Chloroform in the environment: occurrence,sources, sinks and effects

The chloroform flux through the environment is apparently constant at some 660±220 Gg yr⁻¹ (±1σ) and about 90% of the emissions are natural in origin: the largest single source being in offshore sea water (contributing 360±90 Gg yr⁻¹), with soil processes the next most important (220±100 Gg yr⁻¹). Other natural sources, mainly volcanic and geological, account for less than 20 Gg yr⁻¹. The non-natural sources total 66±23 Gg yr⁻¹ and are much better characterised than the natural sources. They are predominantly the result of using strong oxidising agent on organic material in the presence of chloride ion, a direct parallel with the natural processes occurring in soils.

Chloroform partitions preferentially into the atmosphere; the equilibrium distribution is greater than 99% and the average global atmospheric concentration has been calculated to be 18.5 pmol mol⁻¹. Atmospheric oxidation, the principal removal process, is approximately in balance with the identified source fluxes. Chloroform is widely dispersed in the aquatic environment (even naturally present in some mineral waters). Consequently, it is also widely dispersed in the tissue of living creatures and in foodstuffs but there is little evidence of bioaccumulation and the quantities in foodstuffs and drinking water are not problematical for human ingestion at the highest concentrations found. Definitive studies have shown that current environmental concentrations of chloroform do not present an ecotoxicological risk, even to fish at the embryonic and larval stages when they are most susceptible.

By virtue of the very small amounts that actually become transported to the stratosphere, chloroform does not deplete ozone materially, nor is it a photochemically active volatile organic compound (VOC). It has a global warming potential that is less than that of the photochemically active VOCs and is not classed as a greenhouse gas.     

Persistent toxic substances in remote lake and coastal sediments from Svalbard, Norwegian Arctic: Levels, sources and fluxes

Surface sediments from remote lakes and coastal areas from Ny-Ålesund, Svalbard, Norwegian Arctic were analyzed for polycyclic aromatic hydrocarbons (PAHs), polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs). Relatively high levels of PAHs were encountered from several lakes from Ny-Ålesund, which were within the range of levels reported for European high mountain lakes and some urban/industrialized areas in the world, pointing to the role of remote Arctic lakes as potential reservoir of semi-volatile organic compounds. Specific patterns of PBDEs were observed, showing higher concentrations of lower brominated compounds such as BDE-7, 17 and 28. Estimated surface sediment fluxes of PAHs in Ny-Ålesund remote lakes were similar to those observed for some European high mountain lakes. The current PAH levels in sediments from three lakes exceeded Canadian sediment quality guidelines, suggesting the presence of possible risks for aquatic organisms and the need for further studies.     

The significance of PCBs in the atmosphere of the southern hemisphere

Air monitoring stations were set up at 2 sites in the southern hemisphere--Moody Brook, Falkland Island (51 degrees 25' S, 57 degrees 56' W) and Halley, Research Station, Antarctica (75 degrees 35' S, 26 degrees 30' W). PCBs were monitored at the stations throughout 1999. Highest concentrations were observed when temperatures were greater. In general, concentrations were greater at Moody Brook than at Halley, although the difference in concentrations between sites was less for more chlorinated congeners. Air concentrations at both sites were compared with samples collected nearby over-water. Over water air concentrations were found to be greater than over land air concentrations. Concentrations were also compared with literature data for air concentrations at a remote site in the Canadian Arctic. Atmospheric concentrations of tri-chlorinated biphenyls were found to be approximately double those reported for Ellesmere Island in the Canadian Arctic, whilst concentrations in samples from Antarctica were very similar to those found in the high Arctic. Most other PCBs were a factor of 2-4 greater in the Canadian Arctic.     

Polyfluorinated compounds in the atmosphere along a cruise pathway from the Japan Sea to the Arctic Ocean

Neutral polyfluorinated alkyl substances (PFASs) were measured in high-volume air samples collected on board the research vessel Snow Dragon during the 4th Chinese National Arctic Expedition from the Japan Sea to the Arctic Ocean in 2010. Four volatile and semi-volatile PFASs (fluorotelomer alcohols (FTOHs), fluorotelomer acids (FTAs), perfluoroalkyl sulfonamides (FASAs), and sulfonamidoethanols (FASEs)) were analyzed respectively in the gas and particle phases. FTOHs were the dominant PFASs in the gas phase (61-358 pg m⁻³), followed by FTAs (5.2-47.9 pg m⁻³), FASEs (1.9-15.0 pg m⁻³), and FASAs (0.5-2.1 pg m⁻³). In the particle phase, the dominant PFAS class was FTOHs (1.0-9.9 pg m⁻³). The particle-associated fraction followed the general trend of FASEs > FASAs > FTOHs. Compared with other atmospheric PFAS measurements, the ranges of concentrations of ∑FTOH in this study were similar to those reported from Toronto, north America (urban), the northeast Atlantic Ocean, and northern Germany. Significant correlations between FASEs in the gas phase and ambient air temperature indicate that cold surfaces such as sea-ice, snowpack, and surface seawater influence atmospheric FASEs.     

