Nonlinearities in source receptor relationships for sulfur and nitrogen compounds

The relationship between emissions and deposition of air pollutants, both spatially and in time forms an important focus for science and for policy makers. In practice, this relationship may become nonlinear if the underlying processes change with time, or in space. Nonlinearities may also appear due to errors in emission or deposition data, and careful scrutiny of both data sources and their relationship provides a means of picking up such deficiencies. Nonlinearities in source receptor relationships for sulfur and nitrogen compounds in Europe have been identified in measurement data for the UK. In the case of sulfur, the dry deposition process has been shown to be strongly influenced by ambient concentrations of NH3, leading to substantial increases in deposition rate as SO2 concentrations decline and the ratio SO2/NH3 decreases. The field evidence extends to measurements over three different surfaces in three countries across Europe. A mechanistic understanding of the cause of this nonlinearity has been provided. Apparent nonlinearities also exist in the sulfur deposition field through the influence of shipping emissions. The effect is clear at west coast locations, where during a period in which land-based sulfur emissions declined by 50%, no significant decline in concentrations of SO(2-) in precipitation were observed. The sites affected are primarily the coastal regions of southwestern UK, where shipping sources contribute a substantial fraction of the deposited sulfur, but the effect is not detectable elsewhere. Full quantification of the spatially disaggregated emission and their changes in time will eliminate this apparent nonlinearity in the source-receptor data. For oxidized nitrogen emission and deposition in the UK, there is strong evidence of nonlinearity in the source-receptor relationship. The concentrations and deposition of NO(3-) in precipitation have declined little following a reduction in emissions of 45% during the period 1987 to 2001. The data imply a significant decrease in the average transport distance for oxidized nitrogen and most probably an increase in the average oxidation rate. However, the net effect of changes in aerosol chemistry due to changes in sulfur emissions and less competition for the main oxidants as a consequence of reductions in sulfur emission have not been separated. A quantitative explanation of the cause of this nonlinearity is lacking and the effects are therefore identified as an important uncertainty for the development of further protocols to control acidification, eutrophication and photochemical oxidants in Europe.     

Dry Deposition Monitoring in Europe

Between 1993 and 1999 two EU funded projects wereexecuted aimed at (i) the development of drydeposition monitoring methods for core sites andlarge scale application, (ii) the installation andrunning of three core sites in Europe and (iii) the improvement and validation of models used forregional application. This article provides anoverview of the development of depositionmonitoring stations and the main results of thethree core sites, which were operated between1995 and 1998. Furthermore, the results of thedevelopment of a low cost monitoring system arepresented. Continuous measurements were made ofboth wet and dry deposition of sulphur andnitrogen components and base cations. The 4 yearsof data show a decrease in sulphur loads and notrend for the other components. It is shown thatthe surface affinities for sulphur depositionalso changed during the years, underpinning theneed for dry deposition monitoring. A conditionaltime average gradient system was successfullydeveloped and tested and provides a good meansfor low cost monitoring of dry deposition fluxes.The costs can be reduced by a factor of 3–4 without losing the accuracy of the annual average gas fluxes.     

NitroGenius:氮决策支持系统--荷兰氮污染问题最佳解决方案的一个游戏模拟实验

利用计算机模拟的方法,我们为第二届国际氮会议研制开发了一个游戏形式的氮决策支持系统.研制这一系统的目的是:①使科学工作者和决策者们都能认识到荷兰氮污染问题的复杂性,因为荷兰是一个农业、工业和运输业活动密集的区域;②探索以最低的社会经济代价解决氮污染的最佳方案.NitroGenius由有关时空范围内的氮流动模型组成,其中包括氨和氮氧化合物的释放及其对地表水和地下水的污染.NitroGenius中还包括了一个经济模型,它描述了各个重要经济部门之间的关系,以及不同氮排放控制措施对国民生产总值(GDP)、失业率、能源消耗和环境的影响.在第二次国际氮会议期间,大约有50个研究组对NitroGenius进行了测试,结果表明,如果认真进行计划并选择适当的治理措施,就能够以适当的代价解决荷兰的氮污染问题.     

Monitoring and modelling of biosphere/atmosphere exchange of gases and aerosols in Europe

Monitoring and modelling of deposition of air pollutants is essential to develop and evaluate policies to abate the effects related to air pollution and to determine the losses of pollutants from the atmosphere. Techniques for monitoring wet deposition fluxes are widely applied. A recent intercomparison experiment, however, showed that the uncertainty in wet deposition is relatively high, up to 40%, apart from the fact that most samplers are biased because of a dry deposition contribution. Wet deposition amounts to about 80% of the total deposition in Europe with a range of 10-90% and uncertainty should therefore be decreased. During recent years the monitoring of dry deposition has become possible. Three sites have been operational for 5 years. The data are useful for model development, but also for model evaluation and monitoring of progress in policy. Data show a decline in SO(2) dry deposition, whereas nitrogen deposition remained constant. Furthermore, surface affinities for pollutants changed leading to changes in deposition. Deposition models have been further developed and tested with dry deposition measurements and total deposition measurements on forests as derived from throughfall data. The comparison is reasonable given the measurement uncertainties. Progress in ozone surface exchange modelling and monitoring shows that stomatal uptake can be quantified with reasonable accuracy, but external surface uptake yields highest uncertainty.     

