Excellent performance of one-pot synthesized Fe-containing MCM-22 zeolites for the selective catalytic reduction of NOxwith NH3

被引:27
作者
Chen, Jialing [1 ]
Peng, Gang [1 ]
Zheng, Wei [1 ]
Zhang, Wenbo [1 ]
Guo, Li [1 ]
Wu, Xiaoqing [1 ]
机构
[1] Wuhan Univ Sci & Technol, Key Lab Hubei Prov Coal Convers & New Carbon Mat, Sch Chem & Chem Engn, Heping Ave 947, Wuhan 430081, Peoples R China
关键词
OF-THE-ART; NITRIC-OXIDE; HYDROTHERMAL STABILITY; N2O DECOMPOSITION; REACTION-KINETICS; NITROGEN-OXIDES; ACTIVE-SITES; SI/AL RATIO; NH3-SCR; NOX;
D O I
10.1039/d0cy00989j
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
A superior Fe-containing MCM-22 zeolite prepared by a one-pot synthesis method (OP-Fe/M22) showed excellent NH(3)selective catalytic reduction (NH3-SCR) activity and almost 100% N(2)selectivity in a wide temperature window (200-500 degrees C). To investigate the effects of preparation strategies on the NH3-SCR reaction, other three Fe/MCM-22 zeolites with similar iron content (4.4-4.8 wt%) were prepared by solid-state ion exchange (SSIE-Fe/M22), incipient wetness impregnation (IM-Fe/M22) and mechanical mixing (MM-Fe/M22) methods, respectively. Catalytic results in NH3-SCR demonstrate that OP-Fe/M22 gives significantly higher activity in the whole temperature range (100-550 degrees C) than the other three post-synthesized catalysts. As revealed by XRD, UV-vis, H-2-TPR, NH3-TPD, and Py-IR experiments, OP-Fe/M22 has the highest concentrations of isolated Fe(3+)species and acid sites, and the lowest concentration of Fe(2)O(3)nanoparticles among the four catalysts, which ensures its highest activity in the NH3-SCR reaction. Besides, OP-Fe/M22 exhibits the higher activity both in NH(3)oxidation and NO oxidation reactions than IM-Fe/M22, indicating the better NO oxidation ability and NH(3)storage capacity of OP-Fe/M22 which also facilitates the NH3-SCR process. In contrast with Cu-based MCM-22 zeolite obtained from the incipient wetness impregnation method at similar metal content (5% Cu/M22), OP-Fe/M22 shows comparable activity with 5% Cu/M22 in the low-temperature range (100-300 degrees C) while obviously higher activity at high temperatures (300-550 degrees C). Moreover, by removing part of undesired iron oxides in OP-Fe/M22 through mild acid post-treatments, the NH3-SCR activity of OP-Fe/M22 in the medium and high temperature ranges (200-550 degrees C) can be further improved, suggesting that OP-Fe/M22 is a potential catalyst with highly-efficient NH3-SCR activity in a wide temperature window.
引用
收藏
页码:6583 / 6598
页数:16
相关论文
共 82 条
[1]   The effect of iron loading and hydrothermal aging on one-pot synthesized Fe/SAPO-34 for ammonia SCR [J].
Andonova, Stanislava ;
Tamm, Stefanie ;
Montreuil, Clifford ;
Lambert, Christine ;
Olsson, Louise .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2016, 180 :775-787
[2]  
BAERLOCHER C, 1994, STUD SURF SCI CATAL, V85, P391
[3]   Recent advances in automotive catalysis for NOx emission control by small-pore microporous materials [J].
Beale, A. M. ;
Gao, F. ;
Lezcano-Gonzalez, I. ;
Peden, C. H. F. ;
Szanyi, J. .
CHEMICAL SOCIETY REVIEWS, 2015, 44 (20) :7371-7405
[4]   The influence of the preparation procedures on the catalytic activity of Fe-BEA zeolites in SCR of NO with ammonia and N2O decomposition [J].
Boron, Pawel ;
Chmielarz, Lucjan ;
Gurgul, Jacek ;
Latka, Kazimierz ;
Gil, Barbara ;
Krafft, Jean-Marc ;
Dzwigaj, Stanislaw .
CATALYSIS TODAY, 2014, 235 :210-225
[5]   Hydrothermal deactivation of Fe-ZSM-5 catalysts for the selective catalytic reduction of NO with NH3 [J].
Brandenberger, Sandro ;
Kroecher, Oliver ;
Casapu, Maria ;
Tissler, Arno ;
Althoff, Roderik .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2011, 101 (3-4) :649-659
[6]   The determination of the activities of different iron species in Fe-ZSM-5 for SCR of NO by NH3 [J].
Brandenberger, Sandro ;
Kroecher, Oliver ;
Tissler, Arno ;
Althoff, Roderik .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 95 (3-4) :348-357
[7]   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
[8]   THE ROLE OF POLYVALENT CATIONS IN DEVELOPING STRONG ACIDITY - A STUDY OF LANTHANUM-EXCHANGED ZEOLITES [J].
CARVAJAL, R ;
CHU, PJ ;
LUNSFORD, JH .
JOURNAL OF CATALYSIS, 1990, 125 (01) :123-131
[9]   A comparative study of N2O formation during the selective catalytic reduction of NOx with NH3 on zeolite supported Cu catalysts [J].
Chen, Hai-Ying ;
Wei, Zhehao ;
Kollar, Marton ;
Gao, Feng ;
Wang, Yilin ;
Szanyi, Janos ;
Peden, Charles H. F. .
JOURNAL OF CATALYSIS, 2015, 329 :490-498
[10]   Regulation of Framework Aluminum Siting and Acid Distribution in H-MCM-22 by Boron Incorporation and Its Effect on the Catalytic Performance in Methanol to Hydrocarbons [J].
Chen, Jialing ;
Liang, Tingyu ;
Li, Junfen ;
Wang, Sen ;
Qin, Zhangfeng ;
Wang, Pengfei ;
Huang, Lizhi ;
Fan, Weibin ;
Wang, Jianguo .
ACS CATALYSIS, 2016, 6 (04) :2299-2313