The use of δ13              C in CO to determine removal of CH              4              by Cl radicals in the atmosphere

Thomas Röckmann; Maarten Van herpen; Chloe Brashear; Carina van der Veen; Sergey Gromov; Qinyi Li; Alfonso Saiz-Lopez; Daphne Meidan; Africa Barreto; Natalia Prats; Ignacio Mármol; Ramón Ramos; Isabel Baños; Jesús m Arrieta; Sönke Zaehnle; Armin Jordan; Heiko Moossen; Helder Timas; Dickon Young; Peter Sperlich; Rowena Moss; Matthew S. Johnson

doi:10.1088/1748-9326/ad4375

The use of δ¹³ C in CO to determine removal of CH 4 by Cl radicals in the atmosphere

Thomas Röckmann^*, Maarten Van herpen, Chloe Brashear, Carina van der Veen, Sergey Gromov, Qinyi Li, Alfonso Saiz-Lopez, Daphne Meidan, Africa Barreto, Natalia Prats, Ignacio Mármol, Ramón Ramos, Isabel Baños, Jesús m Arrieta, Sönke Zaehnle, Armin Jordan, Heiko Moossen, Helder Timas, Dickon Young, Peter SperlichRowena Moss, Matthew S. Johnson

^*Corresponding author for this work

School of Chemistry

Research output: Contribution to journal › Article (Academic Journal) › peer-review

Abstract

The reaction of CH4 with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where 12CH4 reacts about 70 ‰ faster with Cl than 13CH4. Therefore, although the Cl-based sink of CH4 constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH4 source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH4 + Cl reaction in the atmosphere is the detection of the extremely 13C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH4 at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH4 removal from the atmosphere.

Original language	English
Article number	064054
Number of pages	9
Journal	Environmental Research Letters
Volume	19
Issue number	6
DOIs	https://doi.org/10.1088/1748-9326/ad4375
Publication status	Published - 1 Jun 2024

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© 2024 The Author(s). Published by IOP Publishing Ltd

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Röckmann, T., Van herpen, M., Brashear, C., van der Veen, C., Gromov, S., Li, Q., Saiz-Lopez, A., Meidan, D., Barreto, A., Prats, N., Mármol, I., Ramos, R., Baños, I., Arrieta, J. M., Zaehnle, S., Jordan, A., Moossen, H., Timas, H., Young, D., ... Johnson, M. S. (2024). The use of δ¹³ C in CO to determine removal of CH 4 by Cl radicals in the atmosphere . Environmental Research Letters, 19(6), Article 064054. https://doi.org/10.1088/1748-9326/ad4375

@article{7747a87c915d42da8246ff354c955991,

title = "The use of δ13 C in CO to determine removal of CH 4 by Cl radicals in the atmosphere ",

abstract = "The reaction of CH4 with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where 12CH4 reacts about 70 ‰ faster with Cl than 13CH4. Therefore, although the Cl-based sink of CH4 constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH4 source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH4 + Cl reaction in the atmosphere is the detection of the extremely 13C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH4 at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH4 removal from the atmosphere.",

author = "Thomas R{\"o}ckmann and {Van herpen}, Maarten and Chloe Brashear and {van der Veen}, Carina and Sergey Gromov and Qinyi Li and Alfonso Saiz-Lopez and Daphne Meidan and Africa Barreto and Natalia Prats and Ignacio M{\'a}rmol and Ram{\'o}n Ramos and Isabel Ba{\~n}os and Arrieta, {Jes{\'u}s m} and S{\"o}nke Zaehnle and Armin Jordan and Heiko Moossen and Helder Timas and Dickon Young and Peter Sperlich and Rowena Moss and Johnson, {Matthew S.}",

note = "Publisher Copyright: {\textcopyright} 2024 The Author(s). Published by IOP Publishing Ltd",

year = "2024",

month = jun,

day = "1",

doi = "10.1088/1748-9326/ad4375",

language = "English",

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Röckmann, T, Van herpen, M, Brashear, C, van der Veen, C, Gromov, S, Li, Q, Saiz-Lopez, A, Meidan, D, Barreto, A, Prats, N, Mármol, I, Ramos, R, Baños, I, Arrieta, JM, Zaehnle, S, Jordan, A, Moossen, H, Timas, H, Young, D, Sperlich, P, Moss, R & Johnson, MS 2024, 'The use of δ¹³ C in CO to determine removal of CH 4 by Cl radicals in the atmosphere ', Environmental Research Letters, vol. 19, no. 6, 064054. https://doi.org/10.1088/1748-9326/ad4375

TY - JOUR

T1 - The use of δ13 C in CO to determine removal of CH 4 by Cl radicals in the atmosphere

AU - Röckmann, Thomas

AU - Van herpen, Maarten

AU - Brashear, Chloe

AU - van der Veen, Carina

AU - Gromov, Sergey

AU - Li, Qinyi

AU - Saiz-Lopez, Alfonso

AU - Meidan, Daphne

AU - Barreto, Africa

AU - Prats, Natalia

AU - Mármol, Ignacio

AU - Ramos, Ramón

AU - Baños, Isabel

AU - Arrieta, Jesús m

AU - Zaehnle, Sönke

AU - Jordan, Armin

AU - Moossen, Heiko

AU - Timas, Helder

AU - Young, Dickon

AU - Sperlich, Peter

AU - Moss, Rowena

AU - Johnson, Matthew S.

PY - 2024/6/1

Y1 - 2024/6/1

N2 - The reaction of CH4 with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where 12CH4 reacts about 70 ‰ faster with Cl than 13CH4. Therefore, although the Cl-based sink of CH4 constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH4 source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH4 + Cl reaction in the atmosphere is the detection of the extremely 13C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH4 at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH4 removal from the atmosphere.

AB - The reaction of CH4 with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where 12CH4 reacts about 70 ‰ faster with Cl than 13CH4. Therefore, although the Cl-based sink of CH4 constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH4 source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH4 + Cl reaction in the atmosphere is the detection of the extremely 13C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH4 at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH4 removal from the atmosphere.

U2 - 10.1088/1748-9326/ad4375

DO - 10.1088/1748-9326/ad4375

M3 - Article (Academic Journal)

SN - 1748-9326

VL - 19

JO - Environmental Research Letters

JF - Environmental Research Letters

IS - 6

M1 - 064054

ER -

The use of δ13 C in CO to determine removal of CH 4 by Cl radicals in the atmosphere