Modelling and mapping long-term risks due to reactive nitrogen effects: an overview of LRTAP convention activities

Long-range transboundary air pollution has caused severe environmental effects in Europe. European air pollution abatement policy, in the framework of the UNECE Convention on Long-range Transboundary Air Pollution (LRTAP Convention) and the European Union Clean Air for Europe (CAFE) programme, has used critical loads and their exceedances by atmospheric deposition to design emission abatement targets and strategies. The LRTAP Convention International Cooperative Programme on Modelling and Mapping Critical Loads and Levels and Air Pollution Effects, Risks and Trends (ICP M&M) generates European critical loads datasets to enable this work. Developing dynamic nitrogen flux models and using them for a prognosis and assessment of nitrogen effects remains a challenge. Further research is needed on links between nitrogen deposition effects, climate change, and biodiversity.     

Po-210 and Pb-210 as atmospheric tracers and global atmospheric Pb-210 fallout: a review

Over the past ∼5 decades, the distribution of ²²²Rn and its progenies (mainly ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po) have provided a wealth of information as tracers to quantify several atmospheric processes that include: i) source tracking and transport time scales of air masses; ii) the stability and vertical movement of air masses iii) removal rate constants and residence times of aerosols; iv) chemical behavior of analog species; and v) washout ratios and deposition velocities of aerosols. Most of these applications require that the sources and sink terms of these nuclides are well characterized.Utility of ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po as atmospheric tracers requires that data on the ²²²Rn emanation rates is well documented. Due to low concentrations of ²²⁶Ra in surface waters, the ²²²Rn emanation rates from the continent is about two orders of magnitude higher than that of the ocean. This has led to distinctly higher ²¹⁰Pb concentrations in continental air masses compared to oceanic air masses. The highly varying concentrations of ²¹⁰Pb in air as well the depositional fluxes have yielded insight on the sources and transit times of aerosols. In an ideal enclosed air mass (closed system with respect to these nuclides), the residence times of aerosols obtained from the activity ratios of ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb are expected to agree with each other, but a large number of studies have indicated discordance between the residence times obtained from these three pairs. Recent results from the distribution of these nuclides in size-fractionated aerosols appear to yield consistent residence time in smaller-size aerosols, possibly suggesting that larger size aerosols are derived from resuspended dust. The residence times calculated from the ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb activity ratios published from 1970’s are compared to those data obtained in size-fractionated aerosols in this decade and possible reasons for the discordance is discussed with some key recommendations for future studies.The existing global atmospheric inventory data of ²¹⁰Pb is re-evaluated and a ‘global curve’ for the depositional fluxes of ²¹⁰Pb is established. A current global budget for atmospheric ²¹⁰Po and ²¹⁰Pb is also established. The relative importance of dry fallout of ²¹⁰Po and ²¹⁰Pb at different latitudes is evaluated. The global values for the deposition velocities of aerosols using ²¹⁰Po and ²¹⁰Pb are synthesized.     

Pollution characteristics of atmospheric dustfall and heavy metals in a typical inland heavy industry city in China

Through field sampling of atmospheric dustfall in regions of Zhuzhou City, China for a period of one year, the deposition fluxes of atmospheric dustfall and five heavy metals contained inside, including Cr, As, Cd, Hg and Pb, were analyzed. Meanwhile the enrichment factor and index methods were used to analyze the pollution characteristics of heavy metals of atmospheric dustfall in Zhuzhou. The annual deposition flux of atmospheric dustfall in Zhuzhou was 50.79 g/(m~2·year), while the annual deposition fluxes of Cr, As, Cd, Hg and Pb were 9.80, 59.69, 140.09, 0.87 and 1074.91 mg/(m~2·year), respectively.The pollution level of atmospheric dustfall in Zhuzhou was relatively lower compared with most other cities in China, but the deposition fluxes of As, Cd, Hg and Pb in atmospheric dustfall in Zhuzhou were much higher than that in most cities and regions around the world. Cd is the typical heavy metal element in atmospheric dustfall in Zhuzhou, and both the enrichment factor and pollution index of Cd were the highest. Cd, Hg, Pb and As in atmospheric dustfall were mainly from human activities. According to the single-factor index, Nemerow index and pollution load index analyses, the atmospheric dustfall in Zhuzhou could easily cause severe heavy metal pollution to urban soil, and the most polluting element was Cd, followed by Pb, As and Hg. Only the pollution level of Cr lay in the safety region and mainly originated from natural sources.     

