4.6 Article

Kinetics of CH2OO reactions with SO2, NO2, NO, H2O and CH3CHO as a function of pressure

Journal

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 16, Issue 3, Pages 1139-1149

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cp54391a

Keywords

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Funding

  1. National Centre for Atmospheric Science (NCAS)
  2. Engineering and Physical Sciences Research Council (EPSRC) [EP/J010871/1]
  3. EPSRC [EP/J010871/1] Funding Source: UKRI
  4. NERC [ncas10006] Funding Source: UKRI
  5. Engineering and Physical Sciences Research Council [EP/J010871/1] Funding Source: researchfish
  6. Natural Environment Research Council [ncas10006, 1221209] Funding Source: researchfish

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Kinetics of CH2OO Criegee intermediate reactions with SO2, NO2, NO, H2O and CH3CHO and CH2I radical reactions with NO2 are reported as a function of pressure at 295 K. Measurements were made under pseudo-first-order conditions using flash photolysis of CH2I2-O-2-N-2 gas mixtures in the presence of excess co-reagent combined with monitoring of HCHO reaction products by laser-induced fluorescence (LIF) spectroscopy and, for the reaction with SO2, direct detection of CH2OO by photoionisation mass spectrometry (PIMS). Rate coefficients for CH2OO + SO2 and CH2OO + NO2 are independent of pressure in the ranges studied and are (3.42 +/- 0.42) x 10(-11) cm(3) s(-1) (measured between 1.5 and 450 Torr) and (1.5 +/- 0.5) x 10(-12) cm(3) s(-1) (measured between 25 and 300 Torr), respectively. The rate coefficient for CH2OO + CH3CHO is pressure dependent, with the yield of HCHO decreasing with increasing pressure. Upper limits of 2 x 10(-13) cm(3) s(-1) and 9 x 10(-17) cm(3) s(-1) are placed on the rate coefficients for CH2OO + NO and CH2OO + H2O, respectively. The upper limit for the rate coefficient for CH2OO + H2O is significantly lower than has been reported previously, with consequences for modelling of atmospheric impacts of CH2OO chemistry.

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