Skip to main content
SpringerLink
Log in

AGAGE Observations of Methyl Bromide and Methyl Chloride at Mace Head, Ireland, and Cape Grim, Tasmania, 1998–2001

Journal of Atmospheric Chemistry Aims and scope Submit manuscript

Cite this article

Abstract

In situ AGAGE GC-MS measurements of methyl bromide (CH3Br) and methyl chloride (CH3Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr−1 (CH3Br) and 2.6% yr−1 (CH3Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH3Br and CH3Cl also show annual decreases in their baseline mixing ratios of 2.5% yr−1 and 1.5% yr−1, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH3Br) and 541.3 ± 1.1 ppt (CH3Cl). Although CH3Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH3Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

References

  • Bassford, M. R., Nickless, G., Simmonds, P. G., Lewis, A. C., Pilling, M. J., and Evans, M. J., 1999: The concurrent observation of methyl iodide and dimethyl sulphide in marine air; implications for sources of atmospheric methyl iodide, Atmos. Environ. 33, 2373–2383.

    Article  Google Scholar 

  • Beardsmore, D. J. and Pearman, G. I., 1987: Atmospheric carbon dioxide measurements in the Australian Region: data from surface observatories, Tellus 39B, 42–66.

    Google Scholar 

  • Butler, J. H., 2000: Better budgets for methyl halides? Nature 403, 260–261.

    Google Scholar 

  • Cox, M. L., 2001: A regional study of the natural and anthropogenic sources and sinks of the major halomethanes, PhD Thesis, Monash University, Australia, 2001.

    Google Scholar 

  • Cox, M. L., Sturrock, J. A., Fraser, P. J., Siems, S., Krummel, P., and O'Doherty, S., 2003a: Regional sources of methyl chloride, chloroform and dichloromethane, identified from AGAGE observations at Cape Grim, Tasmania 1988–2000, J. Atmos. Chem. 45, 79–99.

    Article  Google Scholar 

  • Cox, M. L., Sturrock, G. A., Fraser, P. J., Siems, S., and Krummel, P. B., 2003b: Identification of regional sources of methyl bromide and methyl iodide from AGAGE observations at Cape Grim, Tasmania, J. Atmos. Chem., in preparation.

  • Crill, P. M., 2000: Natural terrestrial sources and sinks of tropospheric methyl bromide, IGACtivities, 19, 13–15.

    Google Scholar 

  • Derwent R. G., Simmonds, P. G., O'Doherty, S., Ciais, P., and Ryall, D. B., 1998a: European source strengths and Northern Hemisphere baseline concentrations of radiatively active trace gases at Mace Head, Ireland, Atmos. Environ. 32, 3703–3715.

    Google Scholar 

  • Derwent, R. G., Simmonds, P.G., Seuring, S., and Dimmer, C., 1998b: Observation and interpretation of the seasonal cycles in the surface concentrations of ozone and carbon monoxide at Mace Head, Ireland from 1990 to 1994, Atmos. Environ. 32, 145–147.

    Google Scholar 

  • Derwent, R. G., Ryall, D. B., Manning, A. J., Simmonds, P. G., O'Doherty, S., Biraud, S., Ciais, P., Ramonet, M., and Jennings, S. G., 2002: Continuous observations of carbon dioxide at Mace Head, Ireland from 1995 to 1999 and its net European ecosystem exchange, Atmos. Environ. 36, 2799–2807.

    Article  Google Scholar 

  • Dimmer, C. H., Simmonds, P. G., Nickless, G. N., and Bassford, M. R., 2001: Biogenic fluxes of halomethanes from Irish peatland ecosystems, Atmos. Environ. 31, 321–330.

    Google Scholar 

  • Goodwin, J. W. L., Salway, A. G., Murrells, T. P., Dore, C. J., Passant, N. R., King, K. R., Coleman, P. J., Hobson, M. M., Pye, S. T., and Watterson, J. D., 2001: U.K. emissions of air pollutants 1970–1999, AEA Technology Report AEAT/ENV/R/0798, Oxfordshire, U.K.

  • Harper, D. B., 1985: Halomethane from halide ion — a highly efficient fungal conversion of environmental significance, Nature 315, 55–57.

    Article  Google Scholar 

  • IPCC, 2001: Climate change 2001. The scientific basis, Intergovernmental Panel on Climate Change, Cambridge University Press, U.K.

