Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23

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Standard

Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23. / Sulbaek Andersen, Mads Peter; Madronich, Sasha; Ohide, Joanna May; Frausig, Morten; Nielsen, Ole John.

I: Atmospheric Environment, Bind 314, 120087, 2023.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt

Harvard

Sulbaek Andersen, MP, Madronich, S, Ohide, JM, Frausig, M & Nielsen, OJ 2023, 'Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23', Atmospheric Environment, bind 314, 120087. https://doi.org/10.1016/j.atmosenv.2023.120087

APA

Sulbaek Andersen, M. P., Madronich, S., Ohide, J. M., Frausig, M., & Nielsen, O. J. (2023). Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23. Atmospheric Environment, 314, [120087]. https://doi.org/10.1016/j.atmosenv.2023.120087

Vancouver

Sulbaek Andersen MP, Madronich S, Ohide JM, Frausig M, Nielsen OJ. Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23. Atmospheric Environment. 2023;314. 120087. https://doi.org/10.1016/j.atmosenv.2023.120087

Author

Sulbaek Andersen, Mads Peter ; Madronich, Sasha ; Ohide, Joanna May ; Frausig, Morten ; Nielsen, Ole John. / Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23. I: Atmospheric Environment. 2023 ; Bind 314.

Bibtex

@article{dbec94bd3de9426f8c0f5fda3fc93bc0,
title = "Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23",
abstract = "In this work, the 254 nm photolysis of CF3CHO was investigated using a 101 L quartz chamber coupled with FTIR detection. The overall quantum yield was determined as (0.52 ± 0.07) at 700 Torr, independent of diluent gas. Photolysis in 700 Torr N2 and in the presence of NO yields (26 ± 3) % CF3H and (73 ± 6) % CF3NO. In 700 Torr of air or oxygen, products identified include CF3H, COF2, CF3OH, CF3O2CF3 and CF3O3CF3. In the presence of NO in 700 Torr of air or O2, alkoxy- and peroxy-nitrates were also quantified. A full carbon balance for the fluorine-bearing carbon was achieved. The photolytic channel quantum yields were established: Φ(CF3H + CO) = (0.16 ± 0.02) and Φ(CF3 + HCO) = (0.36 ± 0.07) at 700 Torr total pressure. This is the first large chamber study of the stratospheric photolysis of CF3CHO. The quantum yields measured here are lower than those reported previously and show a different relative importance associated with the photolysis channels. Atmospheric photolysis coefficients of CF3CHO were modeled giving an estimate for the average atmospheric lifetime for CF3CHO of 13 ± 4 days (at 5 km altitude, tropics). Based on the present work, photolytic production of CF3H, which is a strong greenhouse gas, can occur at stratospheric altitudes above 30–40 km. This has implications for the environmental impact of CF3CHO generated as an oxidation product in the higher atmosphere from long-lived chlorofluorocarbon-replacement compounds. However, the majority of CF3CHO will undergo photochemical degradation in the lower troposphere. Hence, photochemical degradation of CF3CHO will make a negligible contribution to the atmospheric burden of CF3H.",
keywords = "Atmospheric chemistry, Climate, HFC-23, Lifetimes, Quantum yield, Stratosphere",
author = "{Sulbaek Andersen}, {Mads Peter} and Sasha Madronich and Ohide, {Joanna May} and Morten Frausig and Nielsen, {Ole John}",
note = "Publisher Copyright: {\textcopyright} 2023",
year = "2023",
doi = "10.1016/j.atmosenv.2023.120087",
language = "English",
volume = "314",
journal = "Atmospheric Environment",
issn = "1352-2310",
publisher = "Pergamon Press",

}

RIS

TY - JOUR

T1 - Photolysis of CF3CHO at 254 nm and potential contribution to the atmospheric abundance of HFC-23

