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1 Bulletin of the Polish Academy of Sciences. Chemistry

1 2001

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Laboratory studies of the reaction between nitrogen dioxide and ammonia in the temperature range of 288-357 K

Pagsberg P., Sillesen A., Brudnik K., Ratajczak E.

Bulletin of the Polish Academy of Sciences. Chemistry

2001

Vol. 49, No. 4

299-304

The title reaction has been studied by infrared tunable diode laser spec-troscopy which allows for the detection of both reactant and product molecules. The decay rate of ammonia in the presence of nitrogen dioxide was found to be second order with respect to the concentration of NO2- The simultaneous formation of water was found to occur with a relative yield of 4[H2O] = —0.5^[NH3]. The formation of aerosols containing crystalline ammonium nitrate implies that nitric acid is also a primary reaction product in the overall reaction 2NO2 + 2NHa —> N2 + H(2)O + NH(4)NOs. A reaction mechanism involving asym-N(2)O(4) reacting with NHa has been tested by detailed computer modelling which was used to account for all of the observed kinetic and mechanistic features. For the rate controlling step 2NO2 + M —> asym- N2C>4 + M (1) we have determined an apparent bimolecular rate constant of k\ — 2.30 x 10(-4) x exp(3838 =360/T)M(-1)s(-1) at a total pressure of 30 mbar.