Aerosol light-scattering in The Netherlands

The relation between the (midday) aerosol light-scattering and the concentrations of nitrate and sulfate has been assessed at a site near the coast of the North Sea in The Netherlands. Midday was selected for the measurements because this is the time at which the aerosol is most effective in the scattering of solar radiation. Automated thermodenuders were used for the hourly measurement of the concentration of nitrate and sulfate with a lower detection limit of 0.1 μ m⁻³. The site is operational since October 1993. The first-year average dry aerosol light-scattering (measured with an integrating nephelometer at a wavelength of 525 nm) was 0.71 × 10⁻⁴ m^1̄. In arctic marine air the aerosol light-scattering was a factor of 10 lower than the average value, in polluted continental air it was up to a factor of 10 higher. The ratio of the total aerosol light-scattering to the concentration of sulfate was 20 m² g⁻¹. The contribution of nitrate to the aerosol light-scattering was higher than that of sulfate in the winter and of about equal magnitude in the summer period. In November and December of 1993, the humidity dependence of the aerosol light-scattering was investigated. Two types of (continental) aerosol were found with respect to the humidity behavior. One type showed a significant increase in light-scattering at the deliquescence points of ammonium nitrate and ammonium sulfate, with that of ammonium nitrate the most pronounced. The second type of continental aerosol did not show deliquescence, but followed the typical humidity dependence of aerosol in a supersaturated droplet state. In this latter aerosol type, nitrate dominated over sulfate. It was concluded from the study that the aerosol light-scattering in The Netherlands, in particular its humidity dependence, is governed by (ammonium) nitrate.     

Measurement of the leaching behaviour of granular solid wastes

Leaching of granular solids can be described in terms of specific mass transfer functions of a simple mathematical form.

The parameters can be determined by column leaching experiments under well known flow conditions.

Initially available concentrations are obtained from batch experiments at high dilution. Total concentrations in the solids are determined independently to calculate the available fractions.

The determination of the flow pattern is done by radiotracer measurements. Leachates are analyzed by various analytical methods including AAS and INAA. Total concentrations in the solids are determined by INAA preferably.     

Trends in summer sulphate in Europe

A trend analysis of the sulphate concentration in Europe in the summer half-year was performed. Data from various measuring networks were analysed, but only stations with quality assured sampling methods and a record of more than 10 years were included in the study. 1978 served as the reference year for the trend, because in that year most stations started operation. The relatively dense network in Belgium provided the most valuable data, as evidenced by the fact that two sites at a distance of only 10 km apart correlated better than 95% over a month. The two sites also show a correlation of better than 90% over a season with two other stations at distances of 45 and 95 km. The relative decrease in summer-sulphate at the four stations in Belgium, as analysed by linear regression, was 3.3% per year which corresponds to an absolute decrease of 0.42 μgm⁻³ per year. In the Netherlands the average yearly decrease in summer-sulphate at two stations was 3.5% (−0.34 μgm⁻³). In other countries stations were further apart or only a single site wits in use, which limits the representativeness of the data. In northwestern Germany, a region with several monitoring stations, a yearly averaged decrease of 3.0% occurred. The lower absolute decrease (0.25 μgm⁻³) per year compared to that in the two neighbouring countries reflects the lower summer-time sulphate concentrations. In the remainder of Germany the average decrease was 1.6%. In South-Scandinavia the yearly relative decrease at two sites was 2.6% (0.13 μgm⁻³ absolute). There was no significant trend in the U.K. Al the Polish station the levels increased, it decreased at the Hungarian and Austrian station and remained constant at the Czechoslovakian site. Reasons for omission of the data from France from the trend analysis are discussed.     

Fate of products of degradation processes: consequences for climatic change

The end products of atmospheric degradation are not only CO2 and H2O but also sulfate and nitrate depending on the chemical composition of the substances which are subject to degradation processes. Atmospheric degradation has thus a direct influence on the radiative balance of the earth not only due to formation of greenhouse gases but also of aerosols. Aerosols of a diameter of 0.1 to 2 micrometer, reflect short wave sunlight very efficiently leading to a radiative forcing which is estimated to be about -0.8 watt per m2 by IPCC. Aerosols also influence the radiative balance by way of cloud formation. If more aerosols are present, clouds are formed with more and smaller droplets and these clouds have a higher albedo and are more stable compared to clouds with larger droplets. Not only sulfate, but also nitrate and polar organic compounds, formed as intermediates in degradation processes, contribute to this direct and indirect aerosol effect. Estimates for the Netherlands indicate a direct effect of -4 watt m-2 and an indirect effect of as large as -5 watt m-2. About one third is caused by sulfates, one third by nitrates and last third by polar organic compounds. This large radiative forcing is obviously non-uniform and depends on local conditions.     

