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:

Discrepancy between simulated and observed ethane and propane levels explained by underestimated fossil emissions

Abstract

Ethane and propane are the most abundant non-methane hydrocarbons in the atmosphere. However, their emissions, atmospheric distribution, and trends in their atmospheric concentrations are insufficiently understood. Atmospheric model simulations using standard community emission inventories do not reproduce available measurements in the Northern Hemisphere. Here, we show that observations of pre-industrial and present-day ethane and propane can be reproduced in simulations with a detailed atmospheric chemistry transport model, provided that natural geologic emissions are taken into account and anthropogenic fossil fuel emissions are assumed to be two to three times higher than is indicated in current inventories. Accounting for these enhanced ethane and propane emissions results in simulated surface ozone concentrations that are 5–13% higher than previously assumed in some polluted regions in Asia. The improved correspondence with observed ethane and propane in model simulations with greater emissions suggests that the level of fossil (geologic + fossil fuel) methane emissions in current inventories may need re-evaluation.

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

Access options

Rent or buy this article

Prices vary by article type

from$1.95

to$39.95

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

Fig. 1: Global total sectoral ethane emissions in this study and other studies.
Fig. 2: Observed and modelled annual mean ethane mixing ratios and inter-polar ratios.
Fig. 3: Comparison of year 2011 modelled and observed ethane and propane at surface sites.
Fig. 4: Footprints at Zeppelin.

Similar content being viewed by others

References

  1. Rudolph, J. The tropospheric distribution and budget of ethane.J. Geophys. Res. Atmos.100, 11369–11381 (1995).

    Google Scholar 

  2. Rosado-Reyes, C. M. & Francisco, J. S. Atmospheric oxidation pathways of propane and its by-products: Acetone, acetaldehyde, and propionaldehyde. J. Geophys. Res Atmos.112, D14310 (2007).

    Google Scholar 

  3. Franco, B. et al. Evaluating ethane and methane emissions associated with the development of oil and natural gas extraction in North America. Environ. Res. Lett.11, 044010 (2016).

    Google Scholar 

  4. Helmig, D. et al. Reversal of global atmospheric ethane and propane trends largely due to US oil and natural gas production. Nat. Geosci.9, 490–495 (2016).

    Google Scholar 

  5. Stein, O. & Rudolph, J. Modeling and interpretation of stable carbon isotope ratios of ethane in global chemical transport models. J. Geophys. Res. Atmos.112, D14308 (2007).

    Google Scholar 

  6. Thompson, A., Rudolph, J., Rohrer, F. & Stein, O. Concentration and stable carbon isotopic composition of ethane and benzene using a global three-dimensional isotope inclusive chemical tracer model. J. Geophys. Res. Atmos.108, 4373 (2003).

    Google Scholar 

  7. Emmons, L. K. et al. The POLARCAT Model Intercomparison Project (POLMIP): overview and evaluation with observations. Atmos. Chem. Phys.15, 6721–6744 (2015).

    Google Scholar 

  8. Li, M. et al. Mapping Asian anthropogenic emissions of non-methane volatile organic compounds to multiple chemical mechanisms. Atmos. Chem. Phys.14, 5617–5638 (2014).

    Google Scholar 

  9. Schwietzke, S., Griffin, W. M., Matthews, H. S. & Bruhwiler, L. M. P. Global bottom-up fossil fuel fugitive methane and ethane emissions inventory for atmospheric modeling. ACS Sustain. Chem. Eng.2, 1992–2001 (2014).

    Google Scholar 

  10. Höglund-Isaksson, L. Bottom-up simulations of methane and ethane emissions from global oil and gas systems 1980 to 2012. Environ. Res. Lett.12, 024007 (2017).

    Google Scholar 

  11. Huang, G. et al. Speciation of anthropogenic emissions of non-methane volatile organic compounds: a global gridded data set for 1970–2012.Atmos. Chem. Phys.17, 7683–7701 (2017).

