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EMEP Assessment Report: French National Contribution 1

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EMEP Assessment Report: French National Contribution 1 EMEP Assessment Report: French national contribution P. Coddeville, B. Oudart, N. Poisson, M. Rico, L. Rouïl 1°/ Precipitations, atmospheric concentrations and emissions: 1a/ Measurements: French EMEP/MERA monitoring network description The French contribution to the EMEP program includes 8 measurement stations integrated in a national monitoring network called MERA (MEsure des Retombées Atmosphériques). The map below shows their locations. REVIN (390 m) LA HAGUE (133 m) DONON (775 m) MORVAN (620 m) MONTANDON LA TARDIERE (836 m) (143 m) BONNEVAUX LA CROUZILLE (836 m) (497 m) LE CASSET PEYRUSSE VIEILLE (1 750 m) (200 m) IRATY (1 300 m) EMEP stations remote stations Equipment implemented at these stations allows getting information on a daily basis about precipitation amount, major ions in precipitation, sulphur dioxide and sulphate aerosols. Since 1998, EMEP/MERA stations (except La Crouzille and La Hague) have been equipped with ozone analysers and meteorological apparatus. Moreover, the measurement of volatile organic compounds (VOC) and carbonyls have been set up at Donon and Peyrusse-Vieille (EMEP super site) stations since 1992 and 1995 respectively. The table below summarises the list of pollutants measured at each French EMEP station, and the date of first measurements: 86 EMEP Assessment Report – Part II (1) (2) Station precipitation SO2 S (part) O3 VOC carbonyls meteorology EMEP stations Bonnevaux (3) 01/1990 01/1990 01/1990 01/1995 Donon 01/1990 01/1990 01/1990 09/1988 09/1992 06/1993 09/1988 Iraty 01/1990 01/1990 01/1990 03/1998 01/2000 La Crouzille 01/1978 01/1978 01/1978 La Hague 01/1978 01/1978 01/1978 Montandon 03/1998 03/1998 03/1998 04/1998 09/1998 Morvan 01/1990 01/1990 01/1990 01/1998 11/1998 Peyrusse-Vieille 01/1995 01/1995 01/1995 01/1995 07/1999 04/2000 02/1999 Revin 01/1990 01/1990 01/1990 01/1990 03/1999 Remote national stations Le Casset 01/1990 01/1990 01/1990 01/1997 09/1998 La Tardière 07/2001 07/2001 07/2001 07/2001 07/2001 06/2002 07/2001 - - 2- + 2+ + + 2+ (1) pH, conductivity, Cl , NO3 , SO4 , Na , Ca , K , NH4 , Mg (2) pressure, temperature, Humidity, precipitation amount, wind, solar radiation (3) Stopped in 1998 Behaviour and trends of measured pollutants (precipitation, SO2, Spart, VOC): Sulphur compounds in air and aerosol SO2 in air The concentrations of sulphur dioxide have significantly declined during the nineties, reflecting the decreasing of SO2 emissions in France and in Europe. This significant trend is very similar for all French EMEP stations and more particularly for the two oldest stations La Hague and La Crouzille started in 1978. The annual mean concentrations were between 2.5 – 8 µg.m-3 in the eighties and dropped to 0.2 – 1 µg.m-3 in the nineties. With the same sampling method it must be noted that the number of values below the analytical detection limit is increasing at most of the French sites. The maximum monthly mean concentrations were generally recorded in winter but some maximum values have been observed in spring or in summer. The highest concentrations were observed in the Northeast of France. A study showed that these maxima occurred with air mass trajectories coming from central Europe for the eastern stations and South Europe for the southern stations. Sulphate in aerosol The concentrations of sulphate in aerosols declined in the nineties but not as significantly as -3 that of SO2. The annual mean concentration amounted to 1 – 1,2 µg.m at the beginning of nineties and to 0,4 – 0,6 µg.m-3 at the end. The annual variations were not prominent. The decrease in emissions of sulphur in Western Europe from 1980 onwards has resulted in much larger decreases in observed concentrations of SO2 in ambient air compared to the decrease in ambient SO4 aerosol concentrations. This result confirms the non-linearity between these two sulphur compounds identified by several authors. Precipitation The annual amount of precipitation in France ranges between 600 and 2300 mm, the maximum heights are regularly recorded in the Northeast of France but the amounts and intensity of precipitation time and spatial variations play an important role. Contribution from: France 87 The average pH for the nineties (see below) stood at 5.0 and the annual averages fluctuated between 4.7 and 5.5 according to the stations. The last five years of nineties were more acidic particularly in 1996 and 1998. The H+ deposition was about 