    Google Scholar 

  • Khalil, M. A. K. and Rasmussen, R. A., 1999: Atmospheric methyl chloride, Atmos. Environ. 33, 1305–1321.

    Google Scholar 

  • King, D. B., Butler, J. H., Montzka, S. A., Yvon-Lewis, S. A., and Elkins, J. W., 2000: Implications of methyl bromide supersaturations in the temperate North Atlantic Ocean, J. Geophys. Res. 105, 19763–19769.

    Google Scholar 

  • Keppler, F., Elden, R., Niedan, V., Pracht, J., and Scholer, H. F., 2000: Halocarbons produced by natural oxidation processes during degradation of organic matter, Nature 403, 298–301.

    Article  Google Scholar 

  • Lagenfelds, R. L., Francey, R. J., Pak, B. C., Steele, L. P., Lloyd, J., Trudinger, C. M., Allison, C. E., 2002, Interannual growth rate variations of atmospheric CO2 and its δ 13C, H2, CH4, and CO between 1992 and 1999 linked to biomass burning, Global Geochem. Cycles 16, 1048, doi:10.1029/2001/GB001466.

    Google Scholar 

  • Li, H-J., Yokouchi, Y., and Akimoto, H., 1999: Measurement of methyl halides in the marine atmosphere, Atmos. Environ. 33, 1881–1887.

    Google Scholar 

  • Lobert, J. M., Yvon-Lewis, S. A., Butler, J. H., Montzka, S. A., and Myers, R. C., 1997: Undersaturations of CH3Br in the Southern Ocean, Geophys. Res. Lett. 24, 171–172.

    Article  Google Scholar 

  • Manning, A. J., Ryall, D. B., Derwent, R. G., Simmonds, P. G., and O'Doherty, S., 2002: Estimating European emissions of ozone-depleting and greenhouse gases using observations and a modelling back-attribution technique, J. Geophys. Res. 108(D14), 4404.

    Google Scholar 

  • Manö, S. and Andreae, M. O., 1994: Emission of methyl bromide from biomass burning, Science 263, 1255–1257.

    Google Scholar 

  • McCulloch, A., Aucott, M. L., Benkovitz, C. M., Graedel, T. E., Kleiman, G., Midgley, P. M., and Li, Y.-F., 1999: Global emissions of hydrogen chloride and chloromethane from coal combustion, incineration and industrial activities, J. Geophys. Res. 104, 8391–8403.

    Google Scholar 

  • Miller, B. R., 1998: Abundances and trends of atmospheric chlorodifluoromethane and bromomethane, PhD Thesis, University of California, San Diego, p. 149.

    Google Scholar 

  • Miller, B. R., Huang, J., Weiss, R. F., Prinn, R. G., and Fraser, P. J., 1998: Atmospheric trend and lifetime of chlorodifluoromethane (HCFC-22) and the global tropospheric OH concentration, J. Geophys. Res. 103, 13237–13248.

    Article  Google Scholar 

  • Montzka and Fraser, 2003: WMO 2002. Scientific assessment of ozone depletion 2002, World meteorological Organisation, Geneva, Switzerland.

    Google Scholar 

  • NASA, 1994: Report on concentrations, lifetimes, and trends of CFCs, halons, and related species, NASA Reference Publication 1339, Washington, D.C.

  • O'Doherty, S., Simmonds, P. G., Cunnold, D. M., Wang, H. J., Sturrock, G. A., Fraser, P. J., Ryall, D., Derwent, R. G., Weiss, R. F., Salameh, P., Miller, B. R., and Prinn, R. G., 2001: In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998, J. Geophys. Res. 106, 20429–20444.

    Google Scholar 

  • Prinn, R. G., Weiss, R. F., Fraser, P. J., Simmonds, P. G., Cunnold, D. M., Alyea, F. N., O'Doherty, S., Salameh, P., Miller, B. R., Huang, J., Wang, H. J., Hartley D. E., Harth, C., Steele, L. P., Sturrock, G., Midgley, P. M., and McCulloch, A., 2000: A history of chemically and radiatively important gases in air deduced from ALE/GAGE/AGAGE, J. Geophys. Res. 105, 17751–17792.

