Comparison among model estimates of critical loads of acidic deposition using different sources and scales of input data

The critical load (CL) of acidic atmospheric deposition represents the load of acidity deposited from the atmosphere to the earth’s surface at which harmful acidification effects on sensitive biological receptors are thought to occur. In this study, the CL for forest soils was estimated for 27 watersheds throughout the United States using a steady-state mass balance approach based on both national and site-specific data and using different approaches for estimating base cation weathering. Results suggested that the scale and source of input data can have large effects on the calculated CL and that the most important parameter in the steady-state model used to estimate CL is base cation weathering. These results suggest that the data and approach used to estimate weathering must be robust if the calculated CL is to be useful for its intended purpose.     

Forest Die-Back Modified Plankton Recovery from Acidic Stress

We examined long-term data on water chemistry of Lake Rachelsee (Germany) following the changes in acidic depositions in central Europe since 1980s. Despite gradual chemical recovery of Rachelsee, its biological recovery was delayed. In 1999, lake recovery was abruptly reversed by a coincident forest die-back, which resulted in elevated terrestrial export of nitrate and ionic aluminum lasting ~5 years. This re-acidification episode provided unique opportunity to study plankton recovery in the rapidly recovering lake water after the abrupt decline in nitrate leaching from the catchment. There were sudden changes both in lake water chemistry and in plankton biomass structure, such as decreased bacterial filaments, increased phytoplankton biomass, and rotifer abundance. The shift from dominance of heterotrophic to autotrophic organisms suggested their substantial release from severe phosphorus stress. Such a rapid change in plankton structure in a lake recovering from acidity has, to the best of our knowledge, not been previously documented.     

Air quality assessment by tree bark biomonitoring in urban, industrial and rural environments of the Rhine Valley: PCDD/Fs, PCBs and trace metal evidence

Tree barks were used as biomonitors to evaluate past atmospheric pollution within and around the industrial zones of Strasbourg (France) and Kehl (Germany) in the Rhine Valley. The here estimated residence time for trace metals, PCBs and PCDD/Fs in tree bark is >10 years. Thus, all pollution observed by tree bark biomonitoring can be older than 10 years. The PCB baseline concentration (sum of seven PCB indicators (Σ₇PCB_ind)) determined on tree barks from a remote area in the Vosges mountains is 4 ng g⁻¹ and corresponds to 0.36 × 10⁻³ ng toxic equivalent (TEQ) g⁻¹ for the dioxin-like PCBs (DL-PCBs). The northern Rhine harbor suffered especially from steel plant, waste incinerator and thermal power plant emissions. The polychlorinated dibenzo-p-dioxin and dibenzofuran (PCDD/Fs) concentrations analyzed in tree barks from this industrial area range between 392 and 1420 ng kg⁻¹ dry-weight (dw) corresponding to 3.9 ng TEQ_PCDD/Fs kg⁻¹ to 17.8 ng TEQ_PCDD/Fs kg⁻¹, respectively. Highest PCDD/F values of 7.2 ng TEQ kg⁻¹ to 17.8 ng TEQ kg⁻¹ have been observed close to and at a distance of <2 km southwest of the chemical waste incinerator. However, very close to this incinerator lowest TEQ dioxin-like PCB (TEQ_DL-PCB) values of 0.006 ng TEQ g⁻¹ have been found. On the other hand close to and southwest and northeast of the steel plant the values are comparatively higher and range between 0.011 ng TEQ g⁻¹ and 0.026 ng TEQ g⁻¹. However, even stronger Σ₇PCB_ind enrichments have been observed at a few places in the city center of Kehl, where ΣDL-PCB values of up to 0.11 ng TEQ g⁻¹ have been detected. These enrichments, however, are the result of ancient pollutions since recent long-term measurements at the same sites indicate that the atmospheric PCB concentrations are close to baseline. Emissions from an old landfill of waste and/or great fires might have been the reasons of these PCB enrichments. Other urban environments of the cities of Kehl and Strasbourg show significantly lower Σ₇PCB_ind concentrations. They suffer especially from road and river traffic and have typically Σ₇PCB_ind concentrations ranging from 11 ng g⁻¹ to 29 ng g⁻¹. The PCB concentration of 29 ng g⁻¹ has been found in tree bark close to the railway station of Strasbourg. Nevertheless, the corresponding TEQ_DL-PCB are low and range between 0.2 × 10⁻³ ng TEQ g⁻¹ and 7 × 10⁻³ ng TEQ g⁻¹. Samples collected near road traffic are enriched in Fe, Sb, Sn and Pb. Cd enrichments were found close to almost all types of industries. Rural environments not far from industrial sites suffered from organic and inorganic pollution. In this case, TEQ_DL-PCB values may reach up to 58 × 10⁻³ ng TEQ g⁻¹ and the corresponding V, Cr, Co, Ni, and Cd concentrations are comparatively high.     

