ABSTRACT INTRODUCTION

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1 The role of clouds in transformation and removal of air pollutants D. Moller, G. Mauersberger Department for Air Chemistry, Fraunhofer Institut for Atmospheric Environmental Research, D-1199 Berlin, Germany ABSTRACT The emission-deposition relationship is discussed from the point of view of multiphase chemistry. The role of clouds is briefly summarized. First results from cloud chemistry measurements at Mt. Brocken (Harz) and modelling are given and discussed in connection with the changing emission situation in the Neue Bundeslander. INTRODUCTION The principal role of clouds in air chemistry consists in a medium (a) for transportation, esp. in linkage between the hydrological and biogeochemical cycles and (b) for transformation, esp. liquid phase chemistry. The role of atmospheric liquid phase chemistry has been referred long time ago [1] as well as the assessment of liquid versus gaseous chemistry [2]. However, a complex view of the multiphase and multicomponent system have started very few years ago [3]. Recently the role of clouds in air pollutants distribution and several open questions have been summarized [4], see Fig. 1. Well accepted is the dominating in-cloud scavenging for wet deposition of trace constituents. An enhancement of Og formation due to dilution of polluted air parcels within cloud systems is shown in [5]. On the other hand, the clouds act as a sink for 0^ [6] and other photooxidants [7]. The problems of theoretical and - more complicated - experimental cloud chemistry research lies within the complexity of the system, in the linkage between chemical, microphysical and dynamical processes. Nevertheless, for any assessment of emission - deposition relations (cf. Fig. 2) and

2 374 Air Pollution especially for emission reduction strategies atmospheric heterogeneous processes must be taken into account owing to the nonlinearity of the processes. 8. onhanood dry dopooltlon (only for rain oloudc) 4. romovml from tho atmocphoro (wot deposition) Fig. 1. Schematic representation of the role of clouds in air chemistry THE NONLINEARITY RELATION BETWEEN EMISSION AND DEPOSITION In case of linear relationships any change of emission leads to the same percentage of deposition variation. Linearity is given if transformation and removal processes are determined by (pseudo-) first order rate equations. This is often the case for atmospheric gas phase chemistry (steady state conditions) and dry deposition. Aqueous phase reactions, however, are characterized by second order rate laws. Therefore, in dependence from the significance of aqueous phase chemistry and the frequency of cloudy conditions the emission-deposition relation deviates more or less from linearity. This point of view is very important in the eastern part of Germany (Neue Bundeslander) where the emission pattern is dramatically changing due to the political and economical changes since Therefore a large scientific project, called SANA (Recovery of the Atmosphere) has been established in 1991 funded by the

3 Air Pollution 375 Federal Ministry for Science and Technolgy. To improve models for air pollutants one subproject is dealing with cloud chemistry modelling in connection with experimental investigations for evaluation of the model modules. At the Brocken in the Harz Mountains (with 1142 m a.s.l. the highest elevation in the northern part of Middle Europe) a measuring station is built-up in 1991/92. The aim is to obtain a long-time data set for trace constituents within the aqueous (clouds, rain), aerosol and gas phase. Besidesthat intensive measuring campaigns are planned. In the following section some results from first measurements and modelling are presented. 802, CO, VOC urban emission dry deposition agricultural emission wet deposition Fig. 2. The emission-deposition relationship via multiphase chemistry processes RESULTS FROM MEASUREMENTS AND MODELLING Little is known on the frequency and liquid water content (LWC) of clouds in Middle Europe; so far no systematic investigations are available. Therefore, we started Gerber last year with continuous measurements by a instrument at the Brocken site. The LWC distribution is nearly log-normal (Fig. 3), the mean

4 376 Air Pollution LWC for all events amounts to 0.29 g/nr* a figure typically reported in literature for stratiform clouds. For the period observed the station lies within clouds for42 % of the whole time where the LWC lies mostly within the range between 0.1 and 0.4 g/nr* (to be 28% of time), see Fig. 4. The cloud frequency, however, shows large variations on a seasonal basis: in June clouds have been observed in 20 % and in november in 80 % of the whole time number of half hour etcnti Fig. 3. Distribution of liquid water content (LWC) of clouds at the Brocken (Harz) from march to november 1991 elovd f**# (38%) > cloudy (42 %) Fig. 4. Percentage of cloud events; LWC given in