Validation of modeling approach to evaluate congener-specific concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans in air and soil near a solid waste incinerator

A concise modeling approach using long-term averaged meteorological data was developed to estimate site-specific concentrations of congeners of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) near a solid waste incinerator. This approach consists of calculation of atmospheric dispersion, dry and wet deposition of gaseous and particle-bound congeners, and non-steady-state concentrations in soil. The predictability of this approach was evaluated by comparison of calculated concentrations of congeners in soil with those measured at eight locations near a municipal solid waste incinerator (MSWI). The variation of these concentrations due to variability of meteorological parameters is small. A considerable number of mean values show good agreement with measured concentrations within a factor of three. The reasonable agreement between calculated and measured concentrations indicates that algorithms for the calculation of vapor-phase deposition and non-steady-state concentrations in soil must be included in the modeling approach for an accurate estimation of the concentrations of congeners of PCDD/Fs emitted from MSWIs to the atmosphere. For a detailed estimation of site-specific concentrations, it is important to specify the bulk density of soil in the evaluated area, together with meteorological parameters.     

Rapid measurement of indoor mass-transfer coefficients

Indoor air pollutant concentrations can be influenced by how rapidly species are transported to and from surfaces. Consequently, a greater understanding of indoor transport phenomena to surfaces improves estimates of human exposure to indoor air pollutants. Here, we introduce two methods of rapidly and directly measuring species fluxes at indoor surfaces, allowing us to evaluate the transport-limited deposition velocity, v_t (a mass-transfer coefficient). The deposition velocity sensor (DeVS) method employs a small microbalance coated with a pure hydrocarbon, preferably octadecane. We quantify flux (or evaporation rate) of the hydrocarbon into a room by observing the rate of mass loss on the microbalance. The transport-limited deposition velocity, v_t,octadecane, is then obtained by combining the flux with the vapor pressure of the hydrocarbon. Simultaneously, v_t,ozone is quantified using the deposition velocity of ozone (DeVO) method, which acts as a standard to calibrate and evaluate DeVS. Specifically, DeVO evaluates ozone transport to surfaces by quantifying the conversion by ozone of nitrite to nitrate on a glass fiber filter. Simultaneous laboratory chamber experiments demonstrates that v_t for octadecane and ozone are strongly correlated, with the values for ozone 1.5 times greater than that for octadecane. In an office experiments, the DeVS method responds within minutes to step changes in conditions such as occupancy, activities and ventilation. At present, the results are in order-of-magnitude agreement with predicted indoor mass-transfer coefficients.     

Laboratory Measurement of Dry Deposition of Ozone onto Northern Chinese Soil Samples

We used laboratory experiments to investigate surface resistance (R _c) to dry deposition of ozone (O₃) on different types of soil samples collected from the arid deserts and the Loess Plateau of northern China. Furthermore, we measured the factors that affected R _c, which depends on the physical and chemical interaction between trace constituents and the deposition surface, and evaluated deposition velocity (V _d). There was little influence of geometric surface area, soil weight, or O₃ concentration on V _d of O₃. The effect of relative humidity (RH) (i.e. moisture content of the soil) on O₃ uptake was in agreement with results reported in the literature: a distinct RH dependence of V _d and little uptake under water-saturated conditions were observed. R _c values for all the soil samples examined were in the range 0.21–3.3 s mm⁻¹ and were exponentially related to the surface area of the particles and the organic carbon content of each soil sample at RH of both <10 and 60%.     

