FTIR study of species arising after NO adsorption and NO+O2 co-adsorption on CoY:: comparison with Co-ZSM-5

被引:74
作者
Ivanova, E
Hadjiivanov, K [1 ]
Klissurski, D
Bevilacqua, M
Armaroli, T
Busca, G
机构
[1] Bulgarian Acad Sci, Inst Gen & Inorgan Chem, BU-1113 Sofia, Bulgaria
[2] Univ Genoa, Ist Chim, Fac Ingn, I-16129 Genoa, Italy
关键词
FTIR spectroscopy; adsorption; nitrogen monoxide; selective catalytic reduction; Co-ZSM-5; CoY; NaY;
D O I
10.1016/S1387-1811(01)00311-0
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
CoY, with its low activity in selective catalytic reduction (SCR) of nitrogen oxides, differs from Co-exchanged pentasil zeolites (e.g. Co-ZSM-5). To obtain more information on the SCR mechanism, the NOx species formed after NO adsorption and NO + O-2 co-adsorption on CoY were studied by means of IR spectroscopy and the results were compared with those obtained for Co-ZSM-5. NO adsorption on CoY leads to the formation of Co2+(NO)(2) species (v(s) at 1900 and v(as) at 1819 cm(-1)) which are characterised by a stability similar to the stability of the dinitrosyls formed on Co-ZSM-5 (1894 and 1812 cm(-1)). This suggests that the Co2+ (NO)2 species are not involved in the SCR. The stable species produced upon NO + O-2 co-adsorption on the two samples are very different. The principal compounds formed on Co-ZSM-5 are surface monodentate nitrates characterised by an IR band at approximate to 1540 cm(-1). These nitrates easily interact with hydrocarbons, which confirms that they are key species in SCR. No monodentate nitrates are formed on CoY. Stable symmetric nitrates (1488 and 1473 cm(-1)) and less stable species, probably bidentate nitrates (1620 and 1320 cm(-1)) appear instead. The symmetric nitrates are converted, during evacuation, into nitro-compounds (1563 and 1383 cm(-1)) that are not removed even by evacuation at 743 K. Interaction of methane with the nitrates on CoY only leads to their partial reduction to nitro-compounds. These results account for the low SCR activity of CoY. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:299 / 309
页数:11
相关论文
共 35 条
[1]   Mechanistic cause of hydrocarbon specificity over Cu/ZSM-5 and Co/ZSM-5 catalysts in the selective catalytic reduction of NOx [J].
Adelman, BJ ;
Beutel, T ;
Lei, GD ;
Sachtler, WMH .
JOURNAL OF CATALYSIS, 1996, 158 (01) :327-335
[2]  
Aylor AW, 1996, STUD SURF SCI CATAL, V101, P661
[3]   Bronsted acidity of extraframework debris in steamed Y zeolites from the FTIR study of CO adsorption [J].
Cairon, O ;
Chevreau, T ;
Lavalley, JC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1998, 94 (19) :3039-3047
[4]  
CAMPA M, 1998, APPL CATAL B-ENVIRON, V8, P315
[5]   Catalytic activity of Co-ZSM-5 for the abatement of NOx with methane in the presence of oxygen [J].
Campa, MC ;
DeRossi, S ;
Ferraris, G ;
Indovina, V .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 8 (03) :315-331
[6]   Reduction of NOx over Fe/ZSM-5 catalysts:: mechanistic causes of activity differences between alkanes [J].
Chen, HY ;
Voskoboinikov, T ;
Sachtler, WMH .
CATALYSIS TODAY, 1999, 54 (04) :483-494
[7]   IR spectroscopic study of NOx adsorption and NOx-O-2 coadsorption on Co2+/SiO2 catalysts [J].
Djonev, B ;
Tsyntsarski, B ;
Klissurski, D ;
Hadjiivanov, K .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (22) :4055-4063
[8]   An FTIR study an the mechanism of the reaction between nitrogen dioxide and propene over acidic mordenites [J].
Gerlach, T ;
Schütze, FW ;
Baerns, M .
JOURNAL OF CATALYSIS, 1999, 185 (01) :131-137
[9]   Effect of water on the reduction of NOx with propane on Fe-ZSM-5.: An FTIR mechanistic study [J].
Hadjiivanov, K ;
Knözinger, H ;
Tsyntsarski, B ;
Dimitrov, L .
CATALYSIS LETTERS, 1999, 62 (01) :35-40
[10]   Stability and reactivity of the nitrogen-oxo species formed after NO adsorption and NO+O2 coadsorption on Co-ZSM-5:: An FTIR spectroscopic study [J].
Hadjiivanov, K ;
Tsyntsarski, B ;
Nikolova, T .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1999, 1 (18) :4521-4528