5 Air Pollution 377 From rain and cloud chemical composition we have only very preliminary results at the Brocken (Fig. 5). From wet deposition investigations it is known that large variations for single events occur. Therefore, conclusions on precipitaion chemistry can be drawn only after longer sampling time. Because the results shown in Fig. 5 seems to be surprising we want to present the data. At first it is seen that there are no significant differences between rain and cloud water composition. However, the high nitrate and relatively low sulphate concentrations are absolutely unexpected. concentration in ppm DU rain cloud rain clo ltd ; R 1 '" " 2 1 L L 1 'h. L : 1 \ S 1 I : I : ; 4 Oct 6/7, 1991 (West) Sept 26, 1991 (East) time/date I N03- EB1NH4+ ES3 Cl- Fig. 5. Rain and cloud chemical composition in sequential samples for a typical westerly and easterly wind episode For comparison the mean ground-level concentrations in rain for the Neue Bundeslander are given (in ppm): 16 for 50*2-, 3 for NOg", 1.6 for NH*+. The sulphate/nitrate ratio amounts to be 0.4 at the Brocken in cloudwater and 5.3 in rainwater at ground-level measuring sites as an average for the New Countries. A first conclusion should be (based on the preliminary

6 378 Air Pollution measured cloud/rain sulphate ratio of 0.7) that sulphur sub-cloud scavenging (as SOj and sulphate aerosol) may be more important in polluted air than expected so far. The reason for the high nitrate content in hydrometeors at the Brocken site must be clarified by systematic investigations. Our investigations on transformation and removal by clouds are focussed on the background of the changing emission situation in the Neue Bundeslander which have taken place since The NC^ and SOj concentrations are decreased significantly at the Brocken (Fig. 6); it must be taken into account, however, that air masses are coming to 60 % of the yearly time from westerly directions. concentration in Mg/m3 SONDJFMAMJ JASONDJ FMAMJ JASONDJ FMAMJ SO2 -*- NO2 Fig. 6. SOj and NO2 concentrations at the Brocken (daily measurements by the former Meteorological Service of the GDR) The decrease of emissions of SO2 leads to a decrease of atmospheric acidity too. However, the decrease of NHg and alkaline flue ash emissions may increase the

7 Air Pollution 379 acidity budget. On the other hand it is likely that photooxidant precursers like NO, VOC and CO (emissions from traffic) increase. Therefore it is of high interest to investigate the relationship between the acidity and the oxidation capacity in the atmosphere under these changing conditions. With our cloud chemistry model [7] we investigated the influence of SOj on the atmospheric concentration of H2O2 and O^ via the liquid phase. The cloud acts as very effective sink for gaseous HjOj, but only for SO% larger than 0.5 ppb aqueous phase ^2^2 will be destroyed by S(IV), see Fig. 7. For lower SOj liquid phase HoOj formation from HO^/O^" is balanced with the decay via the Fenton reaction (Fe%+ as reactant). Only in absence of these components in very remote areas a liquid phase netto production of ^03 is possible [6]. H202(goseous) in ppb H202(liquld) in pmol/ SO2 (gaseous) in ppb H2O2(g<neoai) -*- H2O2(liqnid) Fig. 7. Dependence of gaseous (interstitial) and cloud water H^Og concentration, resp., after 1 h model run (cloud event) from the initial gaseous SO2 concentration; initial ^02 1 ppb A significant influence of 803 on the aqueous phase O^ sink capacity we have found in other direction: decreasing 803 leads to increasing Og destraction via the droplet phase (Fig. 8). The share of transformed 0^ via 8 (IV) On increased with increasing SO^, 2' the reaction (_ however, is much more important. More 02" is~available (a) at higher due to the > HO2 transformation and (b) at higher ph due to pk(hoo/o2~) = 5; both is corresponding with lower SO^. Very interesting seems to be that no O^ accumulation takes place within the droplet phase.

8 380 Air Pollution accumulation O+O' + HO -> YSA <r> ^0.75 O <u o* 0-5 j : 3 OJC « tppbl Fig. 8. Mean Og flux within the cloud water in dependence from the gaseous SOj concentration; gaseous O^ concentration: 30 ppb LITERATURE 1. Junge, C.E. and Ryan, T.G. * Study of the 803 oxidation in solution and its role in atmospheric chemistry' Quart. J. R. Met. Soc., Vol.85, pp , Holler, D. *Kinetic model of atmospheric SOg oxidation based on published data* Atmos. Environ., Vol..14, pp , Jaeschke, W. (Ed.) Chemistry of multiphase atmospheric systems, Springer-Verlag Berlin Heidelberg, WMO (1991) Meeting of Experts on the Role of Clouds in the Chemistry, Transport, Transformation and Deposition of Pollutants..Report WMO/TD-No Walcek, C.J. *Regional-Scale Influence on Cloud- Scale Scavenging and Dynamic Processes', in Proceedings of the Fifth Int. Conf. on Precipitation Scavenging and Atmosphere-Surface Exchange Processes (Ed. Schwartz, S.E. and Slinn, W.G.N.) pp , Hemisphere Publ. Corp. Washington Philadelphia London Lelieveld, J. and Crutzen, P.J. * Influences of cloud photochemical processes on tropospheric ozone* Nature, Vol.14, pp , Moller, D. and Mauersberger, G. * Cloud chemistry effects on tropospheric photooxidants in polluted atmosphere - model results' J. Atmos. Chem., Vol.14, pp , 1992

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