The use of δ 13C in CO to determine removal of CH4 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 δ ¹³C in CO to determine removal of CH₄ 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

^*Corresponding author for this work

Max Planck Institute for Chemistry
Shandong University
Spanish National Research Council (CSIC)
State Meteorological Agency of Spain (AEMet)
Spanish Institute of Oceanography (IEO-CSIC)
Max Planck Institute for Biogeochemistry
Instituto Nacional de Metereologia e Geofisica Ilha do Sal
University of Bristol
NIWA
University of Copenhagen

Research output: Contribution to journal › Article › Academic › 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

Bibliographical note

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

Funding

This research is part of the ISAMO project funded by Spark Climate Solutions. The sampling at Tenerife was supported under the European Union\u2019s Horizon 2020 research and innovation programme through the ATMO-ACCESS Integrating Activity under Grant Agreement No 101008004.

Funders	Funder number
Horizon 2020 Framework Programme	101008004
Horizon 2020 Framework Programme

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 3 Good Health and Well-being
SDG 7 Affordable and Clean Energy

Keywords

CH
Cl
CO
δ C

Access to Document

10.1088/1748-9326/ad4375Licence: CC BY

Röckmann_2024_Environ._Res._Lett._19_064054Final published version, 1.19 MBLicence: CC BY

Cite this

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 δ ¹³C in CO to determine removal of CH₄ by Cl radicals in the atmosphere. Environmental Research Letters, 19(6), Article 064054. https://doi.org/10.1088/1748-9326/ad4375

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title = "The use of δ 13C in CO to determine removal of CH4 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.",

keywords = "CH, Cl, CO, δ C",

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",

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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 δ ¹³C in CO to determine removal of CH₄ by Cl radicals in the atmosphere', Environmental Research Letters, vol. 19, no. 6, 064054. https://doi.org/10.1088/1748-9326/ad4375

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T1 - The use of δ 13C in CO to determine removal of CH4 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.

KW - CH

KW - Cl

KW - CO

KW - δ C

UR - https://www.scopus.com/pages/publications/85195630984

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DO - 10.1088/1748-9326/ad4375

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SN - 1748-9326

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JO - Environmental Research Letters

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