大气气溶胶中重金属元素痕量分析及形态分析研究进展

重金属是大气气溶胶的重要组成部分,由于重金属的气候效应、环境效应和健康效应,其痕量分析和形态分析越来越受重视.综述了大气气溶胶的采集、重金属的总量分析及形态分析技术,指出了当前研究工作中存在的问题及今后的发展方向.     

Assessment of atmospheric sulfur with the epilithic moss Haplocladium microphyllum: Evidences from tissue sulfur and δS analysis

The application of geochemical signals in mosses is more and more popular to investigate the deposition of atmospheric pollutants, but it is unclear whether records of atmospheric sulfur in mosses differ between their diverse habitats. This study aimed to investigate the influence of growing condition on tissue sulfur and δ³⁴S of Haplocladium microphyllum. Epilithic and terricolous mosses in open fields, mosses under different canopy conditions were considered. We found that tissue sulfur and δ³⁴S of mosses under different habitats were not consistent and could not be compared for atmospheric sulfur research with each other even collected at the same site, moss sulfur and δ³⁴S records would be distorted by subsoil and upper canopies in different degrees, which possibly mislead the interpretation of atmospheric sulfur level and sources. Consequently, mosses on open rocks can be used reliably to assess atmospheric-derived sulfur in view of their identical sulfur and δ³⁴S evidences.     

Ocean to continent transfer of atmospheric Se as revealed by epiphytic lichens

There is still a long-term debate concerning the relative contributions of naturally emitted and anthropogenic Se at the regional and local scales. Here, Se and heavy metal concentrations are reported for epiphytic lichens collected in coastal and inland areas from the USA, Canada and France for assessing atmospheric Se source. Correlations found between Se and Cl in lichens confirmed the major marine biogenic source for atmospheric Se. Continental samples do not show systematic relationships between Se and other metal (Pb, Cu, In …) contents, even for lichens collected in the vicinity of smelters or close to urban areas. Our results suggest that, although anthropogenic Se may be present, the marine biogenic Se source is a major contributor to atmospheric Se for our sampling locations. The contribution of naturally emitted atmospheric Se may be significant in urban and industrial areas and should be taken into account for further studies.     

Atmospheric mercury concentrations and speciation measured from 2004 to 2007 in Reno, Nevada, USA

Atmospheric elemental, reactive and particulate mercury (Hg) concentrations were measured north of downtown Reno, Nevada, USA from November 2004 to November 2007. Three-year mean and median concentrations for gaseous elemental Hg (Hg⁰) were 1.6 and 1.5 ng m⁻³ (respectively), similar to global mean Hg⁰ concentrations. The three-year mean reactive gaseous Hg (RGM) concentration (26 pg m⁻³) was higher than values reported for rural sites across the western United States. Well defined seasonal and daily patterns in Hg⁰ and RGM concentrations were observed, with the highest Hg⁰ concentrations measured in winter and early morning, and RGM concentrations being greatest in the summer and mid-afternoon. Elevated Hg⁰ concentrations in winter were associated with periods of cold, stagnant air; while a regularly observed early morning increase in concentration was due to local source and surface emissions. The observed afternoon increase and high summer values of RGM can be explained by in situ oxidation of gaseous Hg⁰ or mixing of RGM derived from the free troposphere to the surface. Because both of these processes are correlated with the same environmental conditions it is difficult to assess their overall contribution to the observed trends.     

Natural and anthropogenic radionuclides in airborne particulate samples collected in Barcelona (Spain)

Results for naturally occurring ⁷Be, ²¹⁰Pb, ⁴⁰K, ²¹⁴Bi, ²¹⁴Pb, ²¹²Pb, ²²⁸Ac and ²⁰⁸Tl and anthropogenic ¹³⁷Cs in airborne particulate matter in the Barcelona area during the period from January 2001 to December 2005 are presented and discussed. The ²¹²Pb and ²⁰⁸Tl, ²¹⁴Bi and ²¹⁴Pb, ⁷Be and ²¹⁰Pb radionuclide levels showed a significant correlation with each other, with correlation coefficients of 0.99, 0.78 and 0.69, respectively, suggesting similar origin/behaviour of these radionuclides in the air. Caessium-137 and Potassium-40 were transported to the air as resuspended particle from the soil. The ⁷Be and ²¹⁰Pb concentrations showed similar seasonal variations, with a tendency for maximum concentrations during the summer months. An inverse relationship was observed between the ⁷Be, ²¹⁰Pb, ⁴⁰K and ¹³⁷Cs concentrations and weekly rainfall, indicating washout of atmospheric aerosols carrying these radionuclides.     

