Abstract
The present study investigates the chemical composition of wet atmospheric precipitation samples on a daily and an intra-event timescales in Opme, an experimental meteorological station located near Clermont-Ferrand, France. The samples have been collected from November 2005 to October 2007. A total of 217 rainwater samples, integrated for 24 h, were collected and analyzed for pH, conductivity, Na+, K+, Mg2+, NH +4 , Ca2+, Cl−, NO −3 , SO 2−4 , PO 3−4 and HCO −3 . The composition of the rainwater collected appeared to be controlled by the following potential sources: neutralisation process (association among calcium, ammonium with nitrate and sulphate), marine and terrestrial sources. In order to determine the role of long-range transport, the integrated events were classified according to four origins of air-masses: (1) West, (2) North and East, (3) South including Iberian and Italian Peninsulae and (4) local. This analysis allows identifying the source areas of the different association of elements defined. Although calcium is always dominant, total content of rainfall is variable and neutralisation process can be more or less efficient and specific. Rainout (long-range transport) and washout (below-cloud scavenging) were investigated through intra-event measurements of chemical species. Four rain-events have been selected according to the four classes of origins of air-masses. It appears that the first fractions are responsible for an important part of the chemical content of the whole event. Terrestrial species, locally emitted, induce the neutralisation process of acid species. Local meteorological conditions, such as wind’s speed and direction, play an important role as they could provoke recharges of the below cloud air column during the event.
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Al-Momani, I.F., Ataman, O.Y., Anwar, M.A., Tuncel, S., Kös, C., Tuncel, G.: Chemical composition of precipitation near an industrial area at Izmir, Turkey. Atmos. Environ 29, 1131–1143 (1995). doi:10.1016/1352-2310(95)00027-V
Avila, A., Queralt-Mitjans, I., Alarcon, M.: Mineralogical composition of African dust delivered by red rains over northeastern Spain. J. Geophys. Res. 102(D18), 21, 977–996 (1997). doi:10.1029/97JD00485
Avila, A., Alarcon, M., Queralt-Mitjans, I.: The chemical composition of dust transported in red rains and its contribution to the biogeochemical cycle of a holm oak forest in Catalonia (Spain). Atmos. Environ. 32, 179–191 (1998). doi:10.1016/S1352-2310(97)00286-0
Avila, A., Alarcon, M.: Relationship between precipitation chemistry and meteorological situations at a rural site in N.E. Spain. Atmos. Environ. 33, 1663–1677 (1999). doi:10.1016/S1352-2310(98)00341-0
Berner, E., Berner, R.: The global water cycle. Prentice Hall, New Jersey (1987)
Beverland, I.J., Crowther, J.M., Srinivas, M.S.N., Heal, M.R.: The influence of meteorology and atmospheric transport patterns on the chemical composition of rainfall in south-east England. Atmos. Environ. 32, 1039–1048 (1998). doi:10.1016/S1352-2310(97)00365-8
Beysens, D., Ohayon, C., Muselli, M., Clus, O.: Chemical and biological characteristics of dew and rain water in an urban coastal area (Bordeaux, France). Atmos. Environ. 40, 3710–3723 (2006). doi:10.1016/j.atmosenv.2006.03.007
Bourrié, G.: Acquisition de la composition chimique des eaux en climat tempéré. Application aux granites des Vosges et de la Margeride. PhD Thesis, Université Louis Pasteur, Strasbourg (1978)
Brewer, P.G.: Chemical Oceanography Vol.1. Academic Press, New-York (1975)
Celle, H.: Caractérisation des précipitations sur le pourtour de la Méditerranée occidentale. Approche isotopique et chimique. PhD Thesis, Université Avignon et Pays de Vaucluse (2000)
Celle-Jeanton, H., Gonfiantini, R., Travi, Y., Sol, B.: Oxygen-18 variations of rainwater during precipitation: application of the Rayleigh model to selected rainfalls in Southern France. J. Hydrol. (Amst.) 289, 165–177 (2004). doi:10.1016/j.jhydrol.2003.11.017
