the zeolite framework. Mild hydrothermal aging (HTA) causes Cu redistribution within the catalyst; ZCuOH sites transform into more stable Z 2 Cu species. In this work, the effect of mild HTA on NH 3 , NO, SO 2 , and CO oxidation is studied on a commercial Cu/SSZ-13 sample. Temperature -programmed reaction experiments, performed in a lab reactor, and previously published catalyst characterization data using H 2 -TPR, NH 3 -TPD, and DRIFTS were used to build and validate a mathematical model. It couples the kinetics of the oxidation reactions with ZCuOH and Z 2 Cu concentration evolution during mild HTA. The model uses two distinct rate coefficients for ZCuOH and Z 2 Cu sites, allowing prediction of the catalyst activity during aging. The results suggest that the rate coefficients for the studied reactions on Z 2 Cu are effectively nil, so the observed activity in NH 3 , NO, SO 2 , and CO oxidation can be attributed solely to ZCuOH sites.
引用
收藏
页数:9
相关论文
共 47 条
  • [1] Akter N, 2018, KOREAN J CHEM ENG, V35, P89
  • [2] Global kinetic model of NO oxidation on Pd/γ-Al2O3 catalyst including PdOx formation and reduction by CO and C3H6
    Arvajova, Adela Buzkova
    Boutikos, Panagiotis
    Pecinka, Rudolf
    Koci, Petr
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 260 (260)
  • [3] Identification of the active Cu site in standard selective catalytic reduction with ammonia on Cu-SSZ-13
    Bates, Shane A.
    Verma, Anuj A.
    Paolucci, Christopher
    Parekh, Atish A.
    Anggara, Trunojoyo
    Yezerets, Aleksey
    Schneider, William F.
    Miller, Jeffrey T.
    Delgass, W. Nicholas
    Ribeiro, Fabio H.
    [J]. JOURNAL OF CATALYSIS, 2014, 312 : 87 - 97
  • [4] Advances and challenges of ammonia delivery by urea-water sprays in SCR systems
    Bornhorst, M.
    Deutschmann, O.
    [J]. PROGRESS IN ENERGY AND COMBUSTION SCIENCE, 2021, 87 (87)
  • [5] Modelling of a combined NOx storage and NH3-SCR catalytic system for Diesel exhaust gas aftertreatment
    Chatterjee, Daniel
    Koci, Petr
    Schmeisser, Volker
    Marek, Milos
    Weibel, Michel
    Krutzsch, Bernd
    [J]. CATALYSIS TODAY, 2010, 151 (3-4) : 395 - 409
  • [6] How changes in Cu-SSZ-13 catalytic oxidation activity via mild hydrothermal aging influence sulfur poisoning extents
    Chen, Yu-Ren
    Wei, Lai
    Kumar, Ashok
    Wang, Di
    Epling, William S.
    [J]. CATALYSIS SCIENCE & TECHNOLOGY, 2022, 12 (22) : 6891 - 6902
  • [7] Kinetic Model for the Reduction of CuIISites by NO + NH3 and Reoxidation of NH3-Solvated CuISites by O2and NO in Cu-SSZ-13
    Daya, Rohil
    Trandal, Dylan
    Menon, Unmesh
    Deka, Dhruba J.
    Partridge, William P.
    Joshi, Saurabh Y.
    [J]. ACS CATALYSIS, 2022, 12 (11): : 6418 - 6433
  • [8] Kinetics and thermodynamics of ammonia solvation on Z2Cu, ZCuOH and ZCu sites in Cu-SSZ-13-Implications for hydrothermal aging
    Daya, Rohil
    Trandal, Dylan
    Dadi, Rama Krishna
    Li, Hui
    Joshi, Saurabh Y.
    Luo, Jinyong
    Kumar, Ashok
    Yezerets, Aleksey
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 297
  • [9] On kinetic modeling of change in active sites upon hydrothermal aging of Cu-SSZ-13
    Daya, Rohil
    Joshi, Saurabh Y.
    Luo, Jinyong
    Dadi, Rama Krishna
    Currier, Neal W.
    Yezerets, Aleksey
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 263
  • [10] Modeling and analysis of transport and reaction in washcoated monoliths: Cu-SSZ-13 SCR and dual-layer Cu-SSZ-13+Pt/Al2O3 ASC
    Dhillon, Pritpal S.
    Harold, Michael P.
    Wang, Di
    Kumar, Ashok
    Joshi, Saurabh Y.
    [J]. REACTION CHEMISTRY & ENGINEERING, 2019, 4 (06) : 1103 - 1115