Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Negligible atmospheric release of methane from decomposing hydrates in mid-latitude oceans

Abstract

Naturally occurring gas hydrates may contribute to a positive feedback for global warming because they sequester large amounts of the potent greenhouse gas methane in ice-like deposits that could be destabilized by increasing ocean/atmospheric temperatures. Most hydrates occur within marine sediments; gas liberated during the decomposition of seafloor hydrates or originating with other methane pools can feed methane emissions at cold seeps. Regardless of the origin of seep methane, all previous measurements of methane emitted from seeps have shown it to have a unique fossil radiocarbon signature, contrasting with other sources of marine methane. Here we present the concentration and natural radiocarbon content of methane dissolved in the water column from the seafloor to the sea surface at seep fields along the US Atlantic and Pacific margins. For shallower water columns, where the seafloor is not within the hydrate stability zone, we do document seep CH4 in some surface-water samples. However, measurements in deeper water columns along the US Atlantic margin reveal no evidence of seep CH4 reaching surface waters when the water-column depth is greater than 430 ± 90 m. Gas hydrates exist only at water depths greater than ~550 m in this region, suggesting that the source of methane escaping to the atmosphere is not from hydrate decomposition.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Summary of surface-water 14C–CH4 results.
Fig. 2: Vertical profiles of Δ14C–CH4.
Fig. 3: Vertical profiles of dissolved CH4 concentration.
Fig. 4: The distribution of the fraction of seep CH4 dissolved in waters as a function of altitude above the seafloor.
Fig. 5: Plot of 14C–CH4 dissolved in surface waters versus total water-column depth where the samples were collected.

Similar content being viewed by others

Data availability

All data in this manuscript are available to the scientific community through the BCO-DMO database56 and through other releases15,57. Source data are provided with this paper.

References

  1. Anthony, K. M., Anthony, P., Grosse, G. & Chanton, J. Geologic methane seeps along boundaries of Arctic permafrost thaw and melting glaciers. Nat. Geosci. 5, 419–426 (2012).

    Article  Google Scholar 

  2. Canadell, J. G. et al. in Climate Change 2021: The Physical Science Basis (eds Masson-Delmotte, V. et al.) Ch. 5 (Cambridge Univ. Press, 2021).

  3. Reeburgh, W. S. Oceanic methane biogeochemistry. Chem. Rev. 107, 486–513 (2007).

    Article  Google Scholar 

  4. Tarnocai, C. et al. Soil organic carbon pools in the northern circumpolar permafrost region. Glob. Biogeochem. Cycles https://doi.org/10.1029/2008gb003327 (2009).

  5. Ruppel, C. D. & Kessler, J. D. The interaction of climate change and methane hydrates. Rev. Geophys. 55, 126–168 (2017).

    Article  Google Scholar 

  6. Ruppel, C. D. Methane hydrates and contemporary climate change. Nat. Educ. Knowl. https://www.nature.com/scitable/knowledge/library/methane-hydrates-and-contemporary-climate-change-24314790/ (2011).

  7. Buffett, B. & Archer, D. Global inventory of methane clathrate: sensitivity to changes in the deep ocean. Earth Planet. Sci. Lett. 227, 185–199 (2004).

    Article  Google Scholar 

  8. Rehder, G., Leifer, I., Brewer, P. G., Friederich, G. & Peltzer, E. T. Controls on methane bubble dissolution inside and outside the hydrate stability field from open ocean field experiments and numerical modeling. Mar. Chem. 114, 19–30 (2009).

    Article  Google Scholar 

  9. Leonte, M. et al. Using carbon isotope fractionation to constrain the extent of methane dissolution into the water column surrounding a natural hydrocarbon gas seep in the northern Gulf of Mexico. Geochem. Geophys. Geosyst. 19, 4459–4475 (2018).

    Article  Google Scholar 

  10. Wang, B., Jun, I., Socolofsky, S. A., DiMarco, S. F. & Kessler, J. D. Dynamics of gas bubbles from a submarine hydrocarbon seep within the hydrate stability zone. Geophys. Res. Lett. https://doi.org/10.1029/2020gl089256 (2020).

