Nature of Active Sites and Surface Intermediates during SCR of NO with NH3 by Supported V2O5-WO3/TiO2 Catalysts

被引:301
作者
Zhu, Minghui [1 ]
Lai, Jun-Kun [1 ]
Tumuluri, Uma [2 ,3 ]
Wu, Zili [2 ,3 ]
Wachs, Israel E. [1 ]
机构
[1] Lehigh Univ, Dept Chem & Biomol Engn, Operando Mol Spect & Catalysis Lab, Bethlehem, PA 18015 USA
[2] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA
[3] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA
关键词
VANADIUM-OXIDE CATALYSTS; NITRIC-OXIDE; REACTION-MECHANISM; REDUCTION; AMMONIA; REACTIVITY; TITANIA;
D O I
10.1021/jacs.7b09646
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Time-resolved in situ IR was performed during selective catalytic reduction of NO with NH3 on supported V2O5-WO3/TiO2 catalysts to examine the distribution and reactivity of surface ammonia species on Lewis and Bronsted acid sites. While both species were found to participate in the SCR reaction, their relative population depends on the coverage of the surface vanadia and tungsta sites, temperature, and moisture. Although the more abundant surface NH4,ads+ intermediates dominate the overall SCR reaction, especially for hydrothermally aged catalysts, the minority, surface NH3,ads intermediates exhibit a higher specific SCR activity. (TOF). The current study serves to resolve the long-standing controversy about the active sites for SCR of NO with NH3 by supported V2O5-WO3/TiO2 catalysts.
引用
收藏
页码:15624 / 15627
页数:4
相关论文
共 21 条
[1]   REACTIVITY AND PHYSICOCHEMICAL CHARACTERIZATION OF V2O5-WO3/TIO2 DE-NOX CATALYSTS [J].
ALEMANY, LJ ;
LIETTI, L ;
FERLAZZO, N ;
FORZATTI, P ;
BUSCA, G ;
GIAMELLO, E ;
BREGANI, F .
JOURNAL OF CATALYSIS, 1995, 155 (01) :117-130
[2]   Selective catalytic reduction of nitric oxide by ammonia over V2O5/TiO2, V2O5/TiO2/SiO2, and V2O5-WO3/TiO2 catalysts: Effect of vanadia content on the activation energy [J].
Amiridis, MD ;
Solar, JP .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1996, 35 (03) :978-981
[3]   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
[4]   A complete reaction mechanism for standard and fast selective catalytic reduction of nitrogen oxides on low coverage VOx/TiO2(001) catalysts [J].
Arnarson, Logi ;
Falsig, Hanne ;
Rasmussen, Soren B. ;
Lauritsen, Jeppe V. ;
Moses, Poul Georg .
JOURNAL OF CATALYSIS, 2017, 346 :188-197
[5]   The reaction mechanism for the SCR process on monomer V5+ sites and the effect of modified Bronsted acidity [J].
Arnarson, Logi ;
Falsig, Hanne ;
Rasmussen, Soren B. ;
Lauritsen, Jeppe V. ;
Moses, Poul Georg .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2016, 18 (25) :17071-17080
[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]   SELECTIVE CATALYTIC REDUCTION OF NO WITH NH3 ON SO4(-2)/TIO2 SUPERACID CATALYST [J].
CHEN, JP ;
YANG, RT .
JOURNAL OF CATALYSIS, 1993, 139 (01) :277-288
[8]   Present status and perspectives in de-NOx SCR catalysis [J].
Forzatti, P .
APPLIED CATALYSIS A-GENERAL, 2001, 222 (1-2) :221-236
[9]   Effect of operating variables on the enhanced SCR reaction over a commercial V2O5-WO3/TiO2 catalyst for stationary applications [J].
Forzatti, Pio ;
Nova, Isabella ;
Tronconi, Enrico ;
Kustov, Arkady ;
Thogersen, Joakim Reimer .
CATALYSIS TODAY, 2012, 184 (01) :153-159
[10]   A review on selective catalytic reduction of NOx by supported catalysts at 100-300 °C-catalysts, mechanism, kinetics [J].
Fu, Mengfan ;
Li, Caiting ;
Lu, Pei ;
Qu, Long ;
Zhang, Mengying ;
Zhou, Yang ;
Yu, Minge ;
Fang, Yang .
CATALYSIS SCIENCE & TECHNOLOGY, 2014, 4 (01) :14-25