ethane; methane; propane; shale gas; surface ozone; air quality
Abstract :
[en] Non-methane hydrocarbons such as ethane are important precursors to tropospheric ozone and aerosols. Using data from a global surface network and atmospheric column observations we show that the steady decline in ethane concentrations that began in the 1970s halted between 2005 and 2010 in most of the Northern Hemisphere, and has since reversed. We calculate a yearly increase in ethane emissions in the Northern Hemisphere of 0.42 (+/-0.19) Tg/yr between mid-2009 and mid-2014. The largest increases in ethane and for the shorter-lived propane are seen over the central and eastern USA, with a spatial distribution that suggests North American oil and natural gas development as the primary source of increasing emissions. By including other co-emitted oil and natural gas non-methane hydrocarbons, we estimate a Northern Hemisphere total non-methane hydrocarbon yearly emission increase of 1.2 (+/-0.8) Tg/yr. Atmospheric chemical transport modelling suggests that these emissions could augment summertime mean surface ozone by several nanomoles per mole near oil and natural gas production regions. Methane/ethane oil and natural gas emission ratios suggest a significant increase in associated methane emissions; however, this increase is inconsistent with observed leak rates in production regions and changes in methane’s global isotopic ratio.
Disciplines :
Earth sciences & physical geography
Author, co-author :
Helmig, Detlev; Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
Rossabi, Samuel; Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
Hueber, Jacques; Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
Tans, Pieter; Earth Systems Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, USA
Montzka, Stephen A.; Earth Systems Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, USA
Masarie, Ken; Earth Systems Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, USA
Thoning, Kirk; Earth Systems Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, USA
Carpenter, Lucy J.; Wolfson Atmospheric Chemistry Laboratories, University of York, UK
Lewis, Alastair C.; National Centre for Atmospheric Science, University of York, UK
Punjabi, Shalini; Wolfson Atmospheric Chemistry Laboratories, University of York, UK
Reimann, Stefan; Laboratory for Air Pollution and Environmental Technology, Empa, Swiss Federal Laboratories for Materials Science and Technology, Duebendorf, Switzerland
Vollmer, Martin K.; Laboratory for Air Pollution and Environmental Technology, Empa, Swiss Federal Laboratories for Materials Science and Technology, Duebendorf, Switzerland
Steinbrecher, Rainer; Karlsruhe Institute for Technology, Campus Alpine, Garmisch- Partenkirchen, Germany
Hannigan, James W.; National Center for Atmospheric Research, Boulder, USA
Emmons, Louisa K.; National Center for Atmospheric Research, Boulder, USA
Mahieu, Emmanuel ; Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Franco, Bruno ; Université de Liège > R&D Direction : Chercheurs ULiège en mobilité
Smale, Dan; National Institute of Water and Atmospheric Research, Lauder, New Zealand
Pozzer, Andrea; Max Planck Institute for Chemistry, Mainz, Germany
BELSPO - SPP Politique scientifique - Service Public Fédéral de Programmation Politique scientifique F.R.S.-FNRS - Fonds de la Recherche Scientifique [BE]
Aydin, M. et al. Recent decreases in fossil-fuel emissions of ethane and methane derived from firn air. Nature 476, 198-201 (2011).
Worton, D. R. et al. Evidence from firn air for recent decreases in non-methane hydrocarbons and a 20th century increase in nitrogen oxides in the northern hemisphere. Atmos. Environ. 54, 592-602 (2012).
Helmig, D. et al. Reconstruction of Northern Hemisphere 1950-2010 atmospheric non-methane hydrocarbons. Atmos. Chem. Phys. 14, 1463-1483 (2014).
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 (2015).
Von Schneidemesser, E., Monks, P. S., Plass-Duelmer, C. Global comparison of VOC and CO observations in urban areas. Atmos. Environ. 44, 5053-5064 (2010).
Warneke, C. et al. Multiyear trends in volatile organic compounds in Los Angeles, California: five decades of decreasing emissions. J. Geophys. Res. 117, D00V17 (2012).
Simpson, I. J. et al. Long-term decline of global atmospheric ethane concentrations and implications for methane. Nature 488, 490-494 (2012).