  11. Fu, X., Waite, W. F. & Ruppel, C. D. Hydrate formation on marine seep bubbles and the implications for water column methane dissolution. J. Geophys. Res. Oceans 126, e2021JC017363 (2021).

    Article  Google Scholar 

  12. Leonte, M. et al. Rapid rates of aerobic methane oxidation at the feather edge of gas hydrate stability in the waters of Hudson Canyon, US Atlantic Margin. Geochim. Cosmochim. Acta 204, 375–387 (2017).

    Article  Google Scholar 

  13. Leonte, M., Ruppel, C. D., RuizAngulo, A. & Kessler, J. D. Surface methane concentrations along the Mid-Atlantic Bight driven by aerobic subsurface production rather than seafloor gas seeps. J. Geophys. Res. Oceans https://doi.org/10.1029/2019jc015989 (2020).

  14. Joung, D. et al. Radiocarbon in marine methane reveals patchy impact of seeps on surface waters. Geophys. Res. Lett. https://doi.org/10.1029/2020gl089516 (2020).

  15. Baldwin, W. E., Moore, E. M., Worley, C. R., Nichols, A. R. & Ruppel, C. D. Marine Geophysical Data Collected to Support Methane Seep Research Along the US Atlantic Continental Shelf Break and Upper Continental Slope Between the Baltimore and Keller Canyons (USGS, 2020); https://doi.org/10.5066/P9Y1MSTN

  16. Johnson, H. P., Miller, U. K., Salmi, M. S. & Solomon, E. A. Analysis of bubble plume distributions to evaluate methane hydrate decomposition on the continental slope. Geochem. Geophys. Geosyst. 16, 3825–3839 (2015).

    Article  Google Scholar 

  17. Seabrook, S., De Leo, F. C., Baumberger, T., Raineault, N. & Thurber, A. R. Heterogeneity of methane seep biomes in the Northeast Pacific. Deep Sea Res. 2 150, 195–209 (2018).

    Article  Google Scholar 

  18. Skarke, A., Ruppel, C., Kodis, M., Brothers, D. & Lobecker, E. Widespread methane leakage from the sea floor on the northern US Atlantic margin. Nat. Geosci. 7, 657–661 (2014).

    Article  Google Scholar 

  19. Torres, M. E. et al. Methane sources feeding cold seeps on the shelf and upper continental slope off central Oregon, USA. Geochem. Geophys. Geosyst. 10, Q11003 (2009).

    Article  Google Scholar 

  20. Grabowski, K. S. et al. Carbon pool analysis of methane hydrate regions in the seafloor by accelerator mass spectrometry. Nucl. Instrum. Methods Phys. Res. B 223–224, 435–440 (2004).

    Article  Google Scholar 

  21. Kessler, J. D., Reeburgh, W. S., Southon, J. & Varela, R. Fossil methane source dominates Cariaco Basin water column methane geochemistry. Geophys. Res. Lett. https://doi.org/10.1029/2005gl022984 (2005).

  22. Kessler, J. D. et al. A survey of methane isotope abundance (14C, 13C, 2H) from five nearshore marine basins that reveals unusual radiocarbon levels in subsurface waters. J. Geophys. Res. Oceans https://doi.org/10.1029/2008jc004822 (2008).

  23. Pohlman, J. W. et al. Methane sources in gas hydrate-bearing cold seeps: evidence from radiocarbon and stable isotopes. Mar. Chem. 115, 102–109 (2009).

    Article  Google Scholar 

  24. Sparrow, K. J. et al. Limited contribution of ancient methane to surface waters of the US Beaufort Sea shelf. Sci. Adv. 4, eaao4842–eaao4842 (2018).

    Article  Google Scholar 

  25. Winckler, G. et al. Noble gases and radiocarbon in natural gas hydrates. Geophys. Res. Lett. https://doi.org/10.1029/2001GL014013 (2002).

  26. Karl, D. M. et al. Aerobic production of methane in the sea. Nat. Geosci. 1, 473–478 (2008).

    Article  Google Scholar 

  27. Repeta, D. J. et al. Marine methane paradox explained by bacterial degradation of dissolved organic matter. Nat. Geosci. 9, 884–887 (2016).

