Stable isotopic signatures of methane from waste sources through atmospheric measurements

Semra Bakkaloglu; Dave Lowry; Rebecca E. Fisher; Malika Menoud; Mathias Lanoisellé; Huilin Chen; Thomas Röckmann; Euan G. Nisbet

doi:10.1016/j.atmosenv.2022.119021

Stable isotopic signatures of methane from waste sources through atmospheric measurements

Semra Bakkaloglu^*, Dave Lowry, Rebecca E. Fisher, Malika Menoud, Mathias Lanoisellé, Huilin Chen, Thomas Röckmann, Euan G. Nisbet

^*Corresponding author for this work

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

Abstract

This study aimed to characterize the carbon isotopic signatures (δ¹³C-CH₄) of several methane waste sources, predominantly in the UK, and during field campaigns in the Netherlands and Turkey. CH₄ plumes emitted from waste sources were detected during mobile surveys using a cavity ring-down spectroscopy (CRDS) analyser. Air samples were collected in the plumes for subsequent isotope analysis by gas chromatography isotope ratio mass spectrometry (GC-IRMS) to characterize δ¹³C-CH₄. The isotopic signatures were determined through a Keeling plot approach and the bivariate correlated errors and intrinsic scatter (BCES) fitting method. The δ¹³C-CH₄ and δ²H-CH₄ signatures were identified from biogas plants (−54.6 ± 5.6‰, n = 34; −314.4 ± 23‰ n = 3), landfills (−56.8 ± 2.3‰, n = 43; −268.2 ± 2.1‰, n = 2), sewage treatment plants (−51.6 ± 2.2‰, n = 15; −303.9 ± 22‰, n = 6), composting facilities (−54.7 ± 3.9‰, n = 6), a landfill leachate treatment plant (−57.1 ± 1.8‰, n = 2), one water treatment plant (−53.7 ± 0.1‰) and a waste recycling facility (−53.2 ± 0.2‰). The overall signature of 71 waste sources ranged from −64.4 to −44.3‰, with an average of −55.1 ± 4.1‰ (n = 102) for δ¹³C, −341 to −267‰, with an average of −300.3 ± 25‰ (n = 11) for δ²H, which can be distinguished from other source types in the UK such as gas leaks and ruminants. The study also demonstrates that δ²H-CH₄ signatures, in addition to δ¹³C-CH₄, can aid in better waste source apportionment and increase the granularity of isotope data required to improve regional modelling.

Original language	English
Article number	119021
Pages (from-to)	1-11
Number of pages	11
Journal	Atmospheric Environment
Volume	276
DOIs	https://doi.org/10.1016/j.atmosenv.2022.119021
Publication status	Published - 1 May 2022

Bibliographical note

Funding Information:
This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO 2 ) project, part of the European Union’s Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479 . We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE /N 016238/1 The Global Methane Budget 2016–2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO 2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study.

Funding Information:
This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO2) project, part of the European Union's Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479. We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE/N016238/1 The Global Methane Budget 2016?2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study.

Publisher Copyright:
© 2022 The Authors

Funding

This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO 2 ) project, part of the European Union’s Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479 . We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE /N 016238/1 The Global Methane Budget 2016–2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO 2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study. This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO2) project, part of the European Union's Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479. We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE/N016238/1 The Global Methane Budget 2016?2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study.

Keywords

Carbon isotopes
Deuterium
Greenhouse gas emissions
Methane emissions
Waste isotopic signature

UN SDGs

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

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Cite this

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title = "Stable isotopic signatures of methane from waste sources through atmospheric measurements",

abstract = "This study aimed to characterize the carbon isotopic signatures (δ13C-CH4) of several methane waste sources, predominantly in the UK, and during field campaigns in the Netherlands and Turkey. CH4 plumes emitted from waste sources were detected during mobile surveys using a cavity ring-down spectroscopy (CRDS) analyser. Air samples were collected in the plumes for subsequent isotope analysis by gas chromatography isotope ratio mass spectrometry (GC-IRMS) to characterize δ13C-CH4. The isotopic signatures were determined through a Keeling plot approach and the bivariate correlated errors and intrinsic scatter (BCES) fitting method. The δ13C-CH4 and δ2H-CH4 signatures were identified from biogas plants (−54.6 ± 5.6‰, n = 34; −314.4 ± 23‰ n = 3), landfills (−56.8 ± 2.3‰, n = 43; −268.2 ± 2.1‰, n = 2), sewage treatment plants (−51.6 ± 2.2‰, n = 15; −303.9 ± 22‰, n = 6), composting facilities (−54.7 ± 3.9‰, n = 6), a landfill leachate treatment plant (−57.1 ± 1.8‰, n = 2), one water treatment plant (−53.7 ± 0.1‰) and a waste recycling facility (−53.2 ± 0.2‰). The overall signature of 71 waste sources ranged from −64.4 to −44.3‰, with an average of −55.1 ± 4.1‰ (n = 102) for δ13C, −341 to −267‰, with an average of −300.3 ± 25‰ (n = 11) for δ2H, which can be distinguished from other source types in the UK such as gas leaks and ruminants. The study also demonstrates that δ2H-CH4 signatures, in addition to δ13C-CH4, can aid in better waste source apportionment and increase the granularity of isotope data required to improve regional modelling.",

keywords = "Carbon isotopes, Deuterium, Greenhouse gas emissions, Methane emissions, Waste isotopic signature",

author = "Semra Bakkaloglu and Dave Lowry and Fisher, {Rebecca E.} and Malika Menoud and Mathias Lanoisell{\'e} and Huilin Chen and Thomas R{\"o}ckmann and Nisbet, {Euan G.}",

note = "Funding Information: This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO 2 ) project, part of the European Union{\textquoteright}s Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479 . We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE /N 016238/1 The Global Methane Budget 2016–2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO 2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study. Funding Information: This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO2) project, part of the European Union's Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479. We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE/N016238/1 The Global Methane Budget 2016?2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study. Publisher Copyright: {\textcopyright} 2022 The Authors",

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AU - Bakkaloglu, Semra

AU - Lowry, Dave

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AU - Menoud, Malika

AU - Lanoisellé, Mathias

AU - Chen, Huilin

AU - Röckmann, Thomas

AU - Nisbet, Euan G.