    Google Scholar 

  12. Xiao, Y. et al. Global budget of ethane and regional constraints on U.S. sources. J. Geophys. Res. Atmos.113, D21306 (2008).

    Google Scholar 

  13. Zavala-Araiza, D. et al. Reconciling divergent estimates of oil and gas methane emissions. Proc. Natl. Acad. Sci. USA112, 15597–15602 (2015).

    Google Scholar 

  14. Karion, A. et al. Aircraft-based estimate of total methane emissions from the Barnett Shale region. Environ. Sci. Technol.49, 8124–8131 (2015).

    Google Scholar 

  15. Kort, E. A. et al. Four corners: the largest US methane anomaly viewed from space. Geophys. Res. Lett.41, 6898–6903 (2014).

    Google Scholar 

  16. Kort, E. A. et al. Fugitive emissions from the Bakken shale illustrate role of shale production in global ethane shift. Geophys. Res. Lett.43, 4617–4623 (2016).

    Google Scholar 

  17. Peischl, J. et al. Quantifying atmospheric methane emissions from the Haynesville, Fayetteville, and northeastern Marcellus shale gas production regions. J. Geophys. Res. Atmos.120, 2119–2139 (2015).

    Google Scholar 

  18. Pétron, G. et al. A new look at methane and nonmethane hydrocarbon emissions from oil and natural gas operations in the Colorado Denver-Julesburg Basin. J. Geophys. Res. Atmos.119, 6836–6852 (2014).

    Google Scholar 

  19. Swarthout, R. F. et al. Impact of Marcellus shale natural gas development in southwest Pennsylvania on volatile organic compound emissions and regional air quality. Environ. Sci. Technol.49, 3175–3184 (2015).

    Google Scholar 

  20. Vinciguerra, T. et al. Regional air quality impacts of hydraulic fracturing and shale natural gas activity: evidence from ambient VOC observations. Atmos. Environ.110, 144–150 (2015).

    Google Scholar 

  21. Schneising, O. et al. Remote sensing of fugitive methane emissions from oil and gas production in North American tight geologic formations.Earth’s Future2, 548–558 (2014).

    Google Scholar 

  22. Moore, C. W., Zielinska, B., Pétron, G. & Jackson, R. B. Air impacts of increased natural gas acquisition, processing, and use: a critical review. Environ. Sci. Technol.48, 8349–8359 (2014).

    Google Scholar 

  23. Roest, G. & Schade, G. Quantifying alkane emissions in the Eagle Ford Shale using boundary layer enhancement. Atmos. Chem. Phys.17, 11163–11176 (2017).

    Google Scholar 

  24. Pozzer, A. et al. Simulating organic species with the global atmospheric chemistry general circulation model ECHAM5/MESSy1: a comparison of model results with observations. Atmos. Chem. Phys.7, 2527–2550 (2007).

    Google Scholar 

  25. González Abad, G. et al. Ethane, ethyne and carbon monoxide concentrations in the upper troposphere and lower stratosphere from ACE and GEOS-Chem: a comparison study. Atmos. Chem. Phys.11, 9927–9941 (2011).

    Google Scholar 

  26. Angelbratt, J. et al. Carbon monoxide (CO) and ethane (C2H6) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model. Atmos. Chem. Phys.11, 9253–9269 (2011).

    Google Scholar 

  27. Lin, M., Holloway, T., Carmichael, G. R. & Fiore, A. M. Quantifying pollution inflow and outflow over East Asia in spring with regional and global models. Atmos. Chem. Phys.10, 4221–4239 (2010).

    Google Scholar 

  28. Helmig, D. et al. Climatology and atmospheric chemistry of the non-methane hydrocarbons ethane and propane over the North Atlantic. Elementa3 (2015).

  29. Pozzer, A. et al. Observed and simulated global distribution and budget of atmospheric C2–C5 alkanes. Atmos. Chem. Phys.10, 4403–4422 (2010).