    Article  Google Scholar 

  28. Garcia‐Tigreros, F. et al. Estimating the impact of seep methane oxidation on ocean pH and dissolved inorganic radiocarbon along the US mid‐Atlantic Bight. J. Geophys. Res. Biogeosci. 126, e2019JG005621 (2021).

    Article  Google Scholar 

  29. Joung, D., Leonte, M. & Kessler, J. D. Methane sources in the waters of Lake Michigan and Lake Superior as revealed by natural radiocarbon measurements. Geophys. Res. Lett. 46, 5436–5444 (2019).

    Article  Google Scholar 

  30. Butman, B., Noble, M. & Folger, D. W. Long-term observations of bottom current and bottom sediment movement on the mid-Atlantic continental shelf. J. Geophys. Res. 84, 1187 (1979).

    Article  Google Scholar 

  31. Johnson, H. P. et al. Anomalous concentration of methane emissions at the continental shelf edge of the northern Cascadia margin. J. Geophys. Res. Solid Earth 124, 2829–2843 (2019).

    Article  Google Scholar 

  32. Riedel, M. et al. Distributed natural gas venting offshore along the Cascadia margin. Nat. Commun. 9, 3264 (2018).

    Article  Google Scholar 

  33. Merle, S. G. et al. Distribution of methane plumes on Cascadia margin and implications for the landward limit of methane hydrate stability. Front. Earth Sci. 9, 104 (2021).

    Article  Google Scholar 

  34. Phrampus, B. J., Harris, R. N. & Tréhu, A. M. Heat flow bounds over the Cascadia margin derived from bottom simulating reflectors and implications for thermal models of subduction. Geochem. Geophys. Geosyst. 18, 3309–3326 (2017).

    Article  Google Scholar 

  35. Feng, X. et al. 14C and 13C characteristics of higher plant biomarkers in Washington margin surface sediments. Geochim. Cosmochim. Acta 105, 14–30 (2013).

    Article  Google Scholar 

  36. Brothers, D. S. et al. Seabed fluid expulsion along the upper slope and outer shelf of the US Atlantic continental margin. Geophys. Res. Lett. https://doi.org/10.1002/2013gl058048 (2014).

  37. McGinnis, D. F., Greinert, J., Artemov, Y., Beaubien, S. E. & Wuest, A. Fate of rising methane bubbles in stratified waters: how much methane reaches the atmosphere? J. Geophys. Res. https://doi.org/10.1029/2005jc003183 (2006).

  38. Yamamoto, A., Yamanaka, Y. & Tajika, E. Modeling of methane bubbles released from large sea-floor area: condition required for methane emission to the atmosphere. Earth Planet. Sci. Lett. https://doi.org/10.1016/j.epsl.2009.05.026 (2009).

  39. Kvenvolden, K. A., Lorenson, T. D. & Reeburgh, W. S. Attention turns to naturally occurring methane seepage. Eos 82, 457–457 (2001).

    Article  Google Scholar 

  40. Saunois, M. et al. The global methane budget 2000~2012. Earth Syst. Sci. Data 8, 697–751 (2016).

    Article  Google Scholar 

  41. Etiope, G., Ciotoli, G., Schwietzke, S. & Schoell, M. Gridded maps of geological methane emissions and their isotopic signature. Earth Syst. Sci. Data https://doi.org/10.5194/essd-11-1-2019 (2019).

  42. Archer, D., Buffett, B. & Brovkin, V. Ocean methane hydrates as a slow tipping point in the global carbon cycle. Proc. Natl Acad. Sci. USA 106, 20596–20601 (2009).

    Article  Google Scholar 

  43. Dyonisius, M. N. et al. Old carbon reservoirs were not important in the deglacial methane budget. Science 367, 907–910 (2020).

    Article  Google Scholar 

  44. Etiope, G. & Schwietzke, S. Global geological methane emissions: an update of top-down and bottom-up estimates. Elementa 7, 47 (2019).

    Google Scholar 

  45. Kessler, J. D. et al. Basin-wide estimates of the input of methane from seeps and clathrates to the Black Sea. Earth Planet. Sci. Lett. 243.3–243.4, 366–375 (2006).

