Causes of high PM 10 values measured in Denmark in 2006

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Causes of high PM 1 values measured in Denmark in 26 Peter Wåhlin and Finn Palmgren Department of Atmospheric Environment National Environmental Research Institute Århus University Denmark Prepared 2 October 28. Background The limit value for 24-hour average concentration on 5 µg/m 3 not to be exceeded more than 35 times per year is exceeded more than 35 times in some busy urban streets in Denmark. In order to select efficient measures it is necessary to identify the most important causes of high 24-hour PM1 concentrations. Analysis The monitoring data from air quality monitoring stations from 26 have been analysed in relation to annual variation and meteorology. A detailed analysis for Copenhagen uses the concurrently measured PM 1 values in 26 (28 days) at the kerbside station and at the roof station. The average during the 28 days was 4.7 µg/m 3 at, and 26.5 µg/m 3 at. An analysis of PM 1 measured with high time resolution (TEOM monitor) shows that the local traffic signal at in average is 16 % (.16) of the signal at. The best estimate for the local traffic contribution PM 1_TRAF at is therefore (PM 1_ PM 1_ )/(1-.16). The non-traffic background is calculated as the rest of the PM 1 at (PM 1_ PM 1_TRAF ). All available measurements are shown in figure 1. The full-drawn red line indicates the 5 µg/m 3 exceedance limit. The dotted red line is a 1:1 line, where the points below the line represent days with the highest background contributions and the points above the line represent highest local traffic contributions. The limit is exceeded in 24 % of the 28 days, corresponding to 88 days, if all 365 measurements were available. In 14 % of the 28 days it is mostly due to high background values, in 1 % it is mostly due to the local traffic. The data are grouped according to the seasons. The exceedances related to traffic take mainly place in late winter, January-March, which indicate significant contributions from road salt for de-icing.

PM1_TRAF = (PM1_ - PM1_)/.84 (µgm -3 ) 8 7 6 5 4 3 2 1-1 -2 76 % 1 % 14 % 2 4 6 8 1 PM1_BACKGR = PM1_ - PM1_TRAF (µgm -3 ) Jan-Mar Apr-Jun Jul-Sep Oct-Dec Figure 1. Local traffic contribution versus background contributions to PM 1 at H.C. Andersen Boulevard in Copenhagen, 26. The data are grouped in the seasons Jan.-Mar., Apr. Jun., Jul.-Sep. and Oct.-Dec. The exceedances related to background take place during all seasons. In order to distinguish between local and regional background we have investigated the correlation between the PM 1 concentrations at several street station (,, and in Denmark and an urban background in Copenhagen () and two regional background stations ( and ) in Denmark. The locations of the stations are shown in figure 2.

Figure 2. The position of the sites,,,,, and. The map is generated using MapSource (Garmin Ltd.) The figures 3a-3f show the measured values of PM 1 at the four kerbside stations,,, and, where the limit values were exceeded in 26 (reddish colours). Also shown (bluish colours) are the PM 1 at the three background sites, and. The LR label indicates days with high PM 1 values at the kerbside stations when the background level in Denmark was increased due to transboundary transport of PM. The transport was mostly from continental Europe (especially the eastern part), which can be seen by the air mass trajectories (figures 5a and 5b) calculated for one of the days (at noon) in each of the different episodes. The S label indicates a frost period in March when road salting was probably the main reason for high PM 1 values. Road salting is usual in Denmark in the winter, also in periods with temperatures around the freezing point. The air temperature in Copenhagen () during 26 is shown in figure 4. A longer frost period occurred in March in the period when we had many exceedances, which was traffic related probably due to de-icing of the roads.

15 1 5 1-1-26 2-1-26 3-1-26 4-1-26 5-1-26 6-1-26 7-1-26 8-1-26 9-1-26 1-1-26 11-1-26 12-1-26 13-1-26 14-1-26 15-1-26 16-1-26 17-1-26 18-1-26 19-1-26 2-1-26 21-1-26 22-1-26 23-1-26 24-1-26 25-1-26 26-1-26 27-1-26 28-1-26 29-1-26 3-1-26 31-1-26 PM1 (µgm -3 ) LR LR LR LR LR LR LR LR LR 15 1 5 1-2-26 2-2-26 3-2-26 4-2-26 5-2-26 6-2-26 7-2-26 8-2-26 9-2-26 1-2-26 11-2-26 12-2-26 13-2-26 14-2-26 15-2-26 16-2-26 17-2-26 18-2-26 19-2-26 2-2-26 21-2-26 22-2-26 23-2-26 24-2-26 25-2-26 26-2-26 27-2-26 28-2-26 PM1 (µgm -3 ) LR LR LR LR LR LR LR Figure 3a. PM 1 January and February 26.