    Google Scholar 

  30. Helmig, D. et al. Reconstruction of Northern Hemisphere 1950–2010 atmospheric non-methane hydrocarbons. Atmos. Chem. Phys.14, 1463–1483 (2014).

    Google Scholar 

  31. Simpson, I. J. et al. Long-term decline of global atmospheric ethane concentrations and implications for methane. Nature488, 490–494 (2012).

    Google Scholar 

  32. Hausmann, P., Sussmann, R. & Smale, D. Contribution of oil and natural gas production to renewed increase in atmospheric methane (2007–2014): top–down estimate from ethane and methane column observations. Atmos. Chem. Phys.16, 3227–3244 (2016).

    Google Scholar 

  33. Aydin, M. et al. Recent decreases in fossil-fuel emissions of ethane and methane derived from firn air. Nature476, 198–201 (2011).

    Google Scholar 

  34. Zeng, G. et al. Trends and variations in CO, C2H6, and HCN in the Southern Hemisphere point to the declining anthropogenic emissions of CO and C2H6. Atmos. Chem. Phys.12, 7543–7555 (2012).

    Google Scholar 

  35. Schwietzke, S., Griffin, W. M., Matthews, H. S. & Bruhwiler, L. M. P. Natural gas fugitive emissions rates constrained by global atmospheric methane and ethane. Environ. Sci. Technol.48, 7714–7722 (2014).

    Google Scholar 

  36. Sherwood, O. A., Schwietzke, S., Arling, V. A. & Etiope, G. Global inventory of gas geochemistry data from fossil fuel, microbial and biomass burning sources, version 2017. Earth Syst. Sci. Data9, 639–656 (2017).

    Google Scholar 

  37. Stohl, A. et al. Black carbon in the Arctic: the underestimated role of gas flaring and residential combustion emissions. Atmos. Chem. Phys.13, 8833–8855 (2013).

    Google Scholar 

  38. McLinden, C. A. et al. Space-based detection of missing sulfur dioxide sources of global air pollution. Nat. Geosci.9, 496–500 (2016).

    Google Scholar 

  39. Nicewonger, M. R., Verhulst, K. R., Aydin, M. & Saltzman, E. S. Preindustrial atmospheric ethane levels inferred from polar ice cores: a constraint on the geologic sources of atmospheric ethane and methane. Geophys. Res. Lett.43, 214–221 (2016).

    Google Scholar 

  40. Etiope, G. & Ciccioli, P. Earth’s degassing: a missing ethane and propane source. Science323, 478–478 (2009).

    Google Scholar 

  41. Aikin, A. C., Herman, J. R., Maier, E. J. & McQuillan, C. J. Atmospheric chemistry of ethane and ethylene. J. Geophys. Res. Oceans87, 3105–3118 (1982).

    Google Scholar 

  42. Patra, P. K. et al. Observational evidence for interhemispheric hydroxyl-radical parity. Nature513, 219–223 (2014).

    Google Scholar 

  43. Strode, S. A. et al. Implications of carbon monoxide bias for methane lifetime and atmospheric composition in chemistry climate models.Atmos. Chem. Phys.15, 11789–11805 (2015).

    Google Scholar 

  44. Rigby, M. et al. Role of atmospheric oxidation in recent methane growth. Proc. Natl Acad. Sci. USA114, 5373–5377 (2017).

    Google Scholar 

  45. Naik, V. et al. Preindustrial to present-day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Atmos. Chem. Phys.13, 5277–5298 (2013).

    Google Scholar 

  46. Søvde, O. A. et al. The chemical transport model Oslo CTM3.Geosci. Model Dev.5, 1441–1469 (2012).

    Google Scholar 

  47. Hoesly, R. M. et al. Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emission Data System (CEDS).Geosci. Model Dev.11, 369–408 (2018).

    Google Scholar 

  48. Stohl, A., Forster, C., Frank, A., Seibert, P. & Wotawa, G. Technical note: the Lagrangian particle dispersion model FLEXPART version 6.2.Atmos. Chem. Phys.5, 2461–2474 (2005).

