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Thermal decomposition of alkyl peroxynitrates

Journal Article · · Journal of Physical Chemistry; (USA)
DOI:https://doi.org/10.1021/j100351a036· OSTI ID:6972109
; ; ;  [1]
  1. Bergische Universitaet Gesamthochschule Wuppertal (Germany, F.R.)

The thermal decomposition of methyl peroxynitrate and ethyl peroxynitrate was studied in a temperature-controlled 420 L glass chamber at temperatures between -28 and 0{degree}C and total pressures from 10 to 800 mbar (M = N{sub 2}). The reactions proceed via OO-N bond fission. The unmolecular decay of the peroxynitrates was followed in situ by long-path IR absorption using a Fourier transform spectrometer. In Troe's notation, the data are represented by the following limiting low- and high-pressure first-order rate constants k{sub 0} and k{sub {infinity}} and the falloff curvature parameters F{sub c}: for R = CH{sub 3}, k{sub 0}/(N{sub 2}) = 9.0 {times} 10{sup {minus}5} exp(-80.6 kJ mol{sup {minus}1}/RT) cm{sup 3} molecule{sup {minus}1} s{sup {minus}1}, k{sub {infinity}} = 1.1 {times} 10{sup 16} exp(-87.8 kJ mol{sup {minus}1}/RT) s{sup {minus}1}, F{sub c} = 0.4; for R = C{sub 2}H{sub 5}, k{sub 0}/(N{sub 2}) = 4.8 {times} 10{sup {minus}4} exp(-77.2 kJ mol{sup {minus}1}/RT) cm{sup 3} molecule{sup {minus}1} s{sup {minus}1}, k{sub {infinity}} = 8.8 {times} 10{sup 15} exp(-86.8 kJ mol{sup {minus}1}/RT) s{sup {minus}1}, F{sub c} = 0.3. Combining the present results for R = CH{sub 3} with literature data on the corresponding recombination reaction, K{sub c} = 1.94 {times} 10{sup 27} exp(-10766 K/T) molecule cm{sup {minus}3} s obtained for the equilibrium CH{sub 3}OONO{sub 2} {l equilibrium} CH{sub 3}OO + NO{sub 2}. Some experiments were performed on the thermal decomposition of isomeric mixtures of butyl, hexyl, and octyl peroxynitrate at 253 K and in 800 mbar of N{sub 2}. Atmospheric implications of the thermal stability of alkyl peroxynitrates are briefly discussed.

OSTI ID:
6972109
Journal Information:
Journal of Physical Chemistry; (USA), Journal Name: Journal of Physical Chemistry; (USA) Vol. 93:14; ISSN 0022-3654; ISSN JPCHA
Country of Publication:
United States
Language:
English