AU - Sulbaek Andersen, Mads Peter

AU - Madronich, Sasha

AU - Ohide, Joanna May

AU - Frausig, Morten

AU - Nielsen, Ole John

N1 - Publisher Copyright: © 2023

PY - 2023

Y1 - 2023

N2 - In this work, the 254 nm photolysis of CF3CHO was investigated using a 101 L quartz chamber coupled with FTIR detection. The overall quantum yield was determined as (0.52 ± 0.07) at 700 Torr, independent of diluent gas. Photolysis in 700 Torr N2 and in the presence of NO yields (26 ± 3) % CF3H and (73 ± 6) % CF3NO. In 700 Torr of air or oxygen, products identified include CF3H, COF2, CF3OH, CF3O2CF3 and CF3O3CF3. In the presence of NO in 700 Torr of air or O2, alkoxy- and peroxy-nitrates were also quantified. A full carbon balance for the fluorine-bearing carbon was achieved. The photolytic channel quantum yields were established: Φ(CF3H + CO) = (0.16 ± 0.02) and Φ(CF3 + HCO) = (0.36 ± 0.07) at 700 Torr total pressure. This is the first large chamber study of the stratospheric photolysis of CF3CHO. The quantum yields measured here are lower than those reported previously and show a different relative importance associated with the photolysis channels. Atmospheric photolysis coefficients of CF3CHO were modeled giving an estimate for the average atmospheric lifetime for CF3CHO of 13 ± 4 days (at 5 km altitude, tropics). Based on the present work, photolytic production of CF3H, which is a strong greenhouse gas, can occur at stratospheric altitudes above 30–40 km. This has implications for the environmental impact of CF3CHO generated as an oxidation product in the higher atmosphere from long-lived chlorofluorocarbon-replacement compounds. However, the majority of CF3CHO will undergo photochemical degradation in the lower troposphere. Hence, photochemical degradation of CF3CHO will make a negligible contribution to the atmospheric burden of CF3H.

AB - In this work, the 254 nm photolysis of CF3CHO was investigated using a 101 L quartz chamber coupled with FTIR detection. The overall quantum yield was determined as (0.52 ± 0.07) at 700 Torr, independent of diluent gas. Photolysis in 700 Torr N2 and in the presence of NO yields (26 ± 3) % CF3H and (73 ± 6) % CF3NO. In 700 Torr of air or oxygen, products identified include CF3H, COF2, CF3OH, CF3O2CF3 and CF3O3CF3. In the presence of NO in 700 Torr of air or O2, alkoxy- and peroxy-nitrates were also quantified. A full carbon balance for the fluorine-bearing carbon was achieved. The photolytic channel quantum yields were established: Φ(CF3H + CO) = (0.16 ± 0.02) and Φ(CF3 + HCO) = (0.36 ± 0.07) at 700 Torr total pressure. This is the first large chamber study of the stratospheric photolysis of CF3CHO. The quantum yields measured here are lower than those reported previously and show a different relative importance associated with the photolysis channels. Atmospheric photolysis coefficients of CF3CHO were modeled giving an estimate for the average atmospheric lifetime for CF3CHO of 13 ± 4 days (at 5 km altitude, tropics). Based on the present work, photolytic production of CF3H, which is a strong greenhouse gas, can occur at stratospheric altitudes above 30–40 km. This has implications for the environmental impact of CF3CHO generated as an oxidation product in the higher atmosphere from long-lived chlorofluorocarbon-replacement compounds. However, the majority of CF3CHO will undergo photochemical degradation in the lower troposphere. Hence, photochemical degradation of CF3CHO will make a negligible contribution to the atmospheric burden of CF3H.

KW - Atmospheric chemistry

KW - Climate

KW - HFC-23

KW - Lifetimes

KW - Quantum yield

KW - Stratosphere

U2 - 10.1016/j.atmosenv.2023.120087

DO - 10.1016/j.atmosenv.2023.120087

M3 - Journal article

AN - SCOPUS:85172082711

VL - 314

JO - Atmospheric Environment

JF - Atmospheric Environment

SN - 1352-2310

M1 - 120087

ER -

ID: 368805564