Measurements of atmospheric mercury species at a German rural background site from 2009 to 2011 – methods and results
Andreas Weigelt A , Christian Temme B , Elke Bieber C , Andreas Schwerin C , Maik Schuetze C , Ralf Ebinghaus A D and Hans Herbert Kock AA Helmholtz-Zentrum Geesthacht, Institute of Coastal Research, Max-Planck-Strasse 1, D-21502 Geesthacht, Germany.
B Eurofins GfA GmbH, Neulaender Kamp 1, D-21079 Hamburg, Germany.
C Federal Environment Agency, Air Pollution Monitoring Network, Paul-Ehrlich-Strasse 29, D-63225 Langen, Germany.
D Corresponding author. Email: ralf.ebinghaus@hzg.de
Environmental Chemistry 10(2) 102-110 https://doi.org/10.1071/EN12107
Submitted: 24 July 2012 Accepted: 25 February 2013 Published: 2 May 2013
Environmental context. Mercury is a very hazardous substance for human and environmental health. Systematic long-term direct measurements in the atmosphere can provide valuable information about the effect of emission controls on the global budget of atmospheric mercury, and offer insight into source–receptor transboundary transport of mercury. A complete setup for the measurement of the four most relevant atmospheric mercury species (total gaseous mercury, gaseous oxidised mercury, particle-bound mercury, and gaseous elemental mercury) has been operating at the rural background site of Waldhof, Germany, since 2009. We present the dataset for 2009–2011, the first full-speciation time series for atmospheric mercury reported in Central Europe.
Abstract. Measurements of mercury species started in 2009 at the air pollution monitoring site ‘Waldhof’ of the German Federal Environmental Agency. Waldhof (52°48′N, 10°45′E) is a rural background site located in the northern German lowlands in a flat terrain, 100 km south-east of Hamburg. The temporally highly resolved measurements of total gaseous mercury (TGM), gaseous oxidised mercury (GOM), particle-bound mercury (PBMPM2.5, with particulate matter of a diameter of ≤2.5 µm) and gaseous elemental mercury (GEM) cover the period from 2009 to 2011. The complete measurement procedure turned out to be well applicable to detect GOM and PBMPM2.5 levels in the range of 0.4 to 65 pg m–3. As the linearity of the analyser was proven to be constant over orders of magnitude, even larger concentrations can be measured accurately. The 3-year median concentration of GEM is found to be 1.61 ng m–3, representing typical northern hemispheric background concentrations. With 6.3 pg m–3, the 3-year average concentration of PBMPM2.5 is found to be approximately six times higher than the 3-year average GOM concentration. During winter the PBMPM2.5 concentration is on average twice as high as the PBMPM2.5 summer concentration, whereas the GOM concentration shows no clear seasonality. However, on a comparatively low level, a significant diurnal cycle is shown for GOM concentrations. This cycle is most likely related to photochemical oxidation mechanisms. Comparison with selected North American long-term mercury speciation datasets shows that the Waldhof 3-year median speciated mercury data represent typical rural background values.
References
[1] O. Lindqvist, K. Johansson, M. Aastrup, A. Andersson, L. Bringmark, G. Hovsenius, L. Haakanson, A. Iverfeldt, M. Meili, B. Timm, Mercury in the Swedish environment – recent research on causes, consequences and corrective methods. Water Air Soil Pollut. 1992, 55, 1.[2] S. E. Lindberg, W. J. Stratton, Atmospheric mercury speciation: concentrations and behaviour of reactive gaseous mercury in ambient air. Environ. Sci. Technol. 1998, 32, 49.
| Atmospheric mercury speciation: concentrations and behaviour of reactive gaseous mercury in ambient air.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK2sXnsFOmu7o%3D&md5=756d474477a1a1c9d12e1466afde95cbCAS |
[3] L. Poissant, M. Pilote, X. Xu, H. Zhang, C. Beauvais, Atmospheric mercury speciation and deposition in the Bay St Francois wetlands. J. Geophys. Res. – Atmos. 2004, 109, D11301.
[4] W.-H. Schroeder, J. Munthe, Atmospheric mercury – an overview. Atmos. Environ. 1998, 32, 809.
| Atmospheric mercury – an overview.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1cXivFOksbo%3D&md5=96a171fc437c2cc31c61b38c25f7d1e0CAS |
[5] S. E. Lindberg, T. P. Meyers, G. E. Taylor, R. R. Turner, W. H. Schroeder, Atmosphere–surface exchange of mercury in a forest: results of modeling and gradient approaches. J. Geophys. Res. 1992, 97, 2519.
| Atmosphere–surface exchange of mercury in a forest: results of modeling and gradient approaches.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK38Xitl2jsbo%3D&md5=8e7831cb4a6321853d1ae391314983eaCAS |
[6] O. R. Bullock, Modeling assessment of transport and deposition patterns of anthropogenic mercury air emissions in the United States and Canada. Sci. Total Environ. 2000, 259, 145.
