Role of excited CF3CFHO radicals in the atmospheric chemistry of HFC-134a
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Role of excited CF3CFHO radicals in the atmospheric chemistry of HFC-134a. / Wallington, T. J.; Hurley, M. D.; Fracheboud, J. M.; Orlando, J. J.; Tyndall, G. S.; Sehested, J.; Møgelberg, T. E.; Nielsen, O. J.
I: Journal of Physical Chemistry, Bind 100, Nr. 46, 14.11.1996, s. 18116-18122.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Role of excited CF3CFHO radicals in the atmospheric chemistry of HFC-134a
AU - Wallington, T. J.
AU - Hurley, M. D.
AU - Fracheboud, J. M.
AU - Orlando, J. J.
AU - Tyndall, G. S.
AU - Sehested, J.
AU - Møgelberg, T. E.
AU - Nielsen, O. J.
PY - 1996/11/14
Y1 - 1996/11/14
N2 - The atmospheric degradation of HFC-134a (CF3CFH2) proceeds via the formation of CF3CFHO radicals. Long path length FTIR environmental chamber techniques were used to study the atmospheric fate of CF3-CFHO radicals. Two competing reaction pathways were identified for CF3CFHO radicals: reaction with O2, CF3CFHO + O2 → CF3C(O)F + HO2, and decomposition via C-C bond scission, CF3CFHO + M → CF3 + HC(O)F + M. CF3CFHO radicals were produced by two different reactions: either via the self-reaction of CF3CFHO2 radicals or via the CF3CFHO2 + NO reaction. It was found that decomposition was much more important when CF3CFHO radicals were produced via the CF3CFHO2 + NO reaction than when they were produced via the self-reaction of CF3CFHO2 radicals. We ascribe this observation to the formation of vibrationally excited CF3CFHO* radicals in the CF3CFHO2 + NO reaction. Rapid decomposition of CF3-CFHO* radicals limits the formation of CF3C(O)F and hence CF3COOH in the atmospheric degradation of HFC-134a. We estimate that the CF3COOH yield from atmospheric oxidation of HFC-134a is 7-20%. Vibrationally excited alkoxy radicals may play an important role in the atmospheric chemistry of other organic compounds.
AB - The atmospheric degradation of HFC-134a (CF3CFH2) proceeds via the formation of CF3CFHO radicals. Long path length FTIR environmental chamber techniques were used to study the atmospheric fate of CF3-CFHO radicals. Two competing reaction pathways were identified for CF3CFHO radicals: reaction with O2, CF3CFHO + O2 → CF3C(O)F + HO2, and decomposition via C-C bond scission, CF3CFHO + M → CF3 + HC(O)F + M. CF3CFHO radicals were produced by two different reactions: either via the self-reaction of CF3CFHO2 radicals or via the CF3CFHO2 + NO reaction. It was found that decomposition was much more important when CF3CFHO radicals were produced via the CF3CFHO2 + NO reaction than when they were produced via the self-reaction of CF3CFHO2 radicals. We ascribe this observation to the formation of vibrationally excited CF3CFHO* radicals in the CF3CFHO2 + NO reaction. Rapid decomposition of CF3-CFHO* radicals limits the formation of CF3C(O)F and hence CF3COOH in the atmospheric degradation of HFC-134a. We estimate that the CF3COOH yield from atmospheric oxidation of HFC-134a is 7-20%. Vibrationally excited alkoxy radicals may play an important role in the atmospheric chemistry of other organic compounds.
UR - http://www.scopus.com/inward/record.url?scp=33748481542&partnerID=8YFLogxK
M3 - Journal article
AN - SCOPUS:33748481542
VL - 100
SP - 18116
EP - 18122
JO - Journal of Physical Chemistry
JF - Journal of Physical Chemistry
SN - 0022-3654
IS - 46
ER -
ID: 227487145