Transport model calculations of NW-European methane emissions

Methane emissions of large parts of NW-Europe are derived from continuous concentration measurements at one sample site (Cabauw tower, The Netherlands) using the COMET transport model. This approach can be used as an independent check of emission estimates based on statistical information. COMET is a two-layer Lagrangian atmospheric transport model that describes the uptake of methane emissions in the mixing layer along a backward trajectory path and the exchange with a reservoir layer during mixing layer height changes. In inverse mode a Singular Value Decomposition (SVD) matrix inversion technique is used to calculate the emissions of a limited number of source areas using four years of 6-hourly concentration data (1993–1996) at Cabauw. The calculated emissions compare well with the current emission inventory data for the Netherlands and the surrounding countries. For the Netherlands a yearly emission of 757 Gg of methane is calculated, excluding the emissions from oil and gas mining at the North Sea continental shelf.     

Results of the “carbon conference” international aerosol carbon round robin test stage I

An international round robin test on the analysis of carbonaceous aerosols on quartz fiber filters sampled at an urban site was organized by the Vienna University of Technology. Seventeen laboratories participated using nine different thermal and optical methods. For the analysis of total carbon (TC), a good agreement of the values obtained by all laboratories was found (7 and 9% r.s.d.) with only two outliers in the complete data set. In contrast the results of the determination of elemental carbon (EC) in two not pre-extracted samples were highly variable ranging over more than one order of magnitude and the relative standard deviations (r.s.d.) of the means were 36.6 and 45.5%. The laboratories that obtained similar results by using methods which reduce the charring artifact were put together to a new data set in order to approach a “real EC” value. The new data set consisting of the results of 10 laboratories using seven different methods showed 16 and 24% lower averages and r.s.d. of 14 and 24% for the two not pre-extracted samples. Taking the current filters as “equivalents” for urban aerosol samples we conclude that the following methods can be used for the analysis of EC in carbonaceous aerosols: thermal methods with an optical feature to correct for charring during pyrolysis, two-step thermal procedures reducing charring during pyrolysis, the VDI 2465/1 method (removal of OC by solvent extraction and thermodesorption in nitrogen) and the VDI 2465/2 method (combustion of OC and EC at different temperatures) with an additional pre-extraction with a dimethyl formamide (DMF)/toluene mixture. Only thermal methods without any correction for charring during pyrolysis and the VDI 2465/2 method were outside the range of twice the standard deviation of the new data set. For a filter sample pre-extracted with the DMF/toluene mixture the average and r.s.d. from all laboratories (20.7 μgC; 24.4% r.s.d.) was very similar as for the laboratory set reduced to 10 laboratories (20.6 μgC; 19% r.s.d.). Thus DMF pre-extraction appears to improve the performance of the thermal methods without charring during pyrolysis control, e.g. the VDI 2465/2 methods.     

The continuous analysis of nitrate and ammonium in aerosols by the steam jet aerosol collector (SJAC): extension and validation of the methodology

Classical methodology based on the application of filters for sampling, followed by extraction and analysis, introduces severe artifacts for semi-volatile compounds like ammonium nitrate. These filter methods do not meet the requirements for the assessment of the impact of aerosols on acidification, air quality and especially on the radiative balance, in terms of required speed, detection limits and selectivity. These artifacts are avoided by using a steam jet aerosol collector sampler, based on scavenging of aerosols by droplet formation, in combination with on-line analytical techniques such as ion-chromatography for nitrate and membrane separation followed by conductivity detection for ammonium. The SJAC sampler combines very low blanks with high efficiency of collection of particles. The ammonium detector and the IC system, based on 1-point internal standard calibration in combination with correction for curved calibration graphs, enables detection of ammonium and nitrate at background conditions, the detection limit is about 0.02 μg m⁻³ of ammonium and nitrate. Accuracy is, depending on ambient concentration, in the order of 5–10% relative, at a range of 0.05–50 μg m⁻³. The time resolution is 15–120 min, depending on required detection limit, and is short enough for continuously monitoring the chemical composition of aerosols. Quality assurance and quality control experiments and intercomparison experiments with classical filter methods, thermo-denuder systems, denuder difference methods and other continuous monitoring techniques have shown that the results are reliable. The instrument has successfully been employed in field campaigns in Europe and the US.     

NitroGenius: a nitrogen decision support system. A game to develop the optimal policy to solve the Dutch nitrogen pollution problem

A nitrogen decision support system in the form of a game (NitroGenius) was developed for the Second International Nitrogen Conference. The aims were to: i) improve understanding among scientists and policy makers about the complexity of nitrogen pollution problems in an area of intensive agricultural, industrial, and transportation activity (The Netherlands); and ii) search for optimal policy solutions to prevent pollution effects at lowest economic and social costs. NitroGenius includes a model of nitrogen flows at relevant spatial and temporal scales including emissions of ammonia and nitrogen oxides and contamination of surface- and groundwaters. NitroGenius also includes an economic model describing relationships for important sectors and impacts of different nitrogen control measures on Gross Domestic Product (GDP), unemployment, energy use, and environmental costs. About 50 teams played NitroGenius during the Second International Nitrogen Conference. The results show that careful planning and selection of abatement options can solve Dutch nitrogen problems at reasonable cost.     

Determination of European methane emissions,using concentration and isotope measurements

The determination of methane emissions on a regional scale is needed in order to reduce some of the uncertainties in the global methane budget. Our measurements of the concentration and the Carbon-13 isotope composition (¹³C) of atmospheric methane are, combined with trajectories, used to get insight in the type and size of the methane emissions of a large area.