N1 - Funding Information: This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO 2 ) project, part of the European Union’s Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479 . We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE /N 016238/1 The Global Methane Budget 2016–2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO 2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study. Funding Information: This work was supported by the MEthane goes MObile: MEasurement and MOdeling (MEMO2) project, part of the European Union's Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant agreement No. 722479. We would like to thank the UK Natural Environment Research Council (NERC) for current grants: NE/P019641/1 New Methodologies for Removal of Methane and NE/N016238/1 The Global Methane Budget 2016?2021. We thank Jerry Morris for maintaining the survey vehicle, and James France for help with driving the vehicle for the surveys. Special thanks go to Mila Stanisavljevic, Sara Defratyka, Piotr Korben and Julianne Fernandez for sharing their MEMO2 data, and colleagues in the Greenhouse Gas Research Group for supporting this study. Publisher Copyright: © 2022 The Authors

PY - 2022/5/1

Y1 - 2022/5/1

N2 - This study aimed to characterize the carbon isotopic signatures (δ13C-CH4) of several methane waste sources, predominantly in the UK, and during field campaigns in the Netherlands and Turkey. CH4 plumes emitted from waste sources were detected during mobile surveys using a cavity ring-down spectroscopy (CRDS) analyser. Air samples were collected in the plumes for subsequent isotope analysis by gas chromatography isotope ratio mass spectrometry (GC-IRMS) to characterize δ13C-CH4. The isotopic signatures were determined through a Keeling plot approach and the bivariate correlated errors and intrinsic scatter (BCES) fitting method. The δ13C-CH4 and δ2H-CH4 signatures were identified from biogas plants (−54.6 ± 5.6‰, n = 34; −314.4 ± 23‰ n = 3), landfills (−56.8 ± 2.3‰, n = 43; −268.2 ± 2.1‰, n = 2), sewage treatment plants (−51.6 ± 2.2‰, n = 15; −303.9 ± 22‰, n = 6), composting facilities (−54.7 ± 3.9‰, n = 6), a landfill leachate treatment plant (−57.1 ± 1.8‰, n = 2), one water treatment plant (−53.7 ± 0.1‰) and a waste recycling facility (−53.2 ± 0.2‰). The overall signature of 71 waste sources ranged from −64.4 to −44.3‰, with an average of −55.1 ± 4.1‰ (n = 102) for δ13C, −341 to −267‰, with an average of −300.3 ± 25‰ (n = 11) for δ2H, which can be distinguished from other source types in the UK such as gas leaks and ruminants. The study also demonstrates that δ2H-CH4 signatures, in addition to δ13C-CH4, can aid in better waste source apportionment and increase the granularity of isotope data required to improve regional modelling.

AB - This study aimed to characterize the carbon isotopic signatures (δ13C-CH4) of several methane waste sources, predominantly in the UK, and during field campaigns in the Netherlands and Turkey. CH4 plumes emitted from waste sources were detected during mobile surveys using a cavity ring-down spectroscopy (CRDS) analyser. Air samples were collected in the plumes for subsequent isotope analysis by gas chromatography isotope ratio mass spectrometry (GC-IRMS) to characterize δ13C-CH4. The isotopic signatures were determined through a Keeling plot approach and the bivariate correlated errors and intrinsic scatter (BCES) fitting method. The δ13C-CH4 and δ2H-CH4 signatures were identified from biogas plants (−54.6 ± 5.6‰, n = 34; −314.4 ± 23‰ n = 3), landfills (−56.8 ± 2.3‰, n = 43; −268.2 ± 2.1‰, n = 2), sewage treatment plants (−51.6 ± 2.2‰, n = 15; −303.9 ± 22‰, n = 6), composting facilities (−54.7 ± 3.9‰, n = 6), a landfill leachate treatment plant (−57.1 ± 1.8‰, n = 2), one water treatment plant (−53.7 ± 0.1‰) and a waste recycling facility (−53.2 ± 0.2‰). The overall signature of 71 waste sources ranged from −64.4 to −44.3‰, with an average of −55.1 ± 4.1‰ (n = 102) for δ13C, −341 to −267‰, with an average of −300.3 ± 25‰ (n = 11) for δ2H, which can be distinguished from other source types in the UK such as gas leaks and ruminants. The study also demonstrates that δ2H-CH4 signatures, in addition to δ13C-CH4, can aid in better waste source apportionment and increase the granularity of isotope data required to improve regional modelling.

KW - Carbon isotopes

KW - Deuterium

KW - Greenhouse gas emissions

KW - Methane emissions

KW - Waste isotopic signature

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U2 - 10.1016/j.atmosenv.2022.119021

DO - 10.1016/j.atmosenv.2022.119021

M3 - Article

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SN - 1352-2310

VL - 276

SP - 1

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JO - Atmospheric Environment

JF - Atmospheric Environment

M1 - 119021

ER -

Stable isotopic signatures of methane from waste sources through atmospheric measurements

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

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