Mechanism of chlorine catalytic oxidation of CO in the gas phase.
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The mechanism of the title reaction is determined under steady state conditions by the irradiation of the mixtures of Cl<SUB>2</SUB>, CO, O<SUB>2</SUB>, and N<SUB>2</SUB> at 300 K with black blue fluorescence lamps using infrared spectroscopy. The pressure dependence of the ratio of the formation rate of carbon dioxide to that of phosgene (COCl<SUB>2</SUB>) and the other results indicated that the oxidation of CO proceeded <I>via</I> intermediates ClCO and ClC(O)O<SUB>2</SUB> as the termolecular process rather than the bimolecular oxidation by ClOO and/or ClO. The ratio of the competitive reactions of chloroformyl radicals, <I>k</I><SUB>8</SUB>⁄<I>k</I><SUB>9a</SUB>, was found to be (6.5±0.4)×10<SUP>−2</SUP> in the total pressure range from 30 to 755 Torr (1 Torr=133 Pa); ClCO+Cl<SUB>2</SUB>→COCl<SUB>2</SUB>+Cl (8), ClCO+O<SUB>2</SUB>→ClC(O)O<SUB>2</SUB><SUP>*</SUP> (9a). And also, the ratio of the competitive reactions of the vibrationally excited intermediates, <I>k</I><SUB>9b</SUB>⁄<I>k</I><SUB>9c</SUB>, was (3.4±0.3)×10<SUP>18</SUP> molecule/cm<SUP>3</SUP>; ClC(O)O<SUB>2</SUB><SUP>*</SUP>→ClCO+O<SUB>2</SUB> (9b), ClC(O)O<SUB>2</SUB><SUP>*</SUP>+M→ClC(O)O<SUB>2</SUB>+M (9c). The role of this reaction in the stratosphere is discussed and estimated to be unimportant.
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