Selective catalytic reduction of NO with NH3 over Mo-Fe/beta catalysts: the effect of Mo loading amounts

被引:32
作者
Deng, Jianlin [1 ]
Liu, Jixing [1 ]
Song, Weiyu [1 ]
Zhao, Zhen [1 ]
Zhao, Liang [1 ]
Zheng, Huiling [1 ]
Lee, Alex Chinghuan [2 ]
Chen, Yongsheng [2 ]
Liu, Jian [1 ]
机构
[1] China Univ Petr, Beijing Key Lab Oil & Gas Pollut Control, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China
[2] Chinese Univ Hong Kong, Dept Mech & Automat Engn, Hong Kong, Hong Kong, Peoples R China
来源
RSC ADVANCES | 2017年 / 7卷 / 12期
基金
中国国家自然科学基金;
关键词
DENSITY-FUNCTIONAL THEORY; MIXED-OXIDE CATALYST; FE-BEA; LOW-TEMPERATURE; N2O DECOMPOSITION; SCR-NOX; AMMONIA; SPECTROSCOPY; ZEOLITES; FE-ZSM-5;
D O I
10.1039/c6ra27126j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A series of Mox-Fe/beta catalysts with constant Fe and variable Mo content were synthesized and investigated for selective catalytic reduction (SCR) of NOx with NH3. It was found that the Mo-0.2-Fe/beta catalyst exhibited excellent activity, N-2 selectivity and preferable resistance to H2O and SO2. The Mo-x-Fe/ beta catalysts were characterized by various analytical techniques. TEM and SEM images showed that the addition of Mo could enhance the dispersion of iron oxides. The results of NH3-TPD and Py-IR indicated that the introduction of Mo resulted in a change of Bronsted acidity, which was associated with high-temperature SCR activity. XPS and XANES results showed that the introduction of Mo resulted in a change of Fe2+ content, which determined the low-temperature activity. DFT calculations showed the strong effects of Mo on the crystal structure, charge distribution and oxygen vacancy formation energy of iron oxides, which further explained the role of Mo in the catalyst behaviors during the SCR process.
引用
收藏
页码:7130 / 7139
页数:10
相关论文
共 53 条
[1]   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
[2]   PROJECTOR AUGMENTED-WAVE METHOD [J].
BLOCHL, PE .
PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979
[3]   Application of copper-gold alloys in catalysis: current status and future perspectives [J].
Bracey, Charlotte L. ;
Ellis, Peter R. ;
Hutchings, Graham J. .
CHEMICAL SOCIETY REVIEWS, 2009, 38 (08) :2231-2243
[4]   The role of Bronsted acidity in the selective catalytic reduction of NO with ammonia over Fe-ZSM-5 [J].
Brandenberger, Sandro ;
Kroecher, Oliver ;
Wokaun, Alexander ;
Tissler, Arno ;
Althoff, Roderik .
JOURNAL OF CATALYSIS, 2009, 268 (02) :297-306
[5]   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
[6]   Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:: A review [J].
Busca, G ;
Lietti, L ;
Ramis, G ;
Berti, F .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 18 (1-2) :1-36
[7]  
Chen P., 2014, APPL CATAL B-ENVIRON, V148, P520
[8]   Insights into current limitations of density functional theory [J].
Cohen, Aron J. ;
Mori-Sanchez, Paula ;
Yang, Weitao .
SCIENCE, 2008, 321 (5890) :792-794
[9]   Multiplet effects in X-ray spectroscopy [J].
de Groot, F .
COORDINATION CHEMISTRY REVIEWS, 2005, 249 (1-2) :31-63
[10]   Control of metal ion species in zeolites by distribution of aluminium in the framework: From structural analysis to performance under real conditions of SCR-NOx and NO, N2O decomposition [J].
Dedecek, J. ;
Capek, L. ;
Sazama, P. ;
Sobalik, Z. ;
Wichterlova, B. .
APPLIED CATALYSIS A-GENERAL, 2011, 391 (1-2) :244-253