The role of pore size on the thermal stability of zeolite supported Cu SCR catalysts

被引:120
作者
Blakeman, Philip G. [1 ]
Burkholder, Eric M. [1 ]
Chen, Hai-Ying [1 ]
Collier, Jillian E. [2 ]
Fedeyko, Joseph M. [1 ]
Jobson, Hoi [2 ]
Rajaram, Raj R. [2 ]
机构
[1] Johnson Matthey Emiss Control Technol, Wayne, PA 19087 USA
[2] Johnson Matthey Technol Ctr, Reading RG4 9NH, Berks, England
关键词
Cu/zeolite SCR catalysts; Hydrothermal stability; Zeolite pore size effect; In situ XRD; Cu/Al2O3; interaction; NOX REDUCTION; HYDROTHERMAL STABILITY; CU/ZSM-5; DEALUMINATION; DEACTIVATION; STATE; UREA; CHEMISTRY; AMMONIA; NH3;
D O I
10.1016/j.cattod.2013.10.047
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
comparison study on the hydrothermal stability of Cu SCR catalysts supported on an 8-ring small pore chabazite and a 12-ring large pore beta zeolite was performed to understand why small pore zeolite supported Cu catalysts are in general hydrothermally more stable than medium pore or large pore zeolite supported Cu catalysts and how different pore sizes affect the hydrothermal stability of the catalysts. In situ XRD hydrothermal experiments show that, even though the parent chabazite and beta zeolites have comparable hydrothermal stability and both can maintain their zeolite framework structure after a 900 degrees C hydrothermal exposure, the presence of Cu in the Cu/beta catalyst accelerates the collapse of the BEA framework structure at temperatures above 800 degrees C whereas Cu in the Cu/chabazite catalyst has little effect on the CHA framework structure. The loss of beta zeolite framework structure is due to a detrimental Cu/Al2O3 interaction. It is proposed that the constricting dimensions of the small openings in a small pore zeolite can hinder the destructive Cu/Al2O3 interaction as well as the zeolite dealumination process, hence significantly improving the hydrothermal stability of the small pore zeolite supported Cu catalyst. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:56 / 63
页数:8
相关论文
共 32 条
[1]  
Andersen P.J., 2008, PCT, Patent No. [WO 2008/132452, 2008132452, WO/2008/132452]
[2]   Control of NOx emissions from diesel engine by selective catalytic reduction (SCR) with urea [J].
Baik, JH ;
Yim, SD ;
Nam, IS ;
Mok, YS ;
Lee, JH ;
Cho, BK ;
Oh, SH .
TOPICS IN CATALYSIS, 2004, 30-1 (1-4) :37-41
[3]   Redox chemistry of Cu/ZSM-5 [J].
Beutel, T ;
Sarkany, J ;
Lei, GD ;
Yan, JY ;
Sachtler, WMH .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (02) :845-851
[4]   The State of the Art in Selective Catalytic Reduction of NOx by Ammonia Using Metal-Exchanged Zeolite Catalysts [J].
Brandenberger, Sandro ;
Kroecher, Oliver ;
Tissler, Arno ;
Althoff, Roderik .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2008, 50 (04) :492-531
[5]  
Bull I., 2009, [No title captured], Patent No. [US 7,601,6622009, 76016622009]
[6]   Catalytic abatement of NOx:: Chemical and mechanistic aspects [J].
Busca, G ;
Larrubia, MA ;
Arrighi, L ;
Ramis, G .
CATALYSIS TODAY, 2005, 107-08 :139-148
[7]  
Castagnola M., 2011, 2011011329 SAE
[8]  
Cavataio G., 2007, SAE TECHNICAL PAPER
[9]   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
[10]   Zeolites upon heating: Factors governing their thermal stability and structural changes [J].
Cruciani, Giuseppe .
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS, 2006, 67 (9-10) :1973-1994