Abstract
Size-segregated high-volume (HV) quartz filter samples were collected daily at the Melpitz rural site in Germany for PM10 (November 1992 until April 2012), and for PM2.5 and PM1 (January 2003 until April 2012, PM1 sampled every sixth day). The samples were analysed for mass concentration (gravimetrically), water-soluble ions (ion-chromatography) and since 2003 for organic carbon (OC) and elemental carbon (EC) (thermography). The long-term measurements first show a decreasing trend for PM10 (1993–2000) followed by a second period (2001–2011) with a mean mass concentration of about 22.4 μgm−3 and an inter-annual variation of about ± 2.9 μgm−3 (13% fluctuation margin). The absolute sulphate and calcium concentration (for the full period), as well as the EC concentration (time after 2003) decrease by about 50, 75 and 30% for PM10, respectively. The nitrate concentration remains constant all the time. For the daily objective weather type classification (OWTC, 1993–2002) the highest PM10 concentration was found for South-East (SE) and the lowest for North-West (NW) wind direction with 44 and 24 μgm−3, respectively. These concentrations decrease for 2003–2011 in comparison to 1993–2002 by about 21% and 26%, respectively. The highest PM10, PM2.5 and PM1 concentrations (2003–2011) were found for SE and the lowest for NW wind direction with about 34 and 17 μgm−3 (PM10), 28 and 19 μgm−3 (PM2.5) and 22 and 11 μgm−3 (PM1), respectively. The relative content of sulphate, OC and EC was the highest for SE wind direction. A differentiation into four categories for winter (Wi) and summer (Su) and air mass inflow from West (W) and East (E) was carried out. The highest PM concentrations were observed for WiE with the highest inter-annual fluctuation. In this category sulphate contents are largest. The lowest concentrations where found for SuW. The means for WiE show the strongest relative decreases, e.g. in PM10 sulphate (1993–2011) and EC (2003–2011) by about 60% and 40%, respectively. Nitrate is an indicator for NOx motor-car emissions. It shows a typical variation with maximum values in the middle of the week, especially for air mass inflow from West. In contrast, chloride mostly originating from sea spray doesn’t show such a concentration pattern. The PM2.5/PM10 as well the PM1/PM10-ratio have the highest median (0.878 and 0.654) during WiE and the lowest (0.718 and 0.578) during SuW, respectively. For the ratio PM2.5/PM10 a slightly increasing trend was found (about 0.71 and 0.83 for 1995 and 2011, respectively). The increase is stronger in summer than in winter.
Published Version
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