15 1 5 1-3-26 2-3-26 3-3-26 4-3-26 5-3-26 6-3-26 7-3-26 8-3-26 9-3-26 1-3-26 11-3-26 12-3-26 13-3-26 14-3-26 15-3-26 16-3-26 17-3-26 18-3-26 19-3-26 2-3-26 21-3-26 22-3-26 23-3-26 24-3-26 25-3-26 26-3-26 27-3-26 28-3-26 29-3-26 3-3-26 31-3-26 PM1 (µgm -3 ) S S S S S S LR S L S S S S S S S S 15 1 5 1-4-26 2-4-26 3-4-26 4-4-26 5-4-26 6-4-26 7-4-26 8-4-26 9-4-26 1-4-26 11-4-26 12-4-26 13-4-26 14-4-26 15-4-26 16-4-26 17-4-26 18-4-26 19-4-26 2-4-26 21-4-26 22-4-26 23-4-26 24-4-26 25-4-26 26-4-26 27-4-26 28-4-26 29-4-26 3-4-26 PM1 (µgm -3 ) LR LR LR LR LR LR Figure 3b. PM 1 March and April 26

15 1 5 1-5-26 2-5-26 3-5-26 4-5-26 5-5-26 6-5-26 7-5-26 8-5-26 9-5-26 1-5-26 11-5-26 12-5-26 13-5-26 14-5-26 15-5-26 16-5-26 17-5-26 18-5-26 19-5-26 2-5-26 21-5-26 22-5-26 23-5-26 24-5-26 25-5-26 26-5-26 27-5-26 28-5-26 29-5-26 3-5-26 31-5-26 PM1 (µgm -3 ) LR LR LR LR LR LR LR 15 1 5 1-6-26 2-6-26 3-6-26 4-6-26 5-6-26 6-6-26 7-6-26 8-6-26 9-6-26 1-6-26 11-6-26 12-6-26 13-6-26 14-6-26 15-6-26 16-6-26 17-6-26 18-6-26 19-6-26 2-6-26 21-6-26 22-6-26 23-6-26 24-6-26 25-6-26 26-6-26 27-6-26 28-6-26 29-6-26 3-6-26 PM1 (µgm -3 ) LR LR LR LR LR LR LR LR LR LR LR Figure 3c. PM 1 May and June 26.

15 1 5 1-7-26 2-7-26 3-7-26 4-7-26 5-7-26 6-7-26 7-7-26 8-7-26 9-7-26 1-7-26 11-7-26 12-7-26 13-7-26 14-7-26 15-7-26 16-7-26 17-7-26 18-7-26 19-7-26 2-7-26 21-7-26 22-7-26 23-7-26 24-7-26 25-7-26 26-7-26 27-7-26 28-7-26 29-7-26 3-7-26 31-7-26 PM1 (µgm -3 ) LR LR LR LR LR LR LR LR LR LR L LR LR LR LR 15 1 5 1-8-26 2-8-26 3-8-26 4-8-26 5-8-26 6-8-26 7-8-26 8-8-26 9-8-26 1-8-26 11-8-26 12-8-26 13-8-26 14-8-26 15-8-26 16-8-26 17-8-26 18-8-26 19-8-26 2-8-26 21-8-26 22-8-26 23-8-26 24-8-26 25-8-26 26-8-26 27-8-26 28-8-26 29-8-26 3-8-26 31-8-26 PM1 (µgm -3 ) Figure 3d. PM 1 July and August 26

