Global inventory of doubly substituted isotopologues of methane (Δ13CH3D and Δ12CH2D2)
(2025) In Earth System Science Data 17(12). p.6889-6910- Abstract
Measurements of methane (CH4) molecules containing two rare isotopes (13CH3D and 12CH2D2), also termed doubly substituted or "clumped" isotopologues, have the potential to provide two additional isotopic dimensions to help investigate the mechanisms underlying global atmospheric trends in CH4. In this work, we summarise the current state of research on doubly substituted CH4 isotopologues, with an emphasis on compiling results of all relevant work. The database comprises 1475 records compiled from the literature published until April 2025 (10.5285/51ae627da5fb41b8a767ee6c653f83e6, Defratyka et al., 2025). For field samples, 40 % of records were... (More)
Measurements of methane (CH4) molecules containing two rare isotopes (13CH3D and 12CH2D2), also termed doubly substituted or "clumped" isotopologues, have the potential to provide two additional isotopic dimensions to help investigate the mechanisms underlying global atmospheric trends in CH4. In this work, we summarise the current state of research on doubly substituted CH4 isotopologues, with an emphasis on compiling results of all relevant work. The database comprises 1475 records compiled from the literature published until April 2025 (10.5285/51ae627da5fb41b8a767ee6c653f83e6, Defratyka et al., 2025). For field samples, 40 % of records were sourced from natural gas reservoirs, while microbial terrestrial (e.g., agriculture, lake, wetland) samples account only for 12.5 %. Lakes samples contribute 75 % to collected microbial terrestrial samples. There is limited or no representation of samples coming from significant microbial CH4 sources to the atmosphere, like wetlands, agricultural practices and landfills. To date, laboratory experiments were mostly focused on microbial (28 % of samples from laboratory experiments) and pyrogenic (15 %) methanogenesis or anaerobic (16 %), and aerobic (8 %) CH4 oxidation, with only single study of photochemical oxidation via OH and Cl, which constitutes 5 % of the laboratory experiments entries. The distinct ranges of Δ13CH3D and Δ12CH2D2 values measured in these studies suggests their potential to improve our understanding of atmospheric CH4. This work provides an overview of the major gaps in measurements and identifies where further studies should be focussed to enable the highest impact on understanding global CH4.
(Less)
- author
- Defratyka, Sara M.
; Fernandez, Julianne M.
; Adnew, Getachew A.
; Dong, Guannan
; Douglas, Peter M.J.
; Eldridge, Daniel L.
; Etiope, Giuseppe
; Giunta, Thomas
; Haghnegahdar, Mojhgan A.
; Hristov, Alexander N.
; Hultquist, Nicole
; Vadillo, Iñaki
; Jautzy, Josue
; Kim, Ji Hyun
; Labidi, Jabrane
; Lalk, Ellen
; Leavitt, Wil
; Li, Jiawen
; Lin, Li Hung
; Liu, Jiarui
; Ojeda, Lucía
; Ono, Shuhei
; Rhim, Jeemin H.
; Röckmann, Thomas
; Sherwood Lollar, Barbara
; Sivan, Malavika
; Sun, Jiayang
; Ventura, Gregory T.
; Wang, David T.
; Young, Edward D.
; Zhang, Naizhong
and Arnold, Tim
LU
(Less) - organization
- publishing date
- 2025-12-08
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Earth System Science Data
- volume
- 17
- issue
- 12
- pages
- 22 pages
- publisher
- Copernicus GmbH
- external identifiers
-
- scopus:105024310416
- ISSN
- 1866-3508
- DOI
- 10.5194/essd-17-6889-2025
- language
- English
- LU publication?
- yes
- additional info
- Publisher Copyright: © 2025 Sara M. Defratyka et al.
- id
- 1cfe4267-e43d-47eb-9857-aa61eebe38a7
- date added to LUP
- 2026-01-04 20:32:41
- date last changed
- 2026-01-08 08:45:25
@article{1cfe4267-e43d-47eb-9857-aa61eebe38a7,
abstract = {{<p>Measurements of methane (CH<sub>4</sub>) molecules containing two rare isotopes (<sup>13</sup>CH<sub>3</sub>D and <sup>12</sup>CH<sub>2</sub>D<sub>2</sub>), also termed doubly substituted or "clumped" isotopologues, have the potential to provide two additional isotopic dimensions to help investigate the mechanisms underlying global atmospheric trends in CH<sub>4</sub>. In this work, we summarise the current state of research on doubly substituted CH<sub>4</sub> isotopologues, with an emphasis on compiling results of all relevant work. The database comprises 1475 records compiled from the literature published until April 2025 (10.5285/51ae627da5fb41b8a767ee6c653f83e6, Defratyka et al., 2025). For field samples, 40 % of records were sourced from natural gas reservoirs, while microbial terrestrial (e.g., agriculture, lake, wetland) samples account only for 12.5 %. Lakes samples contribute 75 % to collected microbial terrestrial samples. There is limited or no representation of samples coming from significant microbial CH<sub>4</sub> sources to the atmosphere, like wetlands, agricultural practices and landfills. To date, laboratory experiments were mostly focused on microbial (28 % of samples from laboratory experiments) and pyrogenic (15 %) methanogenesis or anaerobic (16 %), and aerobic (8 %) CH<sub>4</sub> oxidation, with only single study of photochemical oxidation via OH and Cl, which constitutes 5 % of the laboratory experiments entries. The distinct ranges of Δ<sup>13</sup>CH<sub>3</sub>D and Δ<sup>12</sup>CH<sub>2</sub>D<sub>2</sub> values measured in these studies suggests their potential to improve our understanding of atmospheric CH<sub>4</sub>. This work provides an overview of the major gaps in measurements and identifies where further studies should be focussed to enable the highest impact on understanding global CH<sub>4</sub>.</p>}},
author = {{Defratyka, Sara M. and Fernandez, Julianne M. and Adnew, Getachew A. and Dong, Guannan and Douglas, Peter M.J. and Eldridge, Daniel L. and Etiope, Giuseppe and Giunta, Thomas and Haghnegahdar, Mojhgan A. and Hristov, Alexander N. and Hultquist, Nicole and Vadillo, Iñaki and Jautzy, Josue and Kim, Ji Hyun and Labidi, Jabrane and Lalk, Ellen and Leavitt, Wil and Li, Jiawen and Lin, Li Hung and Liu, Jiarui and Ojeda, Lucía and Ono, Shuhei and Rhim, Jeemin H. and Röckmann, Thomas and Sherwood Lollar, Barbara and Sivan, Malavika and Sun, Jiayang and Ventura, Gregory T. and Wang, David T. and Young, Edward D. and Zhang, Naizhong and Arnold, Tim}},
issn = {{1866-3508}},
language = {{eng}},
month = {{12}},
number = {{12}},
pages = {{6889--6910}},
publisher = {{Copernicus GmbH}},
series = {{Earth System Science Data}},
title = {{Global inventory of doubly substituted isotopologues of methane (Δ<sup>13</sup>CH<sub>3</sub>D and Δ<sup>12</sup>CH<sub>2</sub>D<sub>2</sub>)}},
url = {{http://dx.doi.org/10.5194/essd-17-6889-2025}},
doi = {{10.5194/essd-17-6889-2025}},
volume = {{17}},
year = {{2025}},
}