    Article  Google Scholar 

  46. Pohlman, L. W., Ruppel, C., Boze, L. G. & Xu, X. Significant modern carbon present in microbial methane at gas seeps and gas charged sediments along the northern US Atlantic Margin. In Proc. American Geophysical Union Fall Meeting, OS23A-01 (AGU, 2021).

  47. Hornbach, M. J., Ruppel, C., Saffer, D. M., Van Dover, C. L. & Holbrook, W. S. Coupled geophysical constraints on heat flow and fluid flux at a salt diapir. Geophys. Res. Lett. https://doi.org/10.1029/2005gl024862 (2005).

  48. Brothers, L. L. et al. Evidence for extensive methane venting on the southeastern US Atlantic margin. Geology 41, 807–810 (2013).

    Article  Google Scholar 

  49. Joung, D., Ruppel, C., Southon, J. & Kessler, J. D. Elevated levels of radiocarbon in methane dissolved in seawater reveal likely local contamination from nuclear powered vessels. Sci. Total Environ. 806, 150456 (2021).

    Article  Google Scholar 

  50. Van Dover, C. L. et al. Blake Ridge methane seeps: characterization of a soft-sediment, chemosynthetically based ecosystem. Deep Sea Res. 1 50, 281–300 (2003).

    Article  Google Scholar 

  51. Ruppel, C. D. et al. in World Atlas of Submarine Gas Hydrates in Continental Margins (eds Mienert, J. et al.) 287–302 (Springer, 2022); https://doi.org/10.1007/978-3-030-81186-0_24

  52. Prouty, N. G. et al. Insights into methane dynamics from analysis of authigenic carbonates and chemosynthetic mussels at newly-discovered Atlantic Margin seeps. Earth Planet. Sci. Lett. 449, 332–344 (2016).

    Article  Google Scholar 

  53. Sparrow, K. J. & Kessler, J. D. Efficient collection and preparation of methane from low concentration waters for natural abundance radiocarbon analysis. Limnol. Oceanogr. Methods 15, 601–617 (2017).

    Article  Google Scholar 

  54. Stuiver, M. & Polach, H. A. Discussion reporting of 14C data. Radiocarbon 19, 355–363 (1977).

    Article  Google Scholar 

  55. Weinstein, A. et al. Determining the flux of methane into Hudson Canyon at the edge of methane clathrate hydrate stability. Geochem. Geophys. Geosyst. 17, 3882–3892 (2016).

    Article  Google Scholar 

  56. Kessler, J. D. & Joung, D. Radiocarbon in Methane from Waters of the US Atlantic and Pacific Margins as Collected on R/V Hugh Sharp Cruise HRS1713 and R/V Rachel Carson Cruise RC0026 in 2017 and 2019 Version 1 (BCO-DMO, 2021); https://doi.org/10.26008/1912/bco-dmo.861576.1

  57. Baldwin, W. E. et al. Split-Beam Echo Sounder and Navigation Data Collected Using a Simrad EK80 Wide Band Tranceiver and ES38-10 Transducer During the Mid-Atlantic Resource Imaging Experiment (MATRIX), USGS Field Activity 2018-002-FA (USGS, 2021); https://doi.org/10.5066/P948VJ4X

Download references

Acknowledgements

D.J.J. thanks G. Kim and the Research Institute of Oceanography, Seoul National University, for the financial support. This work was possible due to the outstanding technical support from the officers and crew members of the RV Hugh R. Sharp and the RV Rachel Carlson. This research is funded to University of Rochester by the US National Science Foundation (OCE-1851402) and US Department of Energy (DOE) through DE-FE0028980. The USGS had funding from USGS–DOE interagency agreements DE-FE0026195 and 89243320SFE000013. Any use of trade, firm or product name is for descriptive purposes only and does not imply endorsement by the US government.

Author information

Authors and Affiliations

Authors

Contributions

D.J.J., C.R., T.S.W. and J.D.K. designed the study, and J.S. measured 14C–CH4 using the accelerator mass spectrometry (AMS). D.J.J. and J.D.K collected and prepared samples in the fields and laboratory. All authors equally contributed to the interpretation of the data and writing of this manuscript.

Corresponding author

Correspondence to DongJoo Joung.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Geoscience thanks Giuseppe Etiope, Jeanine Ash and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Xujia Jiang, in collaboration with the Nature Geoscience team.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Extended data

Extended Data Fig. 1 US-Atlantic margin sampling stations with hydroacoustic data.

