Effect of Pt on the water resistance of Co-zeolites upon the SCR of NOx with CH4

被引:30
作者
Gutierrez, L [1 ]
Boix, A [1 ]
Petunchi, J [1 ]
机构
[1] CONICET, INCAPE, FIQ, UNL,Inst Invest Catalisis & Petroquim, RA-3000 Santa Fe, Argentina
关键词
selective catalytic reduction; No-x; water resistance; zeolites; PtCo-zeolites; Pt/Co/Al2O3;
D O I
10.1016/S0920-5861(99)00208-4
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The objective of this work was to study the promotional effect of Pt on Go-zeolite (viz. mordenite, ferrierite, ZSM-5 and Y-zeolite) and Co/Al2O3 on the selective catalytic reduction (SCR) of NOx with CH4 under dry and wet reaction stream. After being reduced in H-2 at 350 degrees C, the PtCo bimetallic zeolites showed higher NO to N-2 conversion and selectivity than the monometallic samples, as well as a combination of the latter samples such as mechanical mixtures or two-stage catalysts. After the same pretreatment, under wet reaction stream, the bimetallic samples were also more active. Among the other catalysts studied with 5% of water in the feed, (NO=CH4=1000 ppm, O-2=2%), the NO conversion dropped to zero over Co(2.0)Mor at 500 degrees C and GHSV = 30,000 h(-1), whereas it is 20% in Pt(0.5)Co(2.0)Mor. In Pt/Co/Al2O3 the NO, conversion dropped below 5% with only 2% of water under the same reaction conditions. The specific activity given as molecules of NO converted per total metal atom per second were 16.5 x 10(-4) s(-1) for Pt(0.5)Co(2.0)Fer, 13 x 10(-4) s(-1) for Pt(0.5)Co(2.0)Mor, 4.33 x 10(-4) s(-1) for Pt(0.5)Co(2.0)ZSM-5 and 0.5 x 10(-4) s(-1) for Pt/Co/Al2O3. The Y-zeolite-based samples were inactive in both mono and bimetallic samples. The species initially present in the solid were Pt degrees and Co degrees, together with Co2+ and Pt2+ at exchange positions. Co degrees seems not to participate as an active site in the SCR of NOx. Those species remained after the reaction but some reorganization occurred. A synergetic effect among the different species that enhances both the NO to NO2 reaction, the activation of CH4 and also the ability of the catalyst to adsorb NO, could be responsible for the high activity and selectivity of the bimetallic zeolites. (C)1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:451 / 464
页数:14
相关论文
共 35 条
[31]   DUAL COBALT SPECIATION IN CO/ZSM-5 CATALYSTS [J].
STENCEL, JM ;
RAO, VUS ;
DIEHL, JR ;
RHEE, KH ;
DHERE, AG ;
DEANGELIS, RJ .
JOURNAL OF CATALYSIS, 1983, 84 (01) :109-118
[32]   Synergistic effect in lean NOx reduction by CH4 over Co/Al2O3 and H-zeolite catalysts [J].
Yan, JY ;
Kung, HH ;
Sachtler, WMH ;
Kung, MC .
JOURNAL OF CATALYSIS, 1998, 175 (02) :294-301
[33]   CATALYTIC REDUCTION OF NO BY PROPENE IN THE PRESENCE OF OXYGEN OVER MECHANICALLY MIXED-METAL OXIDES AND CE-ZSM-5 [J].
YOKOYAMA, C ;
MISONO, M .
CATALYSIS LETTERS, 1994, 29 (1-2) :1-6
[34]   REVERSIBLE AND IRREVERSIBLE ADSORPTION OF NITROGEN MONOXIDE ON COBALT ION-EXCHANGED ZSM-5 AND MORDENITE ZEOLITES AT 273-523-K [J].
ZHANG, WX ;
YAHIRO, H ;
IWAMOTO, M ;
IZUMI, J .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1995, 91 (04) :767-771
[35]   XPS STUDY ON THE EFFECTS OF TREATMENTS ON PT2+ AND CO2+ EXCHANGED INTO NAY ZEOLITE [J].
ZSOLDOS, Z ;
VASS, G ;
LU, GN ;
GUCZI, L .
APPLIED SURFACE SCIENCE, 1994, 78 (04) :467-475