北京大气沉降样品中的PCBs

采集了4个北京大气沉降样品,包括3个总沉降与1个湿沉降样品.利用高分辨率气质联用仪(HRGC-HRMS),参照国际标准方法分析测定了其中的多氯联苯(PCBs)含量.总沉降样品的PCBs含量水平为4.47～7.08ng·g-1(平均为5.52ng·g-1)和TEQ为0.55～5.43 pg·g-1(平均为2.27 pg·g-1).湿沉降样品含量水平为15.02 ng·g-1,其TEQ为2.87 pg·g-1.首钢样品的TEQ远高于其它3个样品.根据我国大气降尘数据,粗略估计北京PCBs大气沉降通量平均值为67.9 ng·m-2·m-1和TEQ平均通量为27.9 pg·m-2·m-1.首钢样品中,IUPAC编号为77的类二(噁)英PCBs含量异常高,但TEQ仍以编号为126的PCBs所占比例最高.随着取代氯原子数的增加,同族体的含量逐渐降低.     

A first generation dynamic ingress,redistribution and transport model of soil track-in: DIRT

This work introduces a spatially resolved quantitative model, based on conservation of mass and first order transfer kinetics, for following the transport and redistribution of outdoor soil to, and within, the indoor environment by track-in on footwear. Implementations of the DIRT model examined the influence of room size, rug area and location, shoe size, and mass transfer coefficients for smooth and carpeted floor surfaces using the ratio of mass loading on carpeted to smooth floor surfaces as a performance metric. Results showed that in the limit for large numbers of random steps the dual aspects of deposition to and track-off from the carpets govern this ratio. Using recently obtained experimental measurements, historic transport and distribution parameters, cleaning efficiencies for the different floor surfaces, and indoor dust deposition rates to provide model boundary conditions, DIRT predicts realistic floor surface loadings. The spatio-temporal variability in model predictions agrees with field observations and suggests that floor surface dust loadings are constantly in flux; steady state distributions are hardly, if ever, achieved. A contribution from ESF Center for the Urban Environment.     

Modelling deposition and air concentration of reduced nitrogen in Poland and sensitivity to variability in annual meteorology

The relative contribution of reduced nitrogen to acid and eutrophic deposition in Europe has increased recently as a result of European policies which have been successful in reducing SO(2) and NO(x) emissions but have had smaller impacts on ammonia (NH(3)) emissions. In this paper the Fine Resolution Atmospheric Multi-pollutant Exchange (FRAME) model was used to calculate the spatial patterns of annual average ammonia and ammonium (NH(4)(+)) air concentrations and reduced nitrogen (NH(x)) dry and wet deposition with a 5 km × 5 km grid for years 2002-2005. The modelled air concentrations of NH(3) and dry deposition of NH(x) show similar spatial patterns for all years considered. The largest year to year changes were found for wet deposition, which vary considerably with precipitation amount. The FRAME modelled air concentrations and wet deposition are in reasonable agreement with available measurements (Pearson's correlation coefficients above 0.6 for years 2002-2005), and with spatial patterns of concentrations and deposition of NH(x) reported with the EMEP results, but show larger spatial gradients. The error statistics show that the FRAME model results are in better agreement with measurements if compared with EMEP estimates. The differences in deposition budgets calculated with FRAME and EMEP do not exceed 17% for wet and 6% for dry deposition, with FRAME estimates higher than for EMEP wet deposition for modelled period and lower or equal for dry deposition. The FRAME estimates of wet deposition budget are lower than the measurement-based values reported by the Chief Inspectorate of Environmental Protection of Poland, with the differences by approximately 3%. Up to 93% of dry and 53% of wet deposition of NH(x) in Poland originates from national sources. Over the western part of Poland and mountainous areas in the south, transboundary transport can contribute over 80% of total (dry + wet) NH(x) deposition. The spatial pattern of the relative contribution of national sources to total deposition of NH(x) may change significantly due to the general circulation of air.     

辽宁省大气湿沉降化学特征分析

通过分析降水酸度、化学特征和湿沉降量等酸沉降控制指标,得出2009年辽宁省大气湿沉降化学特征。研究发现,辽宁省总体上酸雨污染并不严重,但区域性污染突出;降水化学污染严重,呈地域分布不平衡特征,重污染城市位于辽宁省西部和中部;湿沉降量的空间分布与降水化学污染不同,沉降量大的城市位于东部和南部沿海,所有离子湿沉降量最大值均出现在夏季。     

Modelling ice and wax formation in a pipeline in the Arctic environment

In the Arctic environment, the fluid temperature in the pipeline can drop below the freezing point of water, which causes wax and ice to form on the pipeline surface. Solid formation on the pipeline surface can lead to flow assurance and process safety issues, such as blockage of the pipeline, pipeline component failure, and release of hazardous liquid. Remediating the plugging requires a shutdown of pipeline operation, which incurs tremendous cost and delays the entire production system. In order to prevent blockage, the pigging operation can be used to remove the deposits on the pipeline surface on a regular interval. Ice and wax depositions in the pipeline are a slow process. However, if the deposition grows too thick, pipeline blockage can still occur after pigging operation. So, ice and wax deposition rates are required to be estimated accurately. This paper investigates ice and wax deposition rates in a 90,000 m pipeline. A fundamental model for both ice and wax deposition is proposed using the first principles of heat and mass transfer.     

