Detailed surface reaction mechanism for reduction of NO by CO

Abstract In order to meet the stringent regulatory norms of NO x and CO emitted by automobiles, reduction of these pollutants has become an intense field of research. Various catalysts like Pt, Rh, Ir, Cu, and Fe have been found to possess high activity for the reduction of NO. However, the available detailed surface reaction mechanisms are not satisfactory in clarifying all the aspects of the simultaneous reduction of NO and oxidation of CO. Here we have developed a quantitative surface reaction mechanism based on elementary steps, in order to comprehend the phenomena of catalytic reduction of NO by CO. Eleven elementary steps are proposed for the NO–CO and NO–CO–O 2 systems on Pt group catalysts. The elementary reaction mechanism is coupled with the continuously stirred tank reactor/packed bed reactor models and the simulation results are validated against literature experiments for the NO–CO reaction on Pt, and the NO–CO–O 2 reaction on Ir catalyst. Despite the simplicity, the CSTR model is able to capture the observed phenomena well on Pt and Ir catalysts. The effect of O 2 on the activity of CO for NO reduction is also analysed in detail through the simulations.

[1]  G. G. Stokes "J." , 1890, The New Yale Book of Quotations.

[2]  M. Shimokawabe,et al.  Selective Catalytic Reduction of NO by CO over Supported Iridium and Rhodium Catalysts , 2004 .

[3]  F. Meunier,et al.  A review of the selective reduction of NOx, with hydrocarbons under lean-burn conditions with non-zeolitic oxide and platinum group metal catalysts , 2002 .

[4]  Alexis T. Bell,et al.  Decomposition and reduction of NO on transition metal surfaces: bond order conservation Morse potential analysis , 1993 .

[5]  Brent H. Shanks,et al.  Kinetics of NO reduction by CO over supported rhodium catalysts: Isotopic cycling experiments , 1989 .

[6]  Dennys E. Angove,et al.  The Formation and Hydrolysis of Isocyanic Acid during the Reaction of NO, CO, and H2 Mixtures on Supported Platinum, Palladium, and Rhodium , 2001 .

[7]  W. H. Weinberg,et al.  Effect of preadsorbed oxygen on the adsorption of CO on Ir(110) , 1997 .

[8]  H. Kawakami,et al.  Selective reduction of nitric oxide over platinum catalysts in the presence of sulfur dioxide and excess oxygen , 1992 .

[9]  Tao Zhang,et al.  Unique properties of Ir/ZSM-5 catalyst for NO reduction with CO in the presence of excess oxygen , 2003 .

[10]  O Deutschmann,et al.  Detailed surface reaction mechanism in a three-way catalyst. , 2001, Faraday discussions.

[11]  M. S. Hegde,et al.  Combustion synthesis of nanometal particles supported on α-Al2O3: CO oxidation and NO reduction catalysts , 1999 .

[12]  Gbmm Guy Marin,et al.  Competing reactions in three-way catalytic converters : modelling of the NOx conversion maximum in the light-off curves under net oxidising conditions , 2000 .

[13]  Young K. Park,et al.  Construction and optimization of complex surface‐reaction mechanisms , 2000 .

[14]  H. Praliaud,et al.  Kinetics of the CO+NO Reaction over Bimetallic Platinum–Rhodium on Alumina: Effect of Ceria Incorporation into Noble Metals , 2002 .

[15]  D. Belton,et al.  Reaction of coadsorbed nitric oxide and nitrogen atoms on Rh(111) , 1995 .

[16]  L. Leclercq,et al.  Kinetics of the CO+N2O Reaction over Noble Metals: I. Pt/Al2O3 , 1999 .

[17]  Faraday Discuss , 1985 .

[18]  Robert J. Farrauto,et al.  Selective catalytic reduction of nitric oxide by hydrocarbons , 1996 .

[19]  T. Lin,et al.  Modulated molecular beam scattering of CO and NO from Pt(111) and the stepped Pt(557) crystal surfaces , 1981 .

[20]  P. Ciambelli,et al.  Potentialities and limitations of lean de-NOx catalysts in reducing automotive exhaust emissions , 2000 .

[21]  Mônica A. P. Silva,et al.  Reduction of NO by CO on Pt-MoO 3/?-Al 2O 3 catalysts , 2003 .

[22]  Andrew G. Glen,et al.  APPL , 2001 .

[23]  L. Murrell,et al.  The NOCO reaction in the presence of excess O2 as catalyzed by iridium , 1976 .

[24]  D. W. Goodman,et al.  Comparative kinetic studies of CO$z.sbnd;O2 and CO$z.sbnd;NO reactions over single crystal and supported rhodium catalysts , 1986 .

[25]  A. Sarkar,et al.  CO oxidation and NO reduction over supported Pt-Rh and Pd-Rh nanocatalysts: a comparative study , 2005 .

[26]  Alexis T. Bell,et al.  Reduction of NO by CO over silica-supported rhodium: infrared and kinetic studies , 1983 .

[27]  G. Zgrablich,et al.  Lattice-gas study of the kinetics of catalytic conversion of NO–CO mixtures on rhodium surfaces , 2001 .

[28]  K. Krischer,et al.  Kinetic oscillations in the Pt(100)/NO+CO system: Bifurcation analysis , 1992 .

[29]  V. Pitchon,et al.  The current state of research on automotive lean NOx catalysis , 1997 .

[30]  Pascal Granger,et al.  Kinetics of the NO and CO Reaction over Platinum Catalysts: I. Influence of the Support☆ , 1998 .

[31]  Kathleen C. Taylor,et al.  Selective reduction of nitric oxide over noble metals , 1980 .