    Google Scholar 

  49. Smith, M. L. et al. Airborne ethane observations in the Barnett Shale: quantification of ethane flux and attribution of methane emissions.Environ. Sci. Technol.49, 8158–8166 (2015).

    Google Scholar 

  50. Carpenter, L. J. et al. Seasonal characteristics of tropical marine boundary layer air measured at the Cape Verde Atmospheric Observatory. J. Atmos. Chem.67, 87–140 (2010).

    Google Scholar 

  51. Petrenko, V. V. et al. Minimal geological methane emissions during the Younger Dryas–Preboreal abrupt warming event. Nature548, 443–446 (2017).

    Google Scholar 

  52. Schwietzke, S. et al. Upward revision of global fossil fuel methane emissions based on isotope database. Nature538, 88–91 (2016).

    Google Scholar 

  53. Etiope, G., Lassey, K. R., Klusman, R. W. & Boschi, E. Reappraisal of the fossil methane budget and related emission from geologic sources. Geophys. Res. Lett.35, L09307 (2008).

    Google Scholar 

  54. Rigby, M. et al. Renewed growth of atmospheric methane. Geophys. Res. Lett.35, L22805 (2008).

    Google Scholar 

  55. Dlugokencky, E. J. et al. Observational constraints on recent increases in the atmospheric CH4 burden. Geophys. Res. Lett.36, L18803 (2009).

    Google Scholar 

  56. Tzompa-Sosa, Z. A. et al. Revisiting global fossil fuel and biofuel emissions of ethane. J. Geophys. Res. Atmos.122, 2493–2512 (2017).

    Google Scholar 

  57. Dalsøren, S. B. et al. Atmospheric methane evolution the last 40 years. Atmos. Chem. Phys.16, 3099–3126 (2016).

    Google Scholar 

  58. van der Werf, G. R. et al. Global fire emissions and the contribution of deforestation, savanna, forest, agricultural, and peat fires (1997–2009). Atmos. Chem. Phys.10, 11707–11735 (2010).

    Google Scholar 

  59. van van Marle, M. J. E. et al. Historic global biomass burning emissions based on merging satellite observations with proxies and fire models (1750–2015). Geosci. Model Dev.10, 3329–3357 (2017).

    Google Scholar 

  60. Berglen, T., Berntsen, T., Isaksen, I. & Sundet, J. A global model of the coupled sulfur/oxidant chemistry in the troposphere: the sulfur cycle. J. Geophys. Res. Atmos.109, D19310 (2004).

    Google Scholar 

  61. Sindelarova, K. et al. Global dataset of biogenic VOC emissions calculated by the MEGAN model over the last 30 years. Atmos. Chem. Phys.14, 9317–9341 (2014).

    Google Scholar 

  62. Pulles, T. et al. Reanalysis of the Tropospheric Chemical Composition Over the Past 40 years: A Long-term Global Modeling Study of Tropospheric Chemistry Funded Under the 5th EU Framework Programme EU-Contract No. EVK2-CT-2002-00170 (ed. Schultz, M.) (GEIA, Retro, 2008).

  63. Bouwman, A. F. et al. A global high-resolution emission inventory for ammonia. Glob. Biogeochem. Cycles11, 561–587 (1997).

    Google Scholar 

  64. Etiope, G. & Klusman, R. W. Microseepage in drylands: flux and implications in the global atmospheric source/sink budget of methane. Glob. Planet. Change72, 265–274 (2010).

    Google Scholar 

  65. Lamarque, J. F. et al. Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application. Atmos. Chem. Phys.10, 7017–7039 (2010).

    Google Scholar 

  66. Atkinson, R. Kinetics of the gas-phase reactions of OH radicals with alkanes and cycloalkanes. Atmos. Chem. Phys.3, 2233–2307 (2003).

    Google Scholar 

  67. Prinn, R. G. et al. Evidence for variability of atmospheric hydroxyl radicals over the past quarter century. Geophys. Res. Lett.32, L07809 (2005).