The Bulgarian Emergency Response System for dose assessment in the early stage of accidental releases to the atmosphere

The Bulgarian Emergency Response System (BERS) is being developed in the Bulgarian National Institute of Meteorology and Hydrology since 1994. BERS is based on numerical weather forecast meteorological information and a numerical long-range dispersion model accounting for the transport, dispersion, chemical and radioactive transformations of pollutants. In the present paper, the further development of this system for a mixture of radioactive gaseous and aerosol pollutants is described. The basic module for the BERS, the numerical dispersion model EMAP, is upgraded with a “dose calculation block”. Two scenarios for hypothetical accidental atmospheric releases from two NPPs, one in Western, and the other in Eastern Europe, are numerically simulated. The effective doses from external irradiation, from air submersion and ground shinning, effective dose from inhalation and absorbed dose by thyroid gland formed by 37 different radionuclides, significant for the early stage of a nuclear accident, are calculated as dose fields for both case studies and discussed.     

Beryllium-7 atmospheric deposition and sediment inventories in the Neponset River estuary,Massachusetts, USA

Measured monthly atmospheric depositional fluxes of cosmogenically produced ⁷Be ranged from 1 to 67 mBq/cm² in Boston, Massachusetts between September 2000 and August 2007. These fluxes exhibited seasonality and supported a decay-corrected ⁷Be atmospheric depositional running inventory that ranged from 36 to 144 mBq/cm². Annual ⁷Be deposition exhibited an increasing trend that may reflect a general decrease in solar activity and a general increase in precipitation over the 7-year sampling period. To investigate short-term sediment dynamics and accumulation patterns in the Neponset River estuary, we collected six sediment cores in July 2006 and measured ⁷Be sediment inventories ranging from 48 to 546 mBq/cm² Comparisons of these sediment inventories with the ⁷Be running inventory from atmospheric deposition (101 mBq/cm²) at the time of core collection indicated a large degree of spatial heterogeneity in sediment accumulation patterns and its potential use as a tool for assessing the impacts of environmental restoration activities in estuarine environments.     

Allocation and source attribution of lead and cadmium in maize (Zea mays L.) impacted by smelting emissions

Plants grown in contaminated areas may accumulate trace metals to a toxic level via their roots and/or leaves. In the present study, we investigated the distribution and sources of Pb and Cd in maize plants (Zea mays L.) grown in a typical zinc smelting impacted area of southwestern China. Results showed that the smelting activities caused significantly elevated concentrations of Pb and Cd in the surrounding soils and maize plants. Pb isotope data revealed that the foliar uptake of atmospheric Pb was the dominant pathway for Pb to the leaf and grain tissues of maize, while Pb in the stalk and root tissues was mainly derived from root uptake. The ratio of Pb to Cd concentrations in the plants indicated that Cd had a different behavior from Pb, with most Cd in the maize plants coming from the soil via root uptake.     

Ecosystem responses to reduced and oxidised nitrogen inputs in European terrestrial habitats

While it is well established that ecosystems display strong responses to elevated nitrogen deposition, the importance of the ratio between the dominant forms of deposited nitrogen (NH_x and NO_y) in determining ecosystem response is poorly understood. As large changes in the ratio of oxidised and reduced nitrogen inputs are occurring, this oversight requires attention. One reason for this knowledge gap is that plants experience a different NH_x:NO_y ratio in soil to that seen in atmospheric deposits because atmospheric inputs are modified by soil transformations, mediated by soil pH. Consequently species of neutral and alkaline habitats are less likely to encounter high NH₄⁺ concentrations than species from acid soils. We suggest that the response of vascular plant species to changing ratios of NH_x:NO_y deposits will be driven primarily by a combination of soil pH and nitrification rates. Testing this hypothesis requires a combination of experimental and survey work in a range of systems.     

Atmospheric oxidation mechanisms of polychlorinated dibenzo-p-dioxins are different from those of benzene and dibenzofuran: a theoretical prediction

The reaction mechanisms of dibenzo-p-dioxin (DD) and 2,3,7,8-TCDD with OH radical have been studied using density functional theory calculations. Under the atmospheric conditions, ca 42% of DD + OH reaction proceeds as formation of DD − OH-β adduct, which will react with O₂ slowly; while the rest will proceed as formation of DD − OH-γ adduct, which will decompose to the substituted phenoxy radical P1 by the fused-ring C-O bond cleavage. For 2,3,7,8-TCDD + OH, the reaction will predominantly form the substituted phenoxy radical P2. The reaction mechanisms are drastically different from the peroxy mechanism for the atmospheric oxidations of benzene and dibenzofuran.