Enhancement of low-temperature activity over Cu-exchanged zeolite beta from organotemplate-free synthesis for the selective catalytic reduction of NO with NH3 in exhaust gas streams

被引:42
作者
Xu, Li [1 ]
Shi, Chuan [1 ]
Zhang, Zhaoshun [1 ]
Gies, Hermann [2 ]
Xiao, Feng-Shou [3 ]
De Vos, Dirk [4 ]
Yokoi, Toshiyuki [5 ]
Bao, Xinhe [6 ]
Feyen, Mathias [7 ]
Maurer, Stefan [7 ]
Yilmaz, Bilge [8 ]
Mueller, Ulrich [7 ]
Zhang, Weiping [1 ]
机构
[1] Dalian Univ Technol, State Key Lab Fine Chem, Sch Chem, Dalian 116024, Peoples R China
[2] Ruhr Univ Bochum, Inst Geol Mineral & Geophys, Bochum, Germany
[3] Zhejiang Univ, Dept Chem, Hangzhou 310028, Zhejiang, Peoples R China
[4] Katholieke Univ Leuven, Ctr Surface Chem & Catalysis, Leuven, Belgium
[5] Tokyo Inst Technol, Chem Resources Lab, Yokohama, Kanagawa 227, Japan
[6] Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[7] BASF SE, D-67056 Ludwigshafen, Germany
[8] BASF Corp, Chem Res & Engn, Iselin, NJ 08830 USA
基金
中国国家自然科学基金;
关键词
Organotemplate-free Beta zeolite; Cu-Beta catalyst; NH3-SCR; H-2-TPR; CO-FTIR; DIESEL-ENGINE; AMMONIA; SITES; SCR; CU/SAPO-34; CU-SSZ-13; CU-ZSM-5; ROUTE; IONS; FTIR;
D O I
10.1016/j.micromeso.2014.04.034
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A series of Cu-exchanged Al-rich Beta zeolites from organotemplate-free synthesis was prepared and investigated for selective catalytic reduction (SCR) of NOx with NH3 in exhaust gas streams. In comparison to conventional Cu-Beta zeolite with Si/Al ratio of 19, Cu-Beta zeolite with Si/Al ratio of 4 is a superior low-temperature NH3-SCR catalyst. Very high NO conversion (>95%) can be achieved at temperatures as low as 150 to similar to 400 degrees C. XRD, UV-Vis-NIR and NH3-TPD measurements show that more isolated Cu2+ ions are present at the exchange sites of Al-rich Beta zeolite. The combination of CO-FTIR and H-2-TPR analysis demonstrates that Cu2+ ions could be reduced more readily on the Al-rich Beta than on the conventional Beta probably due to the proximity of the isolated Cu2+ ions. These can be correlated to the enhancement of NO conversion at lower temperatures over Cu-exchanged Al-rich Beta zeolite. (C) 2014 Elsevier Inc. All rights reserved.
引用
收藏
页码:304 / 310
页数:7
相关论文
共 30 条
[1]   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
[2]   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
[3]   Determining the nature of the active sites of Cu-beta zeolites for the selective catalytic reduction (SGR) of NOx by using a coupled reaction XAES/XPS study [J].
Corma, A ;
Palomares, A ;
Marquez, F .
JOURNAL OF CATALYSIS, 1997, 170 (01) :132-139
[4]   Microwave-assisted synthesis and characterization of Cu-containing AlPO4-5 and SAPO-5 [J].
Dang, Thi Thuy Hanh ;
Zubowa, Heide-Lore ;
Bentrup, Ursula ;
Richter, Manfred ;
Martin, Andreas .
MICROPOROUS AND MESOPOROUS MATERIALS, 2009, 123 (1-3) :209-220
[5]   Catalytic applications of OSDA-free Beta zeolite [J].
De Baerdemaeker, Trees ;
Yilmaz, Bilge ;
Mueller, Ulrich ;
Feyen, Mathias ;
Xiao, Feng-Shou ;
Zhang, Weiping ;
Tatsumi, Takashi ;
Gies, Hermann ;
Bao, Xinhe ;
De Vos, Dirk .
JOURNAL OF CATALYSIS, 2013, 308 :73-81
[6]   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
[7]   Catalytic NOx Abatement Systems for Mobile Sources: From Three-Way to Lean Burn after-Treatment Technologies [J].
Granger, Pascal ;
Parvulescu, Vasile I. .
CHEMICAL REVIEWS, 2011, 111 (05) :3155-3207
[8]   Stabilization of Cu+ ions in BEA zeolite: Study by FTIR spectroscopy of adsorbed CO and TPR [J].
Kefirov, Radoslav ;
Penkova, Anna ;
Hadjiivanov, Konstantin ;
Dzwigaj, Stanislaw ;
Che, Michel .
MICROPOROUS AND MESOPOROUS MATERIALS, 2008, 116 (1-3) :180-187
[9]   Selective catalytic reduction of nitric oxide by ammonia over Cu-FAU catalysts in oxygen-rich atmosphere [J].
Kieger, S ;
Delahay, G ;
Coq, B ;
Neveu, B .
JOURNAL OF CATALYSIS, 1999, 183 (02) :267-280
[10]   Mn-Fe/ZSM5 as a low-temperature SCR catalyst to remove NOx from diesel engine exhaust [J].
Kim, Young Jin ;
Kwon, Hyuk Jae ;
Heo, Iljeong ;
Nam, In-Sik ;
Cho, Byong K. ;
Choung, Jin Woo ;
Cha, Moon-Soon ;
Yeo, Gwon Koo .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2012, 126 :9-21