Celle-Jeanton, H., Travi, Y., Loye-Pilot, M.D., Huneau, F., Bertrand, G.: Rainwater chemistry at a Mediterranean inland station (Avignon, France): local contribution versus long range supply. Atmos. Res. 91, 118–126 (2009). doi:10.1016/j.atmosres.2008.06.003
Chate, D.M., Kamra, A.K.: Collection efficiencies of large water drops collecting aerosol particles of various densities. Atmos. Environ. 31, 1631–1635 (1997). doi:10.1016/S1352-2310(96)00338-X
Chate, D.M., Rao, P.S.P., Naik, M.S., Momin, G.A., Safai, P.D., Ali, K.: Scavenging of aerosols and their chemical species by rain. Atmos. Environ. 37, 2477–2484 (2003). doi:10.1016/S1352-2310(03)00162-6
Cyrys, J., Gutschmidt, K., Brauer, M., Dumyahn, T., Heinrich, J., Spengler, J.D., Wichmann, H.E.: Determination of acidic sulfate aerosols in urban atmospheres in Erfurt (F.R.G.) and Sokolov (Former C.S.S.R). Atmos. Environ. 29, 3545–3557 (1995). doi:10.1016/1352-2310(95)00133-J
Diaz-Caneja, N., Bonet, A., Gutierrez, I., Martinez, A., Villar, E.: The chemical composition of rainfall in a city of northern Spain. Water Air Soil Pollut. 43, 277–291 (1989)
Durana, N., Casado, H., Ezcurra, A., Garcia, C., Lacaux, J.P.: Pham Van Dinh: experimental study of the scavenging process by means of a sequential precipitation collector, preliminary results. Atmos. Environ. 26A(13), 2437–2443 (1992)
Draxler, R.R., Rolph, G.D.: HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) Model access via NOAA ARL READY Website (http://www.arl.noaa.gov/ ready/hysplit4.html). NOAA Air Resources Laboratory, Silver Spring, MD (2003)
Ezcurra, A., Casado, H., Lacaux, J.P., Garcia, C.: Relationship between meteorological situations and acid rain in Spanish Basque country. Atmos. Environ. 22, 2779–2786 (1988). doi:10.1016/0004-6981(88)90445-3
Fowler, D., Smith, R.I., Muller, J.B.A., Hayman, G., Vincent, K.J.: Changes in the atmospheric deposition of acidifying compounds in the UK between 1986 and 2001. Environ. Pollut. 137, 15–25 (2005). doi:10.1016/j.envpol.2004.12.028
Finlayson-Pitts, B.J., Pitts, J.N.: Atmospheric chemistry-fundamentals and experimental techniques. Wiley, New-York (1986)
Germer, S., Neill, C., Krusche, A.V., Gouveia Neto, S.C., Elsenbeer, H.: Seasonal and within-event dynamics of rainfall and throughfall chemistry in an open tropical rainforest in Rondonia, Brazil. Biogeochemistry 86, 155–174 (2007). doi:10.1007/s10533-007-9152-9
Gonçalves, F.L.T., Ramos, A.M., Freitas, S., Silva Dias, M.A., Massambani, O.: In-cloud and below-cloud numerical simulation of scavenging processes at Serra do Mar Region, SE Brazil. Atmos. Environ. 36, 5245–5255 (2002). doi:10.1016/S1352–2310(02) 00461–2
Hicks, B.B., Shannon, J.D.: A method for modelling the deposition of sulphur by precipitation over regional scales. J. Appl. Meteorol. 18, 1415–1420 (1979). doi:10.1175/1520-0450(1979)018<1415:AMFMTD>2.0.CO;2
Hov, O., Hjollo, B.A.: Transport distance of ammonia and ammonium in northern Europe. Its relation to emissions of SO2, and NOx. J. Geophys. Res. 99, 749–755 (1994)
Huang, K., Zhuang, G., Xu, C., Wang, Y., Tang, A.: The chemistry of the severe acidic precipitation in Shanghai, China. Atmos. Res. 89, 149–160 (2008). doi:10.1016/j.atmosres.2008.01.006
INSEE: Recensement de mars 1999 de l’Institut National de la Statistique et des Etudes Economiques. www.recensement.insee.fr (1999). Accessed 20 June 2007
Jaffrezo, J.L., Colas, N., Bouchet, M.: Carboxylic acids measurements with ionic chromatography. Atmos. Environ. 32(14-15), 2705–2708 (1998). doi:10.1016/S1352-2310(98)00026-0
Junge, C.E.: Air chemistry and radioactivity. Academic, New-York (1963)
Khwaja, H.A., Husain, L.: Chemical characterization of acid precipitation in Albany. New York. Atmos. Environ. 24A, 1869–1882 (1990)
Lim, B., Jickells, T.D., Davies, T.D.: Sequential sampling of particles, major ions and total trace metals in wet deposition. Atmos. Environ. 25A(3–4), 745–762 (1991)
Meszaros, E.: Atmospheric chemistry. Fundamental aspects. Studies in Environmental Science 11. (1981)
Negrel, P., Roy, S.: Chemistry of rainwater in the Massif Central (France): a strontium isotope and major element study. Appl. Geochem. 13(8), 941–952 (1998). doi:10.1016/S0883-2927(98)00029-8