15 1 5 1-9-26 2-9-26 3-9-26 4-9-26 5-9-26 6-9-26 7-9-26 8-9-26 9-9-26 1-9-26 11-9-26 12-9-26 13-9-26 14-9-26 15-9-26 16-9-26 17-9-26 18-9-26 19-9-26 2-9-26 21-9-26 22-9-26 23-9-26 24-9-26 25-9-26 26-9-26 27-9-26 28-9-26 29-9-26 3-9-26 PM1 (µgm -3 ) LR LR LR LR LR LR LR LR LR LR LR LR LR LR LR LR LR LR 15 1 5 1-1-26 2-1-26 3-1-26 4-1-26 5-1-26 6-1-26 7-1-26 8-1-26 9-1-26 1-1-26 11-1-26 12-1-26 13-1-26 14-1-26 15-1-26 16-1-26 17-1-26 18-1-26 19-1-26 2-1-26 21-1-26 22-1-26 23-1-26 24-1-26 25-1-26 26-1-26 27-1-26 28-1-26 29-1-26 3-1-26 31-1-26 PM1 (µgm -3 ) LR LR LR LR LR LR Figure 3e. PM 1 September and October 26

15 1 5 1-11-26 2-11-26 3-11-26 4-11-26 5-11-26 6-11-26 7-11-26 8-11-26 9-11-26 1-11-26 11-11-26 12-11-26 13-11-26 14-11-26 15-11-26 16-11-26 17-11-26 18-11-26 19-11-26 2-11-26 21-11-26 22-11-26 23-11-26 24-11-26 25-11-26 26-11-26 27-11-26 28-11-26 29-11-26 3-11-26 PM1 (µgm -3 ) LR L LR LR 15 1 5 1-12-26 2-12-26 3-12-26 4-12-26 5-12-26 6-12-26 7-12-26 8-12-26 9-12-26 1-12-26 11-12-26 12-12-26 13-12-26 14-12-26 15-12-26 16-12-26 17-12-26 18-12-26 19-12-26 2-12-26 21-12-26 22-12-26 23-12-26 24-12-26 25-12-26 26-12-26 27-12-26 28-12-26 29-12-26 3-12-26 31-12-26 PM1 (µgm -3 ) Figure 3f. PM 1 November and December 26.

Ambient temperature (centigrades) 3 25 2 15 1 5-5 -1 1-1-6 1-2-6 1-3-6 1-4-6 1-5-6 1-6-6 1-7-6 1-8-6 1-9-6 1-1-6 1-11-6 Figure 4. Daily average temperature in Copenhagen () during 26. 1-12-6 The air mass trajectories are calculated using the Flextra model developed by Andreas Stohl (NILU) in cooperation with Gerhard Wotawa og Petra Seibert (Institute of Meteorology and Geophysics, Wienna) and using meteorological data provided from ECMWF (European Centre for Medium Range Weather Forcast). Selected trajectories are shown in Figure 5a-5b. There are 3 trajectories in each plot with three different heights at arrival in Copenhagen (small triangle indicates arrival close to the ground). Height along the trajectories is indicated by colour (red: low, blue: high). Each 3-hour interval along the trajectory path is indicated by a small legend, each 24-hour interval by a big legend. All selected trajectories show possible transport from the southern directions between east and southwest, most pronounced in January and May when transport took place from Poland, the Baltic countries and Germany.

916 1616 2416 1526 936 2346 556 1156 1366 Figure 5a.

266 2566 676 2176 2876 1496 1216 1816 28116 Figure 5b. Discussion and conclusions The analysis showed that in 26 two types of exceedance situations in relation to the 24-hour limit value were especially pronounced, one related to local traffic and one related to background pollution. Many traffic related situations took place in winter, when de-icing of the roads are necessary. We observed these exceedance situations in all investigated cities. The background related situations took place when long-range (transboundary) transport was likely. We found especially high concentration at street stations as well as at background stations. Trajectories confirmed that transport was from continental

European sectors between east and southwest. The background part of PM 1 during these situations was typically between 7 % and 9 % and in many cases above 1 % of the 24-hour limit value 5 µg/m 3. When the air came from the northern sectors (Sweden and Norway) the background values were much lower (around 1 µgm -3 ). This means that the background level is highly influenced by long-range transport, and that it is not possible by local measures to remove this type of exceedances. A few exceedance situations could not clearly be related to these types. They could be special local episodes or combinations of regional and local pollution. A few episodes with contribution from re-suspension of dust from the roads occurred probably in dry periods, e.g. in August, where we observed high traffic contributions in all cities. Pollen and other material from the vegetation that has deposited on the roadway have probably also contributed to re-suspended dust in the period May-October. In the early winter (November-December), after the pollen season and before the road salting season, there were very few exceedances that can be related to traffic.