    Google Scholar 

  68. Prather, M. J., Holmes, C. D. & Hsu, J. Reactive greenhouse gas scenarios: systematic exploration of uncertainties and the role of atmospheric chemistry. Geophys. Res. Lett.39, L09803 (2012).

    Google Scholar 

  69. Rappenglück, B. et al. The first VOC intercomparison exercise within the Global Atmosphere Watch (GAW). Atmos. Environ.40, 7508–7527 (2006).

    Google Scholar 

  70. Hoerger, C. C. et al. ACTRIS non-methane hydrocarbon intercomparison experiment in Europe to support WMO GAW and EMEP observation networks. Atmos. Meas. Tech.8, 2715–2736 (2015).

    Google Scholar 

  71. Plass-Dülmer, C., Schmidbauer, N., Slemr, J., Slemr, F. & D’Souza, H. European hydrocarbon intercomparison experiment AMOHA part 4: Canister sampling of ambient air. J. Geophys. Res. Atmos.111, D04306 (2006).

    Google Scholar 

  72. Schultz, M. G. et al. The Global Atmosphere Watch reactive gases measurement network. Elem. Sci. Anth.3, 67 (2015).

  73. Helmig, D. et al. Volatile organic compounds in the global atmosphere. Eos90, 513–514 (2009).

    Google Scholar 

Download references

Acknowledgements

This research is funded by the Research Council of Norway through the MOCA (Methane Emissions from the Arctic Ocean to the Atmosphere: Present and Future Climate Effects) project (grant no. 225814). The Flexpart work was partially funded by the Nordic Center of Excellence eSTICC (eScience Tools for Investigating Climate Change in northern high latitudes) funded by Nordforsk (grant 57001). Furthermore, the conclusions of the paper is largely supported and strengthened by the use of globally distributed observational data and we acknowledge all data providers and the great efforts of EMEP, ACTRIS, NOAA ESRL/INSTAAR and The World Data Centre for Greenhouse Gases (WDCGG) under the WMO-GAW programme to make long-term measurements public and available. The Horizon 2020 research and innovation programme ACTRIS-2 Integrating Activities (grant agreement no. 654109) is acknowledged for the work with quality assurance and quality control of NMHC data in Europe. The VOC observations within the NOAA-INSTAAR GGGRN are supported in part by the US National Oceanic and Atmospheric Administration’s Climate Program Office’s AC4 Program, and quality control was supported in part by the US National Science Foundation grant no. 1108391. The GLOGOS dataset was kindly provided by CGG Geoconsulting. CGG Geoconsulting also provided us with a derived product from the Global Offshore Seepage Database (GOSD) indicating where offshore seepage occurs.

Author information

Authors and Affiliations

Authors

Contributions

S.B.D., G.M. and Ø.H. designed the study with input from A.S., C.L.M. and I.P. S.B.D performed the simulations with the OsloCTM3 model, analysed the model results and performed the comparisons with measurement data. Ø.H. and G.M. provided assistance with the analysis and comparison studies. I.P performed the simulations with the Flexpart model and I.P. and A.S. analysed the output. S.Schwietzke and L.H.-I. provided the new emission datasets for fugitive fossil fuel emissions. S.B.D. developed gridded inventories for geologic emissions. C.L.M, D.H., S.R., S.S., N.S., K.A.R., L.J.C., A.C.L., S.P. and M.W. provided the observational data for ethane and propane. S.B.D. led the writing of the manuscript in close collaboration with G.M. and Ø.H. All authors contributed to the writing and review of the manuscript.

Corresponding author

Correspondence to Stig B. Dalsøren.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

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

Supplementary information

Supplementary Information

Supplementary Figures, Tables and Discussion.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Dalsøren, S.B., Myhre, G., Hodnebrog, Ø. et al. Discrepancy between simulated and observed ethane and propane levels explained by underestimated fossil emissions. Nature Geosci 11, 178–184 (2018). https://doi.org/10.1038/s41561-018-0073-0

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41561-018-0073-0

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