Highly dispersed CeO2 on carbon nanotubes for selective catalytic reduction of NO with NH3

被引:167
作者
Fang, Cheng [1 ,2 ,3 ]
Zhang, Dengsong [1 ,2 ]
Shi, Liyi [1 ,3 ]
Gao, Ruihua [1 ]
Li, Hongrui [1 ]
Ye, Liping [4 ]
Zhang, Jianping [2 ]
机构
[1] Shanghai Univ, Res Ctr Nano Sci & Technol, Shanghai 200444, Peoples R China
[2] Shanghai Univ, Dept Chem, Shanghai 200444, Peoples R China
[3] Shanghai Univ, Sch Mat Sci & Engn, Shanghai 200072, Peoples R China
[4] Shanghai Res Inst Chem Ind, Shanghai 200062, Peoples R China
基金
中国国家自然科学基金;
关键词
LOW-TEMPERATURE SCR; NITRIC-OXIDE; MANGANESE OXIDES; MIXED OXIDES; MECHANISM; AMMONIA; MNOX/TIO2; OXIDATION; ADSORPTION; FE-ZSM-5;
D O I
10.1039/c2cy20670f
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
Highly dispersed CeO2 on carbon nanotubes (CNTs) is successfully prepared by a pyridine-thermal route for selective catalytic reduction (SCR) of NO with NH3. This catalyst is mainly characterized by the techniques of X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction by hydrogen (H-2-TPR), temperature-programmed desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS). The results of the XRD, TEM and TPR analysis show that the CeO2 particles on the CNTs are highly dispersed with a strong interaction between the particles and the CNTs. The NH3-TPD profiles indicate that this catalyst exhibits abundant strong acid sites. Furthermore, the O 1s XPS spectra show that the O-alpha/(O-alpha + O-beta) ratio of this catalyst is very high, which can result in more surface oxygen vacancies and therefore favor the NH3-SCR reaction. Compared with the catalysts prepared by impregnation or physical mixture methods, the catalyst prepared by the pyridine-thermal route presents the best NH3-SCR activity in the temperature range of 150-380 degrees C as well as favourable stability and good SO2 or H2O resistance. More than 90% of NO can be removed in the range of 250-370 degrees C with a desirable N-2 selectivity. Moreover, the NO conversion can be kept at about 97% with the presence of SO2 or H2O at 300 degrees C. In addition, this catalyst shows a high catalytic activity with a NO conversion remaining constant at ca. 98% during a 16 h continuous run duration at 300 degrees C. Highly dispersed CeO2 on the CNTs as well as the strong interaction between the particles and the CNTs, the large amounts of strong acid sites and the high O-alpha/(O-alpha + O-beta) ratio could be ascribed to the excellent NH3-SCR performance of the catalyst prepared by the pyridine-thermal route.
引用
收藏
页码:803 / 811
页数:9
相关论文
共 69 条
[1]   Carbon supports for low-temperature fuel cell catalysts [J].
Antolini, Ermete .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 88 (1-2) :1-24
[2]  
[白书立 BAI Shu-li], 2009, [燃料化学学报, Journal of Fuel Chemistry and Technology], V37, P583
[3]   SO2-promoted reduction of NO with NH3 over vanadium molecularly anchored on the surface of carbon nanotubes [J].
Bai, Shuli ;
Zhao, Jianghong ;
Wang, Li ;
Zhu, Zhenping .
CATALYSIS TODAY, 2010, 158 (3-4) :393-400
[4]   Selective catalytic reduction of NOx by NH3 on Fe/HBEA zeolite catalysts in oxygen-rich exhaust [J].
Balle, Peter ;
Geiger, Bastian ;
Kureti, Sven .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 85 (3-4) :109-119
[5]   Screening of doped MnOx-CeO2 catalysts for low-templerature NO-SCR [J].
Casapu, Maria ;
Kroecher, Oliver ;
Elsener, Martin .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 88 (3-4) :413-419
[6]   Adsorption of NH3 and NO2 molecules on carbon nanotubes [J].
Chang, H ;
Lee, JD ;
Lee, SM ;
Lee, YH .
APPLIED PHYSICS LETTERS, 2001, 79 (23) :3863-3865
[7]   Promotional Effect of Ce-doped V2O5-WO3/TiO2 with Low Vanadium Loadings for Selective Catalytic Reduction of NOx by NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (50) :21177-21184
[8]   Noncovalent sidewall functionalization of single-walled carbon nanotubes for protein immobilization [J].
Chen, RJ ;
Zhang, YG ;
Wang, DW ;
Dai, HJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (16) :3838-3839
[9]   Selective catalytic reduction of NO over carbon nanotubes supported CeO2 [J].
Chen, Xiongbo ;
Gao, Shan ;
Wang, Haiqiang ;
Liu, Yue ;
Wu, Zhongbiao .
CATALYSIS COMMUNICATIONS, 2011, 14 (01) :1-5
[10]   Effect of oxygen concentration on the NOx reduction with ammonia overV2O5-WO3/TiO2 catalyst [J].
Djerad, S ;
Crocoll, M ;
Kureti, S ;
Tifouti, L ;
Weisweiler, W .
CATALYSIS TODAY, 2006, 113 (3-4) :208-214