Pelicho, A.F., Martins, L.D., Nomi, S.N., Solci, M.C.: Integrated and sequential bulk and wet-only samplings of atmospheric precipitation in Londrina, South Brazil (1998–2002). Atmos. Environ. 40, 6827–6835 (2006). doi:10.1016/j.atmosenv.2006.05.075
Plaisance, H., Coddeville, P., Guillermo, R., Roussel, I.: Spatial variability and source identification of rural precipitation chemistry in France. Sci. Total Environ. 180, 257–270 (1996). doi:10.1016/0048-9697(95)04943-6
Plaisance, H., Galloo, J.C., Guillermo, R.: Source identification and variation in the chemical composition of precipitation at two rural sites in France. Sci. Total Environ. 206, 79–93 (1997). doi:10.1016/S0048-9697(97)00221-0
Rahn, K.A., Brosset, C., Ottar, B., Patterson, E.M.: Black and White episodes, chemical evolution of Eurasian air masses and long range transport of carbon into the Arctic. In: Wolff, T., Klimmish, R.L. (eds.) Particulate carbon: atmospheric life cycle, pp. 339–340. Plenum, New York (1982)
Rangognio, J.: Apport des mesures chimiques infra-événementielles dans la compréhension des mécanismes d’acquisition de la chimie des précipitations. Master Research Report, Université Clermont-Ferrand (2006)
Reade, L., Jennings, S.G., McSweeney, G.: Cloud condensation nuclei measurements at Mace Head, Ireland, over the period 1994–2002. Atmos. Res. 82, 610–621 (2006). doi:10.1016/j.atmosres.2006.02.017
Ricard, V., Jaffrezo, J.L., Kerminen, V.M., Hillamo, R.E., Sillanpaa, M., Ruellan, R., Liousse, C., Cachier, H.: Two years of continuous aerosol measurements in northern Finland. J. Geophys. Res. 107(D11), (2002)
Rolph, G.D.: Real-time Environmental Applications and Display sYstem (READY) Website (http://www.arl.noaa.gov/ready/hysplit4.html). NOAA Air Resources Laboratory, Silver Spring, MD (2003)
Saha, A., Moorthy, K.K.: Impact of precipitation on aerosol spectral optical depth and retrieved size distributions: a case study. J. Appl. Meteorol. 43, 902–914 (2004). doi:10.1175/1520-0450(2004)043<0902:IOPOAS>2.0.CO;2
Sanusi, A., Wortham, H., Millet, M., Mirabel, P.: Chemical composition of rainwater in eastern France. Atmos. Environ. 30(1), 59–71 (1996). doi:10.1016/1352-2310(95)00237-S
Seinfeld, J.H., Pandis, S.N.: Atmospheric chemistry and physics: from air pollution to climate change. Wiley, New York (1998)
Seymour, M.D., Stout, T.: Observations of the chemical composition of rain using a short sampling times during a single event. Atmos. Environ. 17(8), 1483–1487 (1983). doi:10.1016/0004-6981(83)90301-3
Simeonov, V., Kalina, M., Tsakovski, S., Puxbaum, H.: Multivariate statistical study of simultaneously monitored cloud water, aerosol and rainwater data from different elevation levels in an alpine valley (Achenkirch, Tyrol, Austria). Talanta 61, 519–528 (2003). doi:10.1016/S0039-9140(03)00311-4
Sisterson, D.L.: A method for evaluation of acidic sulphate and nitrate in precipitation. Water Air Soil Pollut. 43, 61–72 (1989). doi:10.1007/BF00175583
Tost, H., Jöckel, P., Kerkweg, A., Pozzer, A., Sander, R., Lelieveld, J.: Global cloud and precipitation chemistry and wet deposition: tropospheric model simulations with ECHAM5/MESSy1. Atmos. Chem. Phys. 7, 2733–2757 (2007)
Zunckel, M., Saizar, C., Zarauz, J.: Rainwater composition in northeast Uruguay. Atmos. Environ. 37, 1601–1611 (2003). doi:10.1016/S1352-2310(03)00007-4
Aknowledgments
The authors thank the PREVOIR project financed by the Auvergne region for its material support and gratefully acknowledge the NOAA Air Resources Laboratory (ARL) for the provision of the HYSPLIT transport and dispersion model and/or READY website (http://www.arl.noaa.gov/ready.html) used in this publication.
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Bertrand, G., Celle-Jeanton, H., Laj, P. et al. Rainfall chemistry: long range transport versus below cloud scavenging. A two-year study at an inland station (Opme, France). J Atmos Chem 60, 253–271 (2008). https://doi.org/10.1007/s10874-009-9120-y
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DOI: https://doi.org/10.1007/s10874-009-9120-y