| Modeling assessment of transport and deposition patterns of anthropogenic mercury air emissions in the United States and Canada.Crossref | GoogleScholarGoogle Scholar | 11032144PubMed |
[7] S. Lindberg, R. Bullock, R. Ebinghaus, D. Engstrom, X. Feng, W. Fitzgerald, N. Pirrone, E. M. Prestbo, C. Seigneur, A synthesis of progress and uncertainties in attributing the sources of mercury in deposition. Ambio 2007, 36, 19.
| A synthesis of progress and uncertainties in attributing the sources of mercury in deposition.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1cXksFSrsro%3D&md5=7f7cdbbf2fbdf6df72cf77dcf8cd1faaCAS | 17408188PubMed |
[8] Directive 2004/107/EC of the European Parliament and of the Council of 15 December 2004 relating to arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons in ambient air. Official Journal of the European Union 2005, 26.1.2005, L 23/3.
[9] EMEP monitoring strategy and measurement program 2004-2009. Available at http://www.unece.org/fileadmin/DAM/env/lrtap/emep/Monitoring%20Strategy_full.pdf (accessed 12 March 2013).
[10] R. Ebinghaus, S. G. Jennings, H. H. Kock, R. G. Derwent, A. J. Manning, T. G. Spain, Decreasing trends in total gaseous mercury in baseline air at Mace Head, Ireland from 1996 to 2009. Atmos. Environ. 2011, 45, 3475.
| Decreasing trends in total gaseous mercury in baseline air at Mace Head, Ireland from 1996 to 2009.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3MXmtlemt7s%3D&md5=3e5c4e8c007861a4feb78ea525edf3efCAS |
[11] CSN EN 15852. Ambient air quality – Standard method for the determination of total gaseous mercury 2010. Available at http://www.en-standard.eu/en-15852-ambient-air-quality-standard-method-for-the-determination-of-total-gaseous-mercury/ [Verified 14 January 2013].
[12] W. H. Schroeder, G. Keeler, H. H. Kock, P. Roussel, D. R. Schneeberger, F. Schaedlich, International field intercomparison of atmospheric mercury measurement methods. Water Air Soil Pollut. 1995, 80, 611.
| International field intercomparison of atmospheric mercury measurement methods.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK2MXnsVChtbo%3D&md5=21e01a195550ebc7d627e67718c5d201CAS |
[13] R. Ebinghaus, S. G. Jennings, W. H. Schroeder, T. Berg, T. Donaghy, J. Guntzel, C. Kenny, H. H. Kock, K. Kvietkus, W. Landing, T. Mühleck, J. Munthe, E. Prestbo, D. Schneeberger, F. Slemr, J. Sommar, A. Urba, D. Wallschläger, Z. Xiao, International field intercomparison measurements of atmospheric mercury species at Mace Head, Ireland. Atmos. Environ. 1999, 33, 3063.
| International field intercomparison measurements of atmospheric mercury species at Mace Head, Ireland.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXjtFSrtL0%3D&md5=514bb29e6126ec51ad74e3c9bcc257a8CAS |
[14] K. Aspmo, P.-A. Gauchard, A. Steffen, C. Temme, T. Berg, E. Bahlmann, C. Banic, A. Dommergue, R. Ebinghaus, C. Ferrari, N. Pirrone, F. Sprovieri, G. Wibetoe, Measurements of atmospheric mercury species during an international study of mercury depletion events at Ny-Alesund, Svalbard, spring 2003. How reproducible are our present methods? Atmos. Environ. 2005, 39, 7607.
| Measurements of atmospheric mercury species during an international study of mercury depletion events at Ny-Alesund, Svalbard, spring 2003. How reproducible are our present methods?Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXht1agsLvE&md5=2831645df97ef78a408084d2071d6050CAS |
[15] C. Temme, R. Ebinghaus, H. H. Kock, A. Schwerin, E. Bieber, Field intercomparison of mercury measurements within EMEP, in EMEP/CCC-Report 4/2006, 10–22 2006. Available at http://www.nilu.no/data/inc/leverfil.cfm?id=19603&type=6 [Verified 12 March 2013].
[16] ISO 20988. Air quality – guidelines for estimating measurement uncertainty 2007. Available at http://www.iso.org/iso/catalogue_detail.htm?csnumber=35605 [Verified 5 April 2013].
[17] X. Faïn, H. Moosmüller, D. Obrist, Toward real-time measurement of atmospheric mercury concentrations using cavity ring-down spectroscopy. Atmos. Chem. Phys. 2010, 10, 2879.
| Toward real-time measurement of atmospheric mercury concentrations using cavity ring-down spectroscopy.Crossref | GoogleScholarGoogle Scholar |
[18] J. H. Seinfeld, S. N. Pandis, Atmospheric Chemistry and Physics: From Air Pollution to Climate Change 1998, pp. 766–775 (Wiley: New York).