Kramer, L. J. et al. Seasonal variability of atmospheric nitrogen oxides and non-methane hydrocarbons at the GEOSummit station, Greenland. Atmos. Chem. Phys. 12, 6827-6849 (2015).
Plass-Duelmer, C., Michl, K., Ruf, R., Berresheim, H. C2-C8 hydrocarbon measurement and quality control procedures at the Global AtmosphereWatch Observatory Hohenpeissenberg. J. Chrom. 953, 175-197 (2002).
Read, K. A. et al. Intra-annual cycles of NMVOC in the tropical marine boundary layer and their use for interpreting seasonal variability in CO. J. Geophys. Res. 114, D21303 (2009).
Leuchner, M. et al. Can positive matrix factorization help to understand patterns of organic trace gases at the continental Global AtmosphereWatch site Hohenpeissenberg? Atmos. Chem. Phys. 15, 1221-1236 (2015).
Franco, B. et al. Retrieval of ethane from ground-based FTIR solar spectra using improved spectroscopy: recent burden increase above Jungfraujoch. J. Quant. Spec. Radiat. Trans. 160, 36-49 (2015).
Pétron, G. et al. Hydrocarbon emissions characterization in the Colorado Front Range: a pilot study. J. Geophys. Res. 117, 1-19 (2012).
Helmig, D. et al. Highly elevated atmospheric levels of volatile organic compounds in the Uintah Basin, Utah. Environ. Sci. Technol. 48, 4707-4715 (2014).
Thompson, C. R., Hueber, J., Helmig, D. Influence of oil and gas emissions on ambient atmospheric non-methane hydrocarbons in residential areas of Northeastern Colorado. Elementa 2, 1-16 (2014).
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).
Karion, A. et al. Methane emissions estimate from airborne measurements over a western United States natural gas field. Geophys. Res. Lett. 40, 4393-4397 (2013).
Schnell, R. C. et al. Rapid photochemical production of ozone at high concentrations in a rural site during winter. Nature Geosci. 2, 120-122 (2009).
Oltmans, S. et al. Anatomy of wintertime ozone associated with oil and natural gas extraction activity inWyoming and Utah. Elementa 2, 1-15 (2014).
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).
Schade, G.W., Roest, G. S. Is the shale boom reversing progress in curbing ozone pollution? EOS 96, http://dx.doi.org/10.1029/2015EO028279 (2015).
US Greenhouse Gas Inventory (EPA, accessed 4 April, 2016); https://www3.epa.gov/climatechange/ghgemissions/index.html.
Kirschke, S. et al. Three decades of global methane sources and sinks. Nature Geosci. 6, 813-823 (2013).
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).
Hausmann, P., Sussmann, R., Smale, D. Contribution of oil and natural gas production to renewed increase of atmospheric methane (2007-2014): top-down estimate from ethane and methane column observations. Atmos. Chem. Phys. 16, 3227-3244 (2016).
Turner, A. J. et al. A large increase in US methane emissions over the past decade inferred from satellite data and surface observations. Geophys. Res. Lett. 43, 2218-2224 (2016).
Schaefer, H. et al. A 21st century shift from fossil-fuel to biogenic methane emissions indicated by 13CH4. Science http://dx.doi.org/10.1126/science.aad2705 (2016).
Peischl, J. et al. Quantifying atmospheric methane emissions from the Haynesville, Fayetteville, and northeastern Marcellus shale gas production regions. J. Geophys. Res. 120, 2119-2139 (2015).
Karion, A. et al. Aircraft-based estimate of total methane emissions from the Barnett Shale region. Environ. Sci. Technol. 49, 8124-8131 (2015).
Petron, 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. 119, 6836-6852 (2014).
Pollmann, J. et al. Sampling, storage, and analysis of C2-C7 non-methane hydrocarbons from the US National Oceanic and Atmospheric Administration Cooperative Air Sampling Network glass flasks. J. Chromatogr. A 1188, 75-87 (2008).
Helmig, D. et al. Volatile organic compounds in the global atmosphere. Eos Trans. AGU 90, 513-514 (2009).
World Calibration Centre for Volatile Organic Compounds (WCC-VOC) (Karlsruhe Institute of Technology, accessed 14 April 2016); http://www.imk-ifu.kit.edu/wcc-voc.