Atmospheric fate of non-volatile and ionizable compounds

A modified version of the Multimedia Activity Model for Ionics MAMI, including two-layered atmosphere, air-water interface partitioning, intermittent rainfall and variable cloud coverage was developed to simulate the atmospheric fate of ten low volatility or ionizable organic chemicals. Probabilistic simulations describing the uncertainty of substance and environmental input properties were run to evaluate the impact of atmospheric parameters, ionization and air-water (or air-ice) interface enrichment.The rate of degradation and the concentration of OH radicals, the duration of dry and wet periods, and the parameters describing air-water partitioning (K_AW and temperature) and ionization (pK_a and pH) are the key parameters determining the potential for long range transport. Wet deposition is an important removal process, but its efficiency is limited, primarily by the duration of the dry period between precipitation events.Given the underlying model assumptions, the presence of clouds contributes to the higher persistence in the troposphere because of the capacity of cloud water to accumulate and transport non-volatile (e.g. 2,4-D) and surface-active chemicals (e.g. PFOA). This limits the efficiency of wet deposition from the troposphere enhancing long-range transport.     

The impact of nitrogen deposition on acid grasslands in the Atlantic region of Europe

A survey of 153 acid grasslands from the Atlantic biogeographic region of Europe indicates that chronic nitrogen deposition is changing plant species composition and soil and plant-tissue chemistry. Across the deposition gradient (2-44 kg N ha⁻¹ yr⁻¹) grass richness as a proportion of total species richness increased whereas forb richness decreased. Soil C:N ratio increased, but soil extractable nitrate and ammonium concentrations did not show any relationship with nitrogen deposition. The above-ground tissue nitrogen contents of three plant species were examined: Agrostis capillaris (grass), Galium saxatile (forb) and Rhytidiadelphus squarrosus (bryophyte). The tissue nitrogen content of neither vascular plant species showed any relationship with nitrogen deposition, but there was a weak positive relationship between R. squarrosus nitrogen content and nitrogen deposition. None of the species showed strong relationships between above-ground tissue N:P or C:N and nitrogen deposition, indicating that they are not good indicators of deposition rate.     

Experimental investigation of outdoor and indoor mean concentrations and concentration fluctuations of pollutants

Tracer gas was released upwind of a two-compartment complex shaped building under unstable atmospheric conditions. The mean wind direction was normal to or at 45° to the long face of the building. The general patterns of concentration distribution on the building external walls and inside the building were analysed and the influence of natural and mechanical ventilation on indoor concentration distributions was discussed. Mean concentration levels, as well as the concentration fluctuation intensity, were higher on the windward walls of the building, although concentration levels varied along each wall. Concentration fluctuations measured inside the building were lower than those measured outside. Inside the two compartments of the building, the time series of concentrations had a similar general behaviour; however, gas concentrations took approximately 1.5 times longer to reach the mean maximum concentration value at the downwind compartment 02 while they also decreased more rapidly in the upwind compartment 01 after the source was turned off. The highest indoor concentration and concentration fluctuation values were observed at the detectors located close to the windward walls, especially when the building windows were open. Experiments with and without natural ventilation suggested that infiltration and exfiltration of contaminants is much faster when the building windows are open, resulting to higher indoor concentration levels. Furthermore, mechanical ventilation tends to homogenize concentrations and suppress concentration fluctuations, leading to lower maximum concentration values.     