210Pb deposition in the far East Asia: controlling factors of its spatial and temporal variations

In order to better understand the behavior of ²¹⁰Pb deposition in Far East Asia, comprehensive data of monthly ²¹⁰Pb deposition, which includes several time-series and spatial distribution data at 14 stations in Japan and 2 stations in Taiwan, were analyzed. Pb-210 deposition at most of the sites exhibited a typical seasonal change with higher values in winter and lower values in summer; especially, the greatest ²¹⁰Pb deposition in the world occurred in winter at sites beside the Japan Sea. The deposition behavior of ²¹⁰Pb in Far East Asia differed between winter and summer. The meteorological phenomenon peculiar to winter of the Japan Sea side, i.e., formation of the Japan Sea convergence zone, might cause the high ²¹⁰Pb concentration in rainwater, as may heavy snowfall. The ²¹⁰Pb concentration in rainwater showed long-term variability, although this differed between winter and summer. This long-term variability may be related to climatological factors such as El Niño.     

Biomagnetic monitoring of industry-derived particulate pollution

Clear association exists between ambient PM₁₀ concentrations and adverse health outcomes. However, determination of the strength of associations between exposure and illness is limited by low spatial-resolution of particulate concentration measurements. Conventional fixed monitoring stations provide high temporal-resolution data, but cannot capture fine-scale spatial variations. Here we examine the utility of biomagnetic monitoring for spatial mapping of PM₁₀ concentrations around a major industrial site. We combine leaf magnetic measurements with co-located PM₁₀ measurements to achieve inter-calibration. Comparison of the leaf-calculated and measured PM₁₀ concentrations with PM₁₀ predictions from a widely-used atmospheric dispersion model indicates that modelling of stack emissions alone substantially under-predicts ambient PM₁₀ concentrations in parts of the study area. Some of this discrepancy might be attributable to fugitive emissions from the industrial site. The composition of the magnetic particulates from vehicle and industry-derived sources differ, indicating the potential of magnetic techniques for source attribution.     

Influence of ionic strength and pH on the limitation of latex microsphere deposition sites on iron-oxide coated sand by humic acid

This study, for the first time, investigates and quantifies the influence of slight changes in solution pH and ionic strength (IS) on colloidal microsphere deposition site coverage by Suwannee River Humic Acid (SRHA) in a column matrix packed with saturated iron-oxide coated sand.Triple pulse experimental (TPE) results show adsorbed SRHA enhances microsphere mobility more at higher pH and lower IS and covers more sites than at higher IS and lower pH. Random sequential adsorption (RSA) modelling of experimental data suggests 1 μg of adsorbed SRHA occupied 9.28 ± 0.03 × 10⁹ sites at pH7.6 and IS of 1.6 mMol but covered 2.75 ± 0.2 × 10⁹ sites at pH6.3 and IS of 20 mMol. Experimental responses are suspected to arise from molecular conformation changes whereby SRHA extends more at higher pH and lower ionic strength but is more compact at lower pH and higher IS. Results suggest effects of pH and IS on regulating SRHA conformation were additive.     

The simulation of long-range transport of ¹³⁷Cs from East Asia to Japan in 2002 and 2006

To evaluate the quantities of ¹³⁷Cs from past nuclear tests being transported to and deposited in Japan by naturally-occurring phenomena, the authors developed long-range transport models for ¹³⁷Cs considering Asian dust. The simulation using these models backed the observed recent increase of ¹³⁷Cs deposition along the coast of the Sea of Japan in early spring. For the sake of public safety, it is vital to ascertain whether an increase of radioactive deposition is caused by natural phenomena or a nuclear accident. The observations in recent years have suggested that dust and soil containing ¹³⁷Cs is transported from the regions around Inner Mongolia to Japan by the wind. In this paper, using observation data from the early spring of 2002 and 2006, the authors have found good agreement between the simulations and the measurements. The simulations reproduced the entrainment of ¹³⁷Cs and subsequent transport to Japan caused by strong winds associated with low pressure areas around the Inner Mongolian grasslands. The most likely cause of high-level ¹³⁷Cs deposition over northern Japan during March 2002 was ¹³⁷Cs associated with particles transported at low-altitude (1 km) and subjected to precipitation on the 22nd to 24th.     

Chemical fate,latitudinal distribution and long-range transport of cyclic volatile methylsiloxanes in the global environment: A modeling assessment

Cyclic volatile methylsiloxanes (cVMS) such as octamethycyclotetrasiloxane (D4), decamethycyclopentasiloxane (D5), and dodecamethylcyclohexasiloxane (D6) are widely used as intermediates in the synthesis of high-molecular weight silicone polymers or as ingredients in the formulation of personal care products. The global environmental fate, latitudinal distribution, and long range transport of those cVMS were analyzed by two multimedia chemical fate models using the best available physicochemical properties as inputs and known persistent organic pollutants (POPs) and highly persistent volatile organic chemicals (“fliers”) as reference. The global transport and accumulation characteristics of cVMS differ from those of typical POPs in three significant ways. First, a large fraction of the released cVMS tends to become airborne and is removed from the global environment by degradation in air, whereas known POPs have a tendency to be distributed and persistent in all media. Secondly, although cVMS can travel a substantial distance in the atmosphere, they have little potential for deposition to surface media in remote regions. This contrasts with a deposition potential of known POPs that exceeds that of cVMS by 4–5 orders of magnitude. Thirdly, cVMS have short global residence times with the majority of the global mass removed within 3 months of the end of release. Global residence times of POPs on the other hand are in years. The persistent fliers resemble the cVMS with respect to the first two attributes, but their global residence times are more like those of the POPs.