    Article  Google Scholar 

  • Prinn, R. G., Huang, J., Weiss, R. F., Cunnold, D. M., Fraser, P. J., Simmonds, P. G., McCulloch, A., Harth, C., Salameh, P., O'Doherty, S., Wang, H. J., Porter, L., and Miller, B. R., 2001: Evidence for substantial variations of atmospheric hydroxyl radicals in the past two decades, Science 292, 1882–1888.

    Article  Google Scholar 

  • Rhew, R. C., Miller, B. R., and Weiss, R. F., 2000: Natural methyl bromide and methyl chloride emissions from coastal salt marshes, Nature 403, 292–295.

    Article  Google Scholar 

  • Rhew, R. C., Miller, B. R., Vollmer, M. K., and Weiss, R. F., 2001: Schrubland fluxes of methyl bromide and methyl chloride, J. Geophys. Res. 106, 20875–20882.

    Article  Google Scholar 

  • Ryall, D. B., Maryon, R. H., Derwent, R. G., and Simmonds, P. G., 1998: Modelling long-range transport of CFCs to Mace Head, Ireland, Quart. J. Roy. Meteorol. Soc. 124, 417–446.

    Article  Google Scholar 

  • Sawa, Y., Matsueda, H., Tsutsumi, Y., Jensen, J. B., Inoue, Y., and Makino, Y., 1999: Tropospheric carbon monoxide and hydrogen measurements over Kalimantan in Indonesia and northern Australia during October 1997, Geophys. Res. Lett. 26, 1389–1392.

    Article  Google Scholar 

  • Serca, D., Guenther, A., Klinger, L., Helmig, D., Hereid, D., and Zimmerman, P., 1998: Methyl bromide deposition to soils, Atmos. Environ. 32, 1581–1586.

    Google Scholar 

  • Shorter, J. H., Kolb, C. E., Crill, P.M., Kerwin, R. A., Talbot, R. W., Hines, M. E., and Harriss, R. C., 1995: Rapid degradation of atmospheric bromide in soils, Nature 377, 717–719.

    Article  Google Scholar 

  • Simmonds, P. G., O'Doherty, S., Nickless, G., Sturrock, G. A., Swaby, R., Knight, P., Ricketts, J., Woffendin, G., and Smith, R., 1995: Automated gas chromatograph-mass spectrometer for routine atmospheric field measurements of the CFC replacement compounds, the hydrofluorocarbons and hydrochlorofluorocarbons, Anal. Chem. 34, 717–723.

    Google Scholar 

  • Simmonds, P. G., Seuring, S., Nickless, G., and Derwent, R. G., 1997: Segration and interpretation of ozone and carbon monoxide measurements by air mass origin at the TOR station, Mace Head, Ireland from 1987 to 1995, J. Atmos. Chem. 28, 45–59.

    Article  Google Scholar 

  • Simmonds, P. G., Derwent, R. G., O'Doherty, S., Ryall, D. B., Steele, L. P., Langenfelds, R. L., Salameh, P., Wang, H. J., Dimmer, C. H., and Hudson, L. E., 2000: Continuous high-frequency observations of hydrogen at the Mace Head baseline atmospheric monitoring station over the period 1994–1998, J. Geophys. Res. 105, 12105–12121.

    Article  Google Scholar 

  • Sturrock, G. A., Porter, L., and Fraser, P. J., 2001: In situ measurements of CFC replacement chemicals and other halocarbons at Cape Grim: The AGAGE GC-MS program, in N. W. Tindale, R. J. Francey, and N. Derek (eds), Baseline Atmospheric Program (Australia) 1997–1998, Bureau of Meteorology and CSIRO Atmospheric Research, Melbourne, Australia, pp. 43–49.

    Google Scholar 

  • Thoning, K. W., Tans, P. P., and Komhyr, W. D., 1989: Atmospheric carbon dioxide at Mauna Loa Observatory, 2, Analysis of NOAA/GMCC data, 1974–1985, J. Geophys. Res. 94, 8549–8565.

    Google Scholar 

  • Tokarczyk, R., Goodwin, K. D., and Saltzman E. S., 2003: Methyl chloride and methyl bromide degradation in the Southern Ocean, Geophys. Res. Lett. 30(15), 1808, doi:10.1029/2003GL017459.