黄河中上游能源化工区大气污染跨界环境影响分析

对黄河中上游能源化工区近地面和边界层顶气象流场及该区域大气污染长距离输送产生的跨界环境影响趋势特征进行了分析。结果表明,该区域近地面和边界层顶的流场总体上为西北向东南流动,大气污染物长距离输送可能影响的区域主要为华中地区;区域冷空气的活动对其大气污染物的清除起重要作用;通过CALPUFF模型的模拟结果表明,该区域SO2的影响程度和范围明显大于NO2,在区域内部存在污染物浓度较高的区域,但未对区外造成显著跨界环境影响。     

Which compounds contribute most to elevated airborne exposure and corresponding health risks in the Western Balkans?

A majority of ongoing monitoring of persistent organic pollutants (POPs) is currently focused on chemicals emphasized in the Stockholm Convention. Quantitative detection of other substances (especially those with numerous anthropogenic sources such as polyaromatic hydrocarbons (PAHs)) is, however, also needed since their concentrations are usually several orders of magnitude higher. A goal of this study was to determine how various groups of compounds contribute to total human health risks at the variety of sampling sites in the region of Western Balkan. Distribution of the risks between the gas and particulate phases was also addressed. Results showed that inhalation exposure to organochlorine pesticides (OCPs) does not represent a significant risk to humans, while polychlorinated biphenyls (PCBs) re-volatilized to the atmosphere from contaminated soils and buildings can pose a problem. PCB evaporation from primary sources (currently used PCB-filled transformers or non-adequate storage facilities) generally resulted in much higher atmospheric concentrations than evaporation from the secondary sources (soils at the sites of war destructions). A majority of the human health risks at the urban sites were associated with PAHs. Between 83 and 94% of the cumulative risk at such sites was assigned to chemicals sorbed to particles, and out of it, PAHs were responsible for 99%.     

Temporal patterns of atmospheric mercury species in northern Mississippi during 2011–2012: Influence of sudden population swings

Gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM) and particulate bound mercury (PBM) were measured on the University of Mississippi campus from July 2011 to June 2012. It is believed to be the first time that concentrations of atmospheric mercury species have been documented in northern Mississippi, and at a location with relatively large and sudden swings in population. The mean concentration (±1SD) of GEM was 1.54 ± 0.32 ng m⁻³; levels were lower and generally more stable during the winter (1.48 ± 0.22) and spring (1.46 ± 0.27) compared with the summer (1.56 ± 0.32) and fall (1.63 ± 0.42). Mean concentrations for GOM and PBM were 3.87 pg m⁻³ and 4.58 pg m⁻³, respectively; levels tended to be highest in the afternoon and lowest in the early morning hours. During the fall and spring academic semesters concentrations and variability of GOM and PBM both increased, possibly from vehicle exhaust. There were moderate negative correlations with wind speed (all species) and humidity (GOM and PBM). Backward air mass trajectory modeling for the ten highest peaks for each mercury species revealed that the majority of these events occurred from air masses that passed through the northern continental US region. Overall, this study illustrates the complexity of temporal fluctuations of airborne mercury species, even in a small town environment.     

大气环境数据分析预测方法对比研究

以西安市2006年9月27日至2008年5月3日每日的SO2平均浓度时间序列为例,应用时间序列分析对前555个数据进行拟合,得到合适的时间序列模型ARIMA(1,1,2);利用神经网络中的BP神经网络和RBF神经网络对同样的样本进行训练,用这三种方法对2008年4月4日至2008年5月3日的SO2日均浓度值进行了预测,并用同样的方法分析预测了同期PM10日均浓度值,最后比较了它们的预测效果。结果表明,利用这三种方法进行浓度预测都是可行的,其中RBF神经网络法的预测误差最小,效果最好。