Catalytic reduction of nitric oxide by carbon monoxide over calcined limestone: reversible deactivation in the presence of carbon dioxide

Abstract The influence of carbon dioxide on nitric oxide reduction by carbon monoxide catalyzed over a porous limestone Stevns Chalk was studied in a fixed bed quartz reactor at 850°C under alternating oxidizing and reducing conditions, and under constant reducing conditions. The presence of carbon dioxide was found to inhibit the catalytic nitric oxide reduction. The nitric oxide reduction by carbon monoxide was found to fit the power law expression − r NO = k · [NO] 1 · [CO] (0.8 – 0.9) · [CO 2 ] −0.7 at ambient pressures, for 300–1200 ppmv NO, 2–6 vol.-% CO and 2–16 vol.-% CO 2 . A simple mechanism for the nitric oxide reduction is proposed and a rate expression which agrees with the experimental results is derived. This study indicates that investigations of nitric oxide reduction by carbon monoxide catalyzed by CaO should be carried out in the presence of relevant concentrations of carbon dioxide.

[1]  R. S. Hansen,et al.  Reduction of nitric oxide with carbon monoxide on the Rh(100) single-crystal surface , 1986 .

[2]  Jan Erik Johnsson,et al.  Formation and reduction of nitrogen oxides in fluidized-bed combustion☆ , 1994 .

[3]  Robert H. Borgwardt,et al.  Sintering of nascent calcium oxide , 1989 .

[4]  Bo G Leckner,et al.  Oxidation of Volatile Nitrogen Compounds During Combustion in Circulating Fluidized Bed Boilers , 1991 .

[5]  Peter Glarborg,et al.  Kinetic modeling and sensitivity analysis of nitrogen oxide formation in well-stirred reactors , 1986 .

[6]  Daizo Kunii,et al.  CATALYTIC REDUCTION OF NITRIC OXIDE BY HYDROGEN OVER CALCINED LIMESTONE , 1983 .

[7]  K. Yaldram,et al.  NOCO reaction on square and hexagonal surfaces: A Monte Carlo simulation , 1991 .

[8]  P. Hansma,et al.  EVIDENCE FOR AN OXYGEN INTERMEDIATE IN THE CATALYTIC REDUCTION OF NO BY CO ON RHODIUM SURFACES , 1980 .

[9]  B. Leckner,et al.  Influence of SO2 on the NON2O chemistry in fluidized bed combustion: 2. Interpretation of full-scale observations based on laboratory experiments , 1993 .

[10]  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 .

[11]  K. Dam-Johansen,et al.  High-temperature reaction between sulphur dioxide and limestone—III. A grain-micrograin model and its verification , 1991 .

[12]  P. Hansen,et al.  High-temperature reaction between sulphur dioxide and limestone. V: The effect of periodically changing oxidizing and reducing conditions , 1993 .

[13]  Daizo Kunii,et al.  Catalytic reduction of nitric oxide by carbon monoxide over calcined limestone. , 1983 .

[14]  B. Koel,et al.  Transient kinetic studies of the catalytic reduction of NO by CO on platinum , 1989 .

[15]  K. Østergaard,et al.  High-temperature reaction between sulphur dioxide and limestone. II, An improved experimental basis for a mathematical model , 1991 .

[16]  J. Johnsson,et al.  Catalytic reduction of NO and N2O on limestone during sulfur capture under fluidized bed combustion conditions , 1992 .

[17]  P. Meubus Catalytic Decomposition of Nitric Oxide in the Presence of Alkaline Earth Oxides , 1977 .

[18]  Kim Dam-Johansen,et al.  Hydrogen Chloride Reaction with Lime and Limestone : Kinetics and Sorption Capacity , 1992 .

[19]  K. Østergaard,et al.  High-temperature reaction between sulphur dioxide and limestone—IV. A discussion of chemical reaction mechanisms and kinetics , 1991 .