The need for ammonia abatement with respect to secondary PM reductions in Europe

In Europe, secondary particulate matter (PM) comprises 50% or more of PM 2.5. To reduce PM concentrations requires lowering precursor emissions. Since the 1980s, SO(2) emissions have decreased by more than 60%, while particle concentrations have decreased less. NO(x) and NH(3) emissions have decreased slightly. The role of ammonia in particle formation is addressed here. It is shown that secondary PM concentrations can only be effectively reduced if ammonia emissions are decreased in much the same way as those of SO(2) and NO(x).     

Base cation deposition in europe-part I. Model description, results and uncertainties

Deposition of base cations (Na⁺, Mg²⁺, Ca²⁺, K⁺) in Europe was mapped for 1989 with a spatial resolution of 10 x 20 km using the so-called inferential modeling technique. Deposition fields resembled the geographic variability of sources, land-use and climate. Dry deposition constituted on average 45% of the total base cation deposition in Europe. Modeled deposition estimates compared reasonably well with deposition estimates derived from throughfall and bulk-precipitation measurements made at 174 sites scattered over Europe. Using error propagation, the random and systematic error in total deposition for an average grid cell of 10 x 20 km was estimated to equal 35–50% and 25–40%, respectively. Within individual grids a relatively large variability in deposition is expected.     

Establishing the link between ammonia emission control and measurements of reduced nitrogen concentrations and deposition

In the context of international efforts to reduce the impactsof atmospheric NH₃ and NH₄ ⁺ (collectively, NH_x), it is important to establish the link between NH₃emissions and monitoring of NH_x concentrations and deposition. This is equally relevant to situations where NH₃emissions changes are certain (e.g. due to changed source sectoractivity), as to cases where NH₃ abatement technologies havebeen implemented. Correct interpretation of adequate atmosphericmeasurements is essential, since monitoring data provide the onlymeans to evaluate trends in regional NH₃ emissions.These issues have been reviewed using available measurements and modelling from nine countries. In addition to historic datasets,the analysis here considers countries where NH₃ source sector activity changed (both increases and decreases) and countries where NH₃ abatement policies have been implemented.In The Netherlands an `ammonia gap' was identified between the expected reduction and results of monitoring, and was attributedinitially to ineffectiveness of the abatement measures. The analysis here for a range of countries shows that atmospheric interactions complicate the expected changes, particularly sinceSO₂ emissions have decreased at the same time, while at manysites the few years of available data show substantial inter-annual variation. It is concluded that networks need to beestablished that speciate between NH₃ and aerosol NH₄ ⁺, in addition to providing wet deposition, and sample at sufficient sites for robust regional estimates to be established. Such measurements will be essential to monitor compliance of the international agreements on NH₃ emission abatement.     

Element fluxes through European forest ecosystems and their relationships with stand and site characteristics

This paper describes a European wide assessment of element budgets, using available data on deposition, meteorology and soil solution chemistry at 121 Intensive Monitoring plots. Input fluxes from the atmosphere were derived from fortnightly or monthly measurements of bulk deposition and throughfall, corrected for canopy uptake. Element outputs from the forest ecosystem were derived by multiplying fortnightly or monthly measurements of the soil solution composition at the bottom of the root zone with simulated unsaturated soil water fluxes. Despite the uncertainties in the calculated budgets, the results indicate that: (i) SO4 is still the dominant source of actual soil acidification despite the generally lower input of S than N, due to the different behaviour of S (near tracer) and N (strong retention); (ii) base cation removal due to man-induced soil acidification is limited; and (iii) Al release is high in areas with high S inputs and low base status.     

Distribution of uranium contamination in weathered fractured saprolite/shale and ground water

The objective of this study was to determine how structure, stratigraphy, and weathering influence fate and transport of contaminants (particularly U) in the ground water and geologic material at the Department of Energy (DOE) Environmental Remediation Sciences Department (ERSD) Field Research Center (FRC). Several cores were collected near four former unlined adjoining waste disposal ponds. The cores were collected, described, analyzed for U, and compared with ground water geochemistry from surrounding multilevel wells. At some locations, acidic U-contaminated ground water was found to preferentially flow in small remnant fractures weathering the surrounding shale (nitric acid extractable U [U(NA)] usually < 50 mg kg(-1)) into thin (<25 cm) Fe oxide-rich clayey seams that retain U (U(NA) 239 to 375 mg kg(-1)). However, greatest contaminant transport occurs in a 2 to 3 m thick more permeable stratigraphic transition zone located between two less permeable, and generally less contaminated zones consisting of (i) overlying unconsolidated saprolite (U(NA) < 0.01 to 200 mg kg(-1)) and (ii) underlying less-weathered bedrock (U(NA) generally < 0.01 to 7 mg kg(-1)). In this transition zone, acidic (pH < 4) U-enriched ground water (U of 38 mg L(-1)) has weathered away calcite veins resulting in greater porosity, higher hydraulic conductivity, and higher U contamination (U(NA) 106 to 745 mg kg(-1)) of the weathered interbedded shale and sandstone. These characteristics of the transition zone produce an interval with a high flux of contaminants that could be targeted for remediation.