10 mg/m²/yr and fluctuated between 5 and 25 mg/m²/yr. Higher concentrations and deposition tended to occur in the East and the North of France. A slight increase of H+ deposition (calculated for 100 mm rainwater) has been observed for the last five years of nineties and more particularly for the Northeast sites. In rainwater, the nitrate concentrations did not vary strongly according the years, about 0.2-0.3 mgN/L. Nevertheless, a weak decrease was noted. Maximum concentrations and deposition (10 to 400 mgN/m²/year) were clearly situated in the North of France. The variations of ammonium concentrations were more pronounced, between 0.3 (at the present time) and 0.7 mgN/L (in the early nineties). The centre part of the North of France was also more exposed and deposition varied between 150 to 600 mgN/m²/year. About sulphates in precipitation, the concentrations have decreased slowly since the beginning of nineties (0.6 to 0.4 mgS/L). These concentrations have been very stable for 4-5 years like the emissions. As indicators of a marine influence, the sodium and chloride concentrations and deposition are higher near the sea. They were extremely variable depending on the site and the year. The indicators of terrestrial dust, calcium, magnesium and potassium did not vary according to longitude and latitude. No clear trend was shown either for annual concentrations or deposition. Nevertheless, a larger frequency of Saharan events that lead to calcium depositions was observed. 1,4 1600 DONON DONON IRATY IRATY 1400 1,2 MORVAN MORVAN REVIN REVIN 1200 1 1000 0,8 800 [NH4] mgN/L 0,6 Dépôt NH4 mgN/m²/an 600 0,4 400 0,2 200 0 0 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 0,9 1200 DONON DONON IRATY 0,8 IRATY MORVAN MORVAN 1000 REVIN REVIN 0,7 0,6 800 0,5 600 0,4 [SO4] mgS/L [SO4] [SO4] mgN/m²/an [SO4] 0,3 400 0,2 200 0,1 0 0 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 0,8 700 DONON DONON IRATY IRATY MORVAN 600 MORVAN REVIN REVIN 0,6 500 400 0,4 _ mgN/L [NO3] 300 Dépôt NO3 mgN/m²/an 200 0,2 100 0 0 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Concentration and deposition in four French sites since 1990 for NH4, SO4 and NO3 88 EMEP Assessment Report – Part II Surface ozone Most of EMEP rural stations have been equipped in 1998. The ozone concentrations did not show any trend, but the ozone measurements at Donon and Revin, located in the eastern of France and started in 1995, could give a good idea of temporal variation. 60 1999 55 50 45 Brotonne 40 Iraty [O3] Donon 35 Le Casset ppb Montandon 30 Morvan 25 Peyrusse Revin 20 15 10 Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec O3 monthly mean concentration in 1999 The annual mean concentrations were between 25 and 45 ppb. No concentration gradients were clearly identified from North to South. The highest values were observed in the mountainous sites (Iraty, Le Casset). Pollution roses established for all sites could not define any major direction of pollution episodes in France, as the typologies of the sites are all different and characteristic of meteorological influences. In most cases the daily maximum values (between 90 and 100 ppb) were observed in the sites situated in flat areas and during the summer period (June to August). The diurnal course of surface ozone levels were characterised by a minimum early in the morning and a maximum around 2 p.m. Some maximum values were observed during the night at the high altitude sites. This diurnal course is a function of site altitude. The exceedances of the ambient air quality standard (55 ppb, 8 hours average) were rather frequent but the level requiring information to the public (90 ppb, one-hour average) has been exceeded only occasionally. No significant trends were observed at the French rural sites from the beginning of measurements. Inter-annual variability of ozone concentrations is assigned to the annual variation of photochemical activity. Volatile organic and carbonyl compounds VOCs started to be sampled in 1992 and the carbonyls in 1993 at Donon. The analyses were under the responsibility of NILU until 1996. Since 1997, the laboratory of the Ecole des Mines De Douai has carried out the analyses. A new station in the southern part of France was started in 1997 and a third in 2001 in the western part of the country. The concentrations were higher in the Mediterranean site by one order of magnitude varying from tenths of ppb up to several ppb. Among the VOCs measured the average volumetric composition is the following: alkanes 55%, alkenes 12%, aromatics 13%, alkynes 5%, isoprene 12%.
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