Effects of Alkali and Alkaline Earth Cocations on the Activity and Hydrothermal Stability of Cu/SSZ-13 NH3-SCR Catalysts

被引:269
作者
Gao, Feng [1 ]
Wang, Yilin [1 ]
Washton, Nancy M. [1 ]
Kollar, Marton [1 ]
Szanyi, Janos [1 ]
Peden, Charles H. F. [1 ]
机构
[1] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA
关键词
selective catalytic reduction; chabazite; SSZ-13; diesel engine; emission control; SSZ-13; ZEOLITE; CU-SSZ-13; CATALYST; REACTION-KINETICS; EXCHANGED SSZ-13; MOLECULAR-SIEVES; REDUCTION; NH3; NOX; AMMONIA; IONS;
D O I
10.1021/acscatal.5b01621
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Using a three-step aqueous solution ionexchange method, cocation modified Cu/SSZ-13 SCR catalysts were synthesized. These catalysts, in both fresh and hydrothermally aged forms, were characterized with several methods including temperature-programmed reduction by H-2 (H-2-TPR), temperature-programmed desorption of NH3 (NH3-TPD), and Al-27 solid-state nuclear magnetic resonance (NMR) and diffuse reflectance infrared Fourier transform (DRIFT) spectroscopies. Their catalytic performance was probed using steady-state standard NH3-SCR. Characterization results indicate that cocations weaken interactions between Cu ions and the CHA framework making them more readily reducible. By removing a portion of Bronsted acid sites, cocations also help to mitigate hydrolysis of the zeolite catalysts during hydrothermal aging as evidenced from Al-27 NMR Reaction tests show that certain cocations, especially Li+ and Na+, promote low-temperature SCR rates while others show much less pronounced effects. In terms of applications, our results indicate that introducing cocations can be a viable strategy to improve both low- and high-temperature performance of Cu/SSZ-13 SCR catalysts.
引用
收藏
页码:6780 / 6791
页数:12
相关论文
共 40 条
[1]   Location of Cu2+ in CHA zeolite investigated by X-ray diffraction using the Rietveld/maximum entropy method [J].
Andersen, Casper Welzel ;
Bremholm, Martin ;
Vennestrom, Peter Nicolai Ravnborg ;
Blichfeld, Anders Bank ;
Lundegaard, Lars Fahl ;
Iversen, Bo Brummerstedt .
IUCRJ, 2014, 1 :382-386
[2]  
Andersen P.J., 2008, PCT, Patent No. [WO 2008/132452, 2008132452, WO/2008/132452]
[3]   Identification of the active Cu site in standard selective catalytic reduction with ammonia on Cu-SSZ-13 [J].
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. .
JOURNAL OF CATALYSIS, 2014, 312 :87-97
[4]   Adsorption of H2O, NH3 and C6H6 on alkali metal cations in internal surface of mordenite and in external surface of smectite: a DFT study [J].
Benco, Lubomir ;
Tunega, Daniel .
PHYSICS AND CHEMISTRY OF MINERALS, 2009, 36 (05) :281-290
[5]  
Broach R.W., 2010, Zeolites in Industrial Separation and Catalysis, P27, DOI DOI 10.1002/9783527629565.CH2
[6]  
Bull I., 2009, Copper CHA Zeolite Catalysts, Patent No. 7601662
[7]   NATURE OF ACTIVE SPECIES IN COPPER-BASED CATALYSTS AND THEIR CHEMISTRY OF TRANSFORMATION OF NITROGEN-OXIDES [J].
CENTI, G ;
PERATHONER, S .
APPLIED CATALYSIS A-GENERAL, 1995, 132 (02) :179-259
[8]   Confirmation of Isolated Cu2+ Ions in SSZ-13 Zeolite as Active Sites in NH3-Selective Catalytic Reduction [J].
Deka, Upakul ;
Juhin, Amelie ;
Eilertsen, Einar A. ;
Emerich, Hermann ;
Green, Mark A. ;
Korhonen, Satu T. ;
Weckhuysen, Bert M. ;
Beale, Andrew M. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (07) :4809-4818
[9]   The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites [J].
Fickel, Dustin W. ;
D'Addio, Elizabeth ;
Lauterbach, Jochen A. ;
Lobo, Raul F. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2011, 102 (3-4) :441-448
[10]   Copper Coordination in Cu-SSZ-13 and Cu-SSZ-16 Investigated by Variable-Temperature XRD [J].
Fickel, Dustin W. ;
Fedeyko, Joseph M. ;
Lobo, Raul F. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (03) :1633-1640