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Issue 3, 2014
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Kinetics of CH2OO reactions with SO2, NO2, NO, H2O and CH3CHO as a function of pressure

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Abstract

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–O2–N2 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) × 10−11 cm3 s−1 (measured between 1.5 and 450 Torr) and (1.5 ± 0.5) × 10−12 cm3 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 × 10−13 cm3 s−1 and 9 × 10−17 cm3 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.

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

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Supplementary files

Article information


Submitted
16 Oct 2013
Accepted
19 Nov 2013
First published
20 Nov 2013

This article is Open Access

Phys. Chem. Chem. Phys., 2014,16, 1139-1149
Article type
Paper

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

D. Stone, M. Blitz, L. Daubney, N. U. M. Howes and P. Seakins, Phys. Chem. Chem. Phys., 2014, 16, 1139
DOI: 10.1039/C3CP54391A

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