Manganese oxide catalysts supported on TiO2, Al2O3, and SiO2:: A comparison for low-temperature SCR of NO with NH3

被引:219
作者
Smirniotis, Panagiotis G. [1 ]
Sreekanth, Pavani M.
Pena, Donovan A.
Jenkins, Robert G.
机构
[1] Univ Cincinnati, Dept Chem & Mat Engn, Cincinnati, OH 45221 USA
[2] Univ Vermont, Sch Engn, Burlington, VT 05405 USA
关键词
D O I
10.1021/ie060484t
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
A series of TiO2-, Al2O3-, and SiO2- supported manganese oxide catalysts were prepared, characterized, and catalytically tested for selective catalytic reduction (SCR) of NO with NH3 in the presence of excess oxygen at low temperatures (373-523 K). Various commercial supports were used in this study to find out the influence of surface area, support nature (acidic, basic), and crystalline phase on SCR activity. XRD studies reveal the presence of anatase and rutile phases for titania supports and the existence of gamma-alumina in the case of alumina support. Silica support was amorphous. No independent lines corresponding to the crystalline MnO2 were observed on pure anatase and rutile samples. However, the presence of MnO2 was confirmed on other supports by XRD. BET surface area values suggest that specific surface area of the supports was decreased after impregnating with MnO2. The FT-IR and ammonia TPD studies indicate the presence of two types of acid sites on these catalysts, and the acidic strength of the catalysts is higher than the corresponding pure supports. XPS results revealed the presence of two types of manganese oxides, MnO2 (642.4 eV) and Mn2O3 (641.2 eV), on all the samples. The SCR performance of the supported Mn catalysts decreased in the following order: TiO2 (anatase, high surface area) > TiO2 (rutile) > TiO2 (anatase, rutile) > gamma-Al2O3 > SiO2 > TiO2 (anatase, low surface area). Quantitative NO conversion with 100% N-2 selectivity was achieved at 393 K with Mn supported on TiO2 (anatase). TiO2--supported MnO2 catalysts showed more promising SCR activity than Al2O3- or SiO2-supported manganese oxide catalysts. Various characterization techniques suggest that Lewis acid sites, a high surface concentration of MnO2, and redox properties are important in achieving high catalytic performance at low temperatures.
引用
收藏
页码:6436 / 6443
页数:8
相关论文
共 28 条
[1]   Reactivity of V2O5 catalysts for the selective catalytic reduction of NO by NH3: Influence of vanadia loading, H2O, and SO2 [J].
Amiridis, MD ;
Wachs, IE ;
Deo, G ;
Jehng, JM ;
Kim, DS .
JOURNAL OF CATALYSIS, 1996, 161 (01) :247-253
[2]   An FT-IR study of ammonia adsorption and oxidation over anatase-supported metal oxides [J].
Amores, JMG ;
Escribano, VS ;
Ramis, G ;
Busca, G .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 13 (01) :45-58
[3]  
[Anonymous], CATTECH
[4]   Alumina- and titania-based monolithic catalysts for low temperature selective catalytic reduction of nitrogen oxides [J].
Blanco, J ;
Avila, P ;
Suárez, S ;
Martín, JA ;
Knapp, C .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2000, 28 (3-4) :235-244
[5]  
Bosch H., 1986, CATAL TODAY, V2, P369, DOI DOI 10.1016/0920-5861(88)80002-6
[6]   SELECTIVE CATALYTIC REDUCTION OF NITRIC-OXIDE OVER AMORPHOUS AND CRYSTALLINE CHROMIA .1. COMPARATIVE-STUDY OF ACTIVITIES [J].
CURRYHYDE, HE ;
MUSCH, H ;
BAIKER, A .
APPLIED CATALYSIS, 1990, 65 (02) :211-223
[7]   INFRARED AND RAMAN-STUDY OF THE ADSORPTION OF NH3, PYRIDINE, NO AND NO2 ON ANATASE [J].
DINES, TJ ;
ROCHESTER, CH ;
WARD, AM .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1991, 87 (04) :643-651
[8]   Kinetics of selective catalytic reduction of nitric oxide by ammonia over vanadia/titania [J].
Dumesic, JA ;
Topsoe, NY ;
Topsoe, H ;
Chen, Y ;
Slabiak, T .
JOURNAL OF CATALYSIS, 1996, 163 (02) :409-417
[9]   INFRARED-SPECTRA OF AMMONIA ADSORBED ON TITANIUM-DIOXIDE [J].
HINO, M ;
MIKAMI, Y .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1983, 56 (11) :3495-3496
[10]   ALUMINA-SUPPORTED MANGANESE OXIDE CATALYSTS .2. SURFACE CHARACTERIZATION AND ADSORPTION OF AMMONIA AND NITRIC-OXIDE [J].
KAPTEIJN, F ;
SINGOREDJO, L ;
VANDRIEL, M ;
ANDREINI, A ;
MOULIJN, JA ;
RAMIS, G ;
BUSCA, G .
JOURNAL OF CATALYSIS, 1994, 150 (01) :105-116