    Article  Google Scholar 

  • UN ECE, 2002: Present state of emission data, EB.AIR/GE.1/2002/8, United Nations Economic Commission for Europe, Geneva, Switzerland.

    Google Scholar 

  • UNEP, 2002: Production and consumption of ozone depleting substances under the Montreal Protocol, Ozone Secretariat, Nairobi, Kenya, p. 71, April 2002.

    Google Scholar 

  • UNEP, 2003: Handbook for the International Treaties for the Protection of the Ozone Layer, 6th edn, Nairobi, Kenya.

  • Varner, R. K., Crill, P. M., and Talbot, R. W., 1999: Wetlands: A potentially significant source of atmospheric methyl bromide and methyl chloride, Geophys. Res. Lett. 26, 2433–2435.

    Google Scholar 

  • Wingenter, O. W., Wang, C. J. L., Blake, D. R., and Rowland, F. S., 1998: Seasonal variation of tropospheric methyl bromide concentrations: Constraints on anthropogenic input, Geophys. Res. Lett, 25, 2797–2800.

    Article  Google Scholar 

  • Yokouchi, Y., Nojiri, Y., Barrie, L. A., Toom-Sauntry, D., Machida, T., Inuzuka, Y., Akimoto, H., Li, H. J., Fuginuma, Y., and Aoki, S., 2000a: A strong source of methyl chloride to the atmosphere from tropical coastal land, Nature 403, 29–298.

    Article  Google Scholar 

  • Yokouchi, Y., Machida, T., Barrie, L. A., Toom-Sauntry, D., Nojiri, Y., Fujinuma, Y., Inuzka, Y., Li, H. J., Akimoto, H., and Aoki, S., 2000b: Latitudinal distribution of atmospheric methyl bromide: Measurements and modelling, Geophys. Res. Lett, 27, 697–700.

    Article  Google Scholar 

  • Yokouchi, Y., Ikeda, M., Inuzuka, Y., and Yukawa, T., 2002a: Strong emissions of methyl chloride from tropical plants, Nature 416, 163–165.

    Article  Google Scholar 

  • Yokouchi, Y., Toom-Sauntry, D., Yazawa, K., Inagaki, T., and Tamaru, T., 2002b: Recent decline of methyl bromide in the troposphere, Atmos. Environ. 36, 4985–4989.

    Article  Google Scholar 

  • Yvon-Lewis, S. A., 2000: Methyl bromide in the atmosphere and ocean, IGACtivities, Newsletter, 9–12.

Download references

Author information

Authors and Affiliations

  1. School of Chemistry, University of Bristol, Cantock's Close, Bristol, BS8 1TS, U.K.

    P. G. Simmonds & S. O'Doherty

  2. Climate Research, Meteorological Office, Bracknell, U.K.

    R. G. Derwent, A. J. Manning & D. B. Ryall

  3. Atmospheric Research, CSIRO, Melbourne, Victoria, Australia

    P. J. Fraser & P. B. Krummel

  4. School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, U.S.A.

    D. M. Cunnold & H. J. Wang

  5. Scripps Institution of Oceanography, University of California at San Diego, La Jolla, California, U.S.A.

    B. R. Miller, R. F. Weiss & P. K. Salameh

  6. Cape Grim Baseline Air Pollution Monitoring Station, Bureau of Meteorology, Smithton, Tasmania, Australia

    R. G. Prinn & L. W. Porter

Authors
  1. P. G. Simmonds
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. R. G. Derwent
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. A. J. Manning
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. P. J. Fraser
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. P. B. Krummel
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. S. O'Doherty
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. R. G. Prinn
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. D. M. Cunnold
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. B. R. Miller
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. H. J. Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. D. B. Ryall
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. L. W. Porter
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. R. F. Weiss
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. P. K. Salameh
    View author publications

    You can also search for this author in PubMed Google Scholar

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Simmonds, P.G., Derwent, R.G., Manning, A.J. et al. AGAGE Observations of Methyl Bromide and Methyl Chloride at Mace Head, Ireland, and Cape Grim, Tasmania, 1998–2001. Journal of Atmospheric Chemistry 47, 243–269 (2004). https://doi.org/10.1023/B:JOCH.0000021136.52340.9c

Download citation

  • Issue Date:

  • DOI: https://doi.org/10.1023/B:JOCH.0000021136.52340.9c

search

Navigation