骆马湖现代沉积物137Cs和210Pbex的测定分析与环境指示意义

选取骆马湖进湖口、湖中心和出湖口3个位置的沉积物柱芯样品,采用放射性核素137Cs、210Pbex纪年技术定年,对其垂向分布特征及沉积速率指标变化对比分析,并测定沉积物中重金属垂直剖面分布。结果表明：137Cs数值较低,不足以建立137Cs计年时标;210Pbex比活度随深度增加大致呈指数降低,采用210Pbex CIC模式计算获得3个采样点的平均沉积速率及对应的沉积年代区间,进湖口相比湖中心和出湖口沉积速率较低,这与人为活动和水流因素有关;近50年来,骆马湖重金属污染物蓄积峰值总体出现在1975—1977年及1989—1994年两个时期,在2008年之后重金属的蓄积特征呈现逐渐增加趋势     

Relation between forest vegetation, atmospheric deposition and site conditions at regional and European scales

Several monitoring programs have been set up to assess effects of atmospheric deposition on forest ecosystems. The aim of the present study was to evaluate effects on the understorey vegetation, based on the first round of a regional (the Netherlands) and a European forest monitoring program. A multivariate statistical analysis showed surprisingly similar results for both data sets; the vegetation appeared to be largely determined by the ‘traditional’ factors soil, climate, and tree species, but there was a small but statistically significant effect of atmospheric deposition. The effects of deposition include a slight shift towards nitrophytic species at high N deposition in the European network, and towards acidophytic species at high S-deposition in the Dutch network. The relatively small effect of atmospheric deposition is understandable in view of the very large natural variation in environmental conditions. Time series of both vegetation and environment are needed to assess deposition effects in detail.     

Rates of particulate pollution deposition onto leaf surfaces: Temporal and inter-species magnetic analyses

Evaluation of health impacts arising from inhalation of pollutant particles <10 μm (PM₁₀) is an active research area. However, lack of exposure data at high spatial resolution impedes identification of causal associations between exposure and illness. Biomagnetic monitoring of PM₁₀ deposited on tree leaves may provide a means of obtaining exposure data at high spatial resolution. To calculate ambient PM₁₀ concentrations from leaf magnetic values, the relationship between the magnetic signal and total PM₁₀ mass must be quantified, and the exposure time (via magnetic deposition velocity (MV_d) calculations) known. Birches display higher MV_d (∼5 cm⁻¹) than lime trees (∼2 cm⁻¹). Leaf saturation remanence values reached ‘equilibrium’ with ambient PM₁₀ concentrations after ∼6 ‘dry’ days (<3 mm/day rainfall). Other co-located species displayed within-species consistency in MV_d; robust inter-calibration can thus be achieved, enabling magnetic PM₁₀ biomonitoring at unprecedented spatial resolution.     

Wet deposition of poly- and perfluorinated compounds in Northern Germany

Twenty precipitation samples were taken concurrently with air samples at a northern German monitoring site over a period of 7 months in 2007 and 2008. Thirty four poly- and perfluorinated compounds (PFC) were determined in rain water samples by solid phase extraction and HPLC-MS/MS analysis. Seventeen compounds were detected in rain water with ΣPFC concentrations ranging from 1.6 ng L⁻¹ to 48.6 ng L⁻¹. Perfluorooctanoate (PFOA) and perfluorobutanate (PFBA) were the compounds that were usually observed in highest concentrations. Calculated ΣPFC deposition rates were between 2 and 91 ng m⁻² d⁻¹. These findings indicate that particle phase PFC are deposited from the atmosphere by precipitation. A relationship between PFC wet deposition and air concentration may be established via precipitation amounts. Trajectory analysis revealed that PFC concentration and deposition estimates in precipitation can only be explained if a detailed air mass history is considered.