Reactivity of V2O5 catalysts for the selective catalytic reduction of NO by NH3: Influence of vanadia loading, H2O, and SO2

被引:358
作者
Amiridis, MD
Wachs, IE
Deo, G
Jehng, JM
Kim, DS
机构
[1] WR GRACE & CO CONN,DIV RES,COLUMBIA,MD 21044
[2] LEHIGH UNIV,ZETTLEMOYER CTR SURFACE STUDIES,BETHLEHEM,PA 18015
[3] LEHIGH UNIV,DEPT CHEM ENGN,BETHLEHEM,PA 18015
关键词
D O I
10.1006/jcat.1996.0182
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 [物理化学]; 081704 [应用化学];
摘要
A systematic investigation of the selective catalytic reduction (SCR) of NO by NH3 over V2O5/TiO2 catalysts of variable vanadia loading has been carried out at 623 K. Kinetic studies were conducted both in the presence and in the absence of H2O and SO2, The structure of the various catalysts, as well as adsorbed species present on their surface, was characterized by in situ Raman and infrared spectroscopies, Under dry and SO2-free conditions, the turnover frequency of the SCR reaction was found to go through a maximum with vanadia surface coverage at approximately half a monolayer, The observed decrease in the SCR turnover frequency at vanadia surface coverages exceeding half a monolayer can be attributed to the loss of strong acid sites which are associated with the TiO2 support. Addition of H2O to the reacting gas mixture results in a decrease in the SCR turnover frequency of approximately 40-50%, which is independent of the vanadia surface coverage. In situ Raman results suggest that such a decrease can be attributed to the competitive adsorption of H2O on the active vanadia sites, The presence of SO2 in the gas phase during the SCR reaction results in a significant increase of the turnover frequency at low vanadia surface coverages, while it has no effect at vanadia surface coverages above half a monolayer, Raman and infrared results suggest that the effect of SO2 can be attributed to the formation of surface sulfate species, which are only present on the titania surface below half a monolayer coverage due to repulsive interactions between the surface vanadia and sulfate species. (C) 1996 Academic Press, Inc.
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页码:247 / 253
页数:7
相关论文
共 32 条
[1]
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
[2]
SELECTIVE CATALYTIC REDUCTION OF NITRIC-OXIDE OVER VANADIA GRAFTED ON TITANIA - INFLUENCE OF VANADIA LOADING ON STRUCTURAL AND CATALYTIC PROPERTIES OF CATALYSTS [J].
BAIKER, A ;
HANDY, B ;
NICKL, J ;
SCHRAMLMARTH, M ;
WOKAUN, A .
CATALYSIS LETTERS, 1992, 14 (01) :89-99
[3]
DESIGN OF MONOLITH CATALYSTS FOR POWER-PLANT NOX EMISSION CONTROL [J].
BEECKMAN, JW ;
HEGEDUS, LL .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1991, 30 (05) :969-978
[4]
MEASUREMENT OF THE EFFECTIVE DIFFUSION-COEFFICIENT OF NITROGEN MONOXIDE THROUGH POROUS MONOLITH-TYPE CERAMIC CATALYSTS [J].
BEECKMAN, JW .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1991, 30 (02) :428-430
[5]
Bosch H., 1986, CATAL TODAY, V2, P369, DOI DOI 10.1016/0920-5861(88)80002-6
[7]
MECHANISM OF POISONING OF THE V2O5 TIO2 CATALYST FOR THE REDUCTION OF NO BY NH3 [J].
CHEN, JP ;
YANG, RT .
JOURNAL OF CATALYSIS, 1990, 125 (02) :411-420
[8]
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
[9]
REACTIVITY OF SUPPORTED VANADIUM-OXIDE CATALYSTS - THE PARTIAL OXIDATION OF METHANOL [J].
DEO, G ;
WACHS, IE .
JOURNAL OF CATALYSIS, 1994, 146 (02) :323-334
[10]
SOLID-STATE V-15 NMR STRUCTURAL STUDIES ON SUPPORTED VANADIUM(V) OXIDE CATALYSTS - VANADIUM-OXIDE SURFACE-LAYERS ON ALUMINA AND TITANIA SUPPORTS [J].
ECKERT, H ;
WACHS, IE .
JOURNAL OF PHYSICAL CHEMISTRY, 1989, 93 (18) :6796-6805