AWMO/GAW ExpertWorkshop on Global Long-Term Measurements of Volatile Organic Compounds (VOCs), Report No. 171 36 (WMO, 2007).
Pollmann, J., Helmig, D., Hueber, J., Tanner, D., Tans, P. P. Evaluation of solid adsorbent materials for cryogen-free trapping-gas chromatographic analysis of atmospheric C2-C6 non-methane hydrocarbons. J. Chromatogr. A 1134, 1-15 (2006).
Global Atmospheric VOC Monitoring Program (Atmospheric Research Laboratory, Institute of Arctic and Alpine Research, University of Colorado, accessed 31 March 2016); http://instaar.colorado.edu/arl/Global-VOC.html
Helmig, D., Stephens, C. R., Caramore, J., Hueber, J. Seasonal behavior of non-methane hydrocarbons in the firn air at Summit, Greenland. Atmos. Environ. 85, 234-246 (2014).
Miller, B. R. et al. Medusa: a sample preconcentration and GC/MS detector system for in situ measurements of atmospheric trace halocarbons, hydrocarbons, and sulfur compounds. Anal. Chem. 80, 1536-1545 (2008).
Rhoderick, G. C. et al. International comparison of a hydrocarbon gas standard at the picomol per mol level. Anal. Chem. 86, 2580-2589 (2014).
Thoning, K.W., Tans, P. P., Komhyr,W. D. Atmospheric carbon-dioxide at Mauna Loa observatory.2. analysis of the NOAA GMCC data, 1974-1985. J. Geophys. Res. 94, 8549-8565 (1989).
Yue, S., Pilon, P., Cavadias, G. Power of the Mann-Kendall and Spearman's rho tests for detecting monotonic trends in hydrological series. J. Hydrol. 259, 254-271 (2002).
Masarie, K. A., Tans, P. P. Extension and integration of atmospheric carbon-dioxide data into a globally consistent measurement record. J. Geophys. Res. 100, 11593-11610 (1995).
GLOBALVIEW (NOAA Earth System Research Laboratory Global Monitoring Division, accessed 4 April 2016), http://www.esrl.noaa.gov/gmd/ccgg/globalview.
Tans, P. P., Conway, T. J., Nakazawa, T. Latitudinal distribution of the sources and sinks of atmospheric carbon-dioxide derived from surface observations and an atmospheric transport model. J. Geophys. Res. 94, 5151-5172 (1989).
Rinsland, C. P. et al. Multiyear infrared solar spectroscopic measurements of HCN, CO, C2H6, and C2H2 tropospheric columns above Lauder, New Zealand (45-S latitude). J. Geophys. Res. 107, ACH 1-1-ACH 1-12 (2002).
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).
Gardiner, T. et al. Trend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments. Atmos. Chem. Phys. 8, 6719-6727 (2008).
Janssens-Maenhout, G. et al. HTAP-v2: a mosaic of regional and global emission gridmaps for 2008 and 2010 to study hemispheric transport of air pollution. Atmos. Chem. Phys. 15, 12867-12909 (2015).
Guenther, A. B. et al. The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions. Geosci. Model Dev. 5, 1471-1492 (2012).
Wiedinmyer, C. et al. The Fire INventory from NCAR (FINN): a high resolution global model to estimate the emissions from open burning. Geosci. Model Dev. 4, 625-641 (2011).
Riahi, K., Grübler, A., Nakicenovic, N. Scenarios of long-term socio-economic and environmental development under climate stabilization. Technol. Forecast. Soc. Change 74, 887-935 (2007).
Pozzer, A. et al. AOD trends during 2001-2010 from observations and model simulations. Atmos. Chem. Phys. 15, 5521-5535 (2015).
Swarthout, R. F., Russo, R. S., Zhou, Y., Hart, A. H., Sive, B. C. Volatile organic compound distributions during the NACHTT campaign at the Boulder Atmospheric Observatory: influence of urban and natural gas sources. J. Geophys. Res. 118, 10614-10637 (2013).
Jöckel, P. et al. Development cycle 2 of the modular earth submodel system (MESSy2). Geosci. Model Dev. 3, 717-752 (2010).
Pozzer, A. et al. Observed and simulated global distribution and budget of atmospheric C2-C5 alkanes. Atmos. Chem. Phys. 10, 4403-4422 (2010).