Screen images of hydroacoustic data collected with a calibrated 38 kHz transducer on an EK60 split-beam sonar during the 2017 R/V Hugh Sharp cruise on the USAM. More information about data acquisition and the full dataset are available in refs. 15,57.

Extended Data Fig. 2 Measurement data of 14C–CH4 for US-Atlantic margin along with mixing model results.

Plots of (a) vertical profiles of 14C–CH4 and its relationship with depth from the US Atlantic margin, (b) the measured data (blue dots) and results from the two-endmember mixing model (red line)14, and (c) the comparison between the measured and mixing modeled 14C–CH4. For the regression in (a), two data points, 570 pMC and 325 pMC from T3S3 surface and T6S1 50 m, respectively, were excluded due to the potential impact from local anthropogenic contamination from nuclear power generation. For figure (b), values in T1S2 (458 nM and 0.1 pMC) and T6S1 (3.7 nM, 123.4 pMC) were used for the bottom and surface endmembers, respectively.

Source data

Extended Data Fig. 3 Hydroacoustic observations along the US-Pacific margin.

Screen images of seafloor seeps detected on the US-Pacific margin using a hydroacoustic sensor (EK80) during the research cruise.

Extended Data Fig. 4 Surface distributions of water properties.

Surface contour plots of (a) temperature, (b) salinity, (c) dissolved oxygen, (d) CH4 concentrations, (e) Chlorophyll a, and (f) nitrate concentrations (measured via Seabird Scientific, SUNA V2) in the Pacific margin. Colored dot represents 14C–CH4, and the color scale and station ID are shown in (b).

Source data

Extended Data Fig. 5 Procedures for sample collection and preparation for measurement.

Schematic diagrams of (a) gas extraction in the field and (c) gas purification in the laboratory. Pictures of equipment (b) in the field and (d) in the laboratory are also shown. Schematic diagrams (a and c) and photograph (d) were accessed from ref. 53.

Extended Data Fig. 6 Examples of gas standards and blanks subjected to the laboratory preparation procedures.

Example diagrams for the gas standard tests monitoring the performance of the laboratory gas-purification system; High and low standards, which were customized based on the concentrations in the collected samples, were measured throughout this study, the results of which are shown in (a) and (b), respectively. Total carbon blanks (c) for the purification system were also monitored daily when samples were run. Subplots in (a) and (b) show the trapping of CO2 converted from CH4. Plots (a) and (b) were reproduced from ref. 29.

Source data

Extended Data Fig. 7 Vertical profiles of ancillary data.

Top panel shows (a) temperature, (b) salinity, and (c) dissolved oxygen in Pacific margin sites. Bottom panel represents (d) temperature, (e) salinity and (f) dissolved oxygen in Atlantic margin sites.

Source data

Supplementary information

Supplementary Information

Additional discussion about the distributions of CH4 concentration and the fate of the released CH4.

Supplementary Table 1

Data from Pacific margin

Supplementary Table 2

Data from Atlantic margin

Source data

Source Data Fig. 1

Data for Fig. 1 in the main manuscript.

Source Data Fig. 2

Data for Fig. 2 in the main manuscript.

Source Data Fig. 3

Data for Fig. 3 in the main manuscript.

Source Data Fig. 4

Data for Fig. 4 in the main manuscript.

Source Data Fig. 5

Data for Fig. 5 in the main manuscript.

Source Data Extended Data Fig. 2

Data for Extended Data Fig. 2 in the main manuscript.

Source Data Extended Data Fig. 4

Data for Extended Data Fig. 4 in the main manuscript.

Source Data Extended Data Fig. 6

Data for Extended Data Fig. 6 in the main manuscript.

Source Data Extended Data Fig. 7

Data for Extended Data Fig. 7 in the main manuscript.

Rights and permissions

Springer Nature or its licensor holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Joung, D., Ruppel, C., Southon, J. et al. Negligible atmospheric release of methane from decomposing hydrates in mid-latitude oceans. Nat. Geosci. 15, 885–891 (2022). https://doi.org/10.1038/s41561-022-01044-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41561-022-01044-8

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing