Atmospheric Chemistry of (CF3)2CF-C≡N: A Replacement Compound for the Most Potent Industrial Greenhouse Gas, SF6

Mads Peter Sulbæk Andersen; Mildrid Kyte; Simone  Thirstrup Andersen; Claus J. Nielsen; Ole John Nielsen

doi:10.1021/acs.est.6b03758

Atmospheric Chemistry of (CF₃)₂CF-C≡N: A Replacement Compound for the Most Potent Industrial Greenhouse Gas, SF₆

Mads Peter Sulbæk Andersen, Mildrid Kyte, Simone Thirstrup Andersen, Claus J. Nielsen, Ole John Nielsen

Kemisk Institut

69 Citationer (Scopus)

Abstract

FTIR/smog chamber experiments and ab initio quantum calculations were performed to investigate the atmospheric chemistry of (CF3)2CFCN, a proposed replacement compound for the industrially important sulfur hexafluoride, SF6. The present study determined k(Cl + (CF3)2CFCN) = (2.33 ± 0.87) × 10–17, k(OH + (CF3)2CFCN) = (1.45 ± 0.25) × 10–15, and k(O3 + (CF3)2CFCN) ≤ 6 × 10–24 cm3 molecule–1 s–1, respectively, in 700 Torr of N2 or air diluent at 296 ± 2 K. The main atmospheric sink for (CF3)2CFCN was determined to be reaction with OH radicals. Quantum chemistry calculations, supported by experimental evidence, shows that the (CF3)2CFCN + OH reaction proceeds via OH addition to −C(≡N), followed by O2 addition to −C(OH)═N·, internal H-shift, and OH regeneration. The sole atmospheric degradation products of (CF3)2CFCN appear to be NO, COF2, and CF3C(O)F. The atmospheric lifetime of (CF3)2CFCN is approximately 22 years. The integrated cross section (650–1500 cm–1) for (CF3)2CFCN is (2.22 ± 0.11) × 10–16 cm2 molecule–1 cm–1 which results in a radiative efficiency of 0.217 W m–2 ppb–1. The 100-year Global Warming Potential (GWP) for (CF3)2CFCN was calculated as 1490, a factor of 15 less than that of SF6.

Originalsprog	Engelsk
Tidsskrift	Environmental Science & Technology (Washington)
Vol/bind	51
Udgave nummer	3
Sider (fra-til)	1321-1329
Antal sider	9
ISSN	0013-936X
DOI	https://doi.org/10.1021/acs.est.6b03758
Status	Udgivet - 7 feb. 2017

Adgang til dokumentet

10.1021/acs.est.6b03758

Citationsformater

Atmospheric Chemistry of (CF₃)₂CF-C≡N : A Replacement Compound for the Most Potent Industrial Greenhouse Gas, SF₆. / Andersen, Mads Peter Sulbæk; Kyte, Mildrid; Thirstrup Andersen, Simone et al.

I: Environmental Science & Technology (Washington), Bind 51, Nr. 3, 07.02.2017, s. 1321-1329.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review

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title = "Atmospheric Chemistry of (CF3)2CF-C≡N: A Replacement Compound for the Most Potent Industrial Greenhouse Gas, SF6",

abstract = "FTIR/smog chamber experiments and ab initio quantum calculations were performed to investigate the atmospheric chemistry of (CF3)2CFCN, a proposed replacement compound for the industrially important sulfur hexafluoride, SF6. The present study determined k(Cl + (CF3)2CFCN) = (2.33 ± 0.87) × 10–17, k(OH + (CF3)2CFCN) = (1.45 ± 0.25) × 10–15, and k(O3 + (CF3)2CFCN) ≤ 6 × 10–24 cm3 molecule–1 s–1, respectively, in 700 Torr of N2 or air diluent at 296 ± 2 K. The main atmospheric sink for (CF3)2CFCN was determined to be reaction with OH radicals. Quantum chemistry calculations, supported by experimental evidence, shows that the (CF3)2CFCN + OH reaction proceeds via OH addition to −C(≡N), followed by O2 addition to −C(OH)═N·, internal H-shift, and OH regeneration. The sole atmospheric degradation products of (CF3)2CFCN appear to be NO, COF2, and CF3C(O)F. The atmospheric lifetime of (CF3)2CFCN is approximately 22 years. The integrated cross section (650–1500 cm–1) for (CF3)2CFCN is (2.22 ± 0.11) × 10–16 cm2 molecule–1 cm–1 which results in a radiative efficiency of 0.217 W m–2 ppb–1. The 100-year Global Warming Potential (GWP) for (CF3)2CFCN was calculated as 1490, a factor of 15 less than that of SF6.",

author = "Andersen, {Mads Peter Sulb{\ae}k} and Mildrid Kyte and {Thirstrup Andersen}, Simone and Nielsen, {Claus J.} and Nielsen, {Ole John}",

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doi = "10.1021/acs.est.6b03758",

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T1 - Atmospheric Chemistry of (CF3)2CF-C≡N

T2 - A Replacement Compound for the Most Potent Industrial Greenhouse Gas, SF6

AU - Andersen, Mads Peter Sulbæk

AU - Kyte, Mildrid

AU - Thirstrup Andersen, Simone

AU - Nielsen, Claus J.

AU - Nielsen, Ole John

PY - 2017/2/7

Y1 - 2017/2/7

N2 - FTIR/smog chamber experiments and ab initio quantum calculations were performed to investigate the atmospheric chemistry of (CF3)2CFCN, a proposed replacement compound for the industrially important sulfur hexafluoride, SF6. The present study determined k(Cl + (CF3)2CFCN) = (2.33 ± 0.87) × 10–17, k(OH + (CF3)2CFCN) = (1.45 ± 0.25) × 10–15, and k(O3 + (CF3)2CFCN) ≤ 6 × 10–24 cm3 molecule–1 s–1, respectively, in 700 Torr of N2 or air diluent at 296 ± 2 K. The main atmospheric sink for (CF3)2CFCN was determined to be reaction with OH radicals. Quantum chemistry calculations, supported by experimental evidence, shows that the (CF3)2CFCN + OH reaction proceeds via OH addition to −C(≡N), followed by O2 addition to −C(OH)═N·, internal H-shift, and OH regeneration. The sole atmospheric degradation products of (CF3)2CFCN appear to be NO, COF2, and CF3C(O)F. The atmospheric lifetime of (CF3)2CFCN is approximately 22 years. The integrated cross section (650–1500 cm–1) for (CF3)2CFCN is (2.22 ± 0.11) × 10–16 cm2 molecule–1 cm–1 which results in a radiative efficiency of 0.217 W m–2 ppb–1. The 100-year Global Warming Potential (GWP) for (CF3)2CFCN was calculated as 1490, a factor of 15 less than that of SF6.

AB - FTIR/smog chamber experiments and ab initio quantum calculations were performed to investigate the atmospheric chemistry of (CF3)2CFCN, a proposed replacement compound for the industrially important sulfur hexafluoride, SF6. The present study determined k(Cl + (CF3)2CFCN) = (2.33 ± 0.87) × 10–17, k(OH + (CF3)2CFCN) = (1.45 ± 0.25) × 10–15, and k(O3 + (CF3)2CFCN) ≤ 6 × 10–24 cm3 molecule–1 s–1, respectively, in 700 Torr of N2 or air diluent at 296 ± 2 K. The main atmospheric sink for (CF3)2CFCN was determined to be reaction with OH radicals. Quantum chemistry calculations, supported by experimental evidence, shows that the (CF3)2CFCN + OH reaction proceeds via OH addition to −C(≡N), followed by O2 addition to −C(OH)═N·, internal H-shift, and OH regeneration. The sole atmospheric degradation products of (CF3)2CFCN appear to be NO, COF2, and CF3C(O)F. The atmospheric lifetime of (CF3)2CFCN is approximately 22 years. The integrated cross section (650–1500 cm–1) for (CF3)2CFCN is (2.22 ± 0.11) × 10–16 cm2 molecule–1 cm–1 which results in a radiative efficiency of 0.217 W m–2 ppb–1. The 100-year Global Warming Potential (GWP) for (CF3)2CFCN was calculated as 1490, a factor of 15 less than that of SF6.

U2 - 10.1021/acs.est.6b03758

DO - 10.1021/acs.est.6b03758

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EP - 1329

JO - Environmental Science & Technology

JF - Environmental Science & Technology

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