The effect of H2 and the presence of hot-O(ads) during the decomposition of N2O on platinum

被引:13
作者
Burch, R [1 ]
Daniells, ST [1 ]
Breen, JP [1 ]
Hu, P [1 ]
机构
[1] Queens Univ Belfast, Sch Chem, CenTACat, Belfast BT9 5AG, Antrim, North Ireland
关键词
N2O+H-2; platinum; catalysts;
D O I
10.1023/B:CATL.0000019338.35919.c5
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 ; 081704 ;
摘要
The decomposition of N2O was studied using a silica-supported Pt catalyst. The catalyst was found to exhibit short-lived activity at low temperatures to yield N-2 and O-(ads), the latter remained adsorbed on the surface and poisoned the active sites. Creation of hot-O-(ads) atoms during N2O decomposition is proposed to allow O-2 desorption at intermediate temperatures. Inclusion of H-2 as a reducing agent greatly enhanced the activity and suppressed low temperature deactivation. Simultaneous and sequential pulsing of N2O and H-2 showed that H-2 inclusion with the N2O gas stream produced the greatest activity. A mechanism involving H-(ads) addition to "hot'' oxygen atoms for H2O formation is proposed.
引用
收藏
页码:103 / 108
页数:6
相关论文
共 29 条
[1]   THE PROMOTION OF SURFACE-CATALYZED REACTIONS BY GASEOUS ADDITIVES - THE ROLE OF A SURFACE OXYGEN TRANSIENT [J].
AU, CT ;
ROBERTS, MW .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1987, 83 :2047-2059
[2]   SPECIFIC ROLE OF TRANSIENT O-(S) AT MG(0001) SURFACES IN ACTIVATION OF AMMONIA BY DIOXYGEN AND NITROUS-OXIDE [J].
AU, CT ;
ROBERTS, MW .
NATURE, 1986, 319 (6050) :206-208
[3]   An investigation of the NO/H2/O2 reaction on noble-metal catalysts at low temperatures under lean-burn conditions [J].
Burch, R ;
Coleman, MD .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1999, 23 (2-3) :115-121
[4]   A transient kinetic study of the mechanism of the NO+H2 reaction over Pt/SiO2 catalysts -: 1.: Isotopic transient kinetics and temperature programmed analysis [J].
Burch, R ;
Shestov, AA ;
Sullivan, JA .
JOURNAL OF CATALYSIS, 1999, 186 (02) :353-361
[5]   Reduction of N2O by H2 on the Ir(110) surface:: oscillations in rate [J].
Carabineiro, SA ;
Nieuwenhuys, BE .
SURFACE SCIENCE, 2001, 495 (1-2) :1-7
[6]   Oscillations in the N2O-H2 reaction over Ir(110).: Route to chaos [J].
Carabineiro, SAC ;
van Noort, WD ;
Nieuwenhuys, BE .
SURFACE SCIENCE, 2003, 532 :96-102
[7]   The development of a new concept: the role of oxygen transients, defect and precursor states in surface reactions [J].
Carley, AF ;
Davies, PR ;
Roberts, MW .
CATALYSIS LETTERS, 2002, 80 (1-2) :25-34
[8]   Oscillating behavior in N2O decomposition over Rh supported on zirconia-based catalysts:: The role of the reaction conditions [J].
Centi, G ;
Dall'Olio, L ;
Perathoner, S .
JOURNAL OF CATALYSIS, 2000, 192 (01) :224-235
[9]  
CENTI G, 2000, APPL CATAL A-GEN, V79, P194
[10]   N2O as an intermediate for the formation of N2 during SCR (NO):: stationary and transient conditions [J].
Denton, P ;
Schuurman, Y ;
Giroir-Fendler, A ;
Praliaud, H ;
Primet, M ;
Mirodatos, C .
COMPTES RENDUS DE L ACADEMIE DES SCIENCES SERIE II FASCICULE C-CHIMIE, 2000, 3 (06) :437-441