Pesticides in the groundwater of a spring draining a sandy aquifer: temporal variability of concentrations and fluxes

A 250 ha agricultural catchment has been characterized with respect to its hydrogeology and groundwater contamination by pesticides from October 1999 to August 2004. Five years after the ending of atrazine (At) application, used since the sixties, At and deethylatrazine (DEA) are still systematically quantified at the outlet of the watershed with concentrations from 0.07 to 0.43 microg l(-1) for At, and between 0.14 and 1.16 microg l(-1) for DEA. Isoproturon and chlortoluron are detected in only one (0.3 microg l(-1)) and two (0.7 and 2.0 microg l(-1)) of the 124 semi-monthly samples, respectively. DEA concentrations can be very different between two samples with a 15-day time step. The annual mean exported fluxes of cumulated At and DEA are stable, which indicates a long time transfer in the unsaturated or saturated zone with a progressive leaching of the stock of At and DEA probably accumulated in the soil and the vadose zone. These fluxes, between 0.90% and 2.82% of the annual mean dose of At applied before 1999, similar to those calculated in several studies at the bottom of the root zone, could be explained by low adsorption and degradation properties of At and DEA in the unsaturated and saturated zone.     

Lichen-based critical loads for atmospheric nitrogen deposition in Western Oregon and Washington Forests, USA

Critical loads (CLs) define maximum atmospheric deposition levels apparently preventative of ecosystem harm. We present first nitrogen CLs for northwestern North America’s maritime forests. Using multiple linear regression, we related epiphytic-macrolichen community composition to: 1) wet deposition from the National Atmospheric Deposition Program, 2) wet, dry, and total N deposition from the Communities Multi-Scale Air Quality model, and 3) ambient particulate N from Interagency Monitoring of Protected Visual Environments (IMPROVE). Sensitive species declines of 20-40% were associated with CLs of 1-4 and 3-9 kg N ha⁻¹ y⁻¹ in wet and total deposition. CLs increased with precipitation across the landscape, presumably from dilution or leaching of depositional N. Tight linear correlation between lichen and IMPROVE data suggests a simple screening tool for CL exceedance in US Class I areas. The total N model replicated several US and European lichen CLs and may therefore be helpful in estimating other temperate-forest lichen CLs.     

Atmospheric pollutants in alpine peat bogs record a detailed chronology of industrial and agricultural development on the Australian continent

Two peat bogs from remote alpine sites in Australia were found to contain detailed and coherent histories of atmospheric metal pollution for Pb, Zn, Cu, Mo, Ag, As, Cd, Sb, Zn, In, Cr, Ni, Tl and V. Dramatic increases in metal deposition in the post-1850 AD portion of the cores coincide with the onset of mining in Australia. Using both Pb isotopes and metals, pollutants were ascribed to the main atmospheric pollution emitting sources in Australia, namely mining and smelting, coal combustion and agriculture. Results imply mining and metal production are the major source of atmospheric metal pollution, although coal combustion may account for up to 30% of metal pollutants. A novel finding of this study is the increase in the otherwise near-constant Y/Ho ratio after 1900 AD. We link this change to widespread and increased application of marine phosphate fertiliser in Australia's main agricultural area (the Murray Darling Basin).     

乌鲁木齐市不同区域大气降尘中重金属污染及来源分析

为进一步了解城市不同区域间大气降尘中重金属含量及其差异性,沿城市走向梯度布设降尘采样点采集样品。采用电感耦合等离子体原子发射光谱(ICP-AES)仪测定样品中Cu、Cr、Mn、Fe、Ni、Zn、Cd、Pb和As等重金属含量,并计算富集因子来判断不同区域间的污染源类型,通过因子分析方法探讨污染的来源。结果显示,所测重金属元素中除Mn外,均受到人为源的影响,且十分严重。从贡献率来看,不同区域间第一因子的贡献率虽有差异,但均为来自土壤的风沙扬尘造成;第二因子的贡献率也不尽相同,主要是燃煤产生的污染;第三因子出现了差异,市南区和市北区主要是受金属冶炼的影响,而市中区的影响可能来自垃圾焚烧;市南区未出现第四因子,而市中区和市北区的污染源也不相同。分析表明,城市大气降尘污染依然严重,做好防控风沙和建筑扬尘,减少煤炭消耗,调整能源结构和产业布局是整体减少大气降尘的关键。     

Manganese in the urban atmosphere: identifying anomalous concentrations and sources

Purpose  

Industrial emissions can raise urban background levels of inhalable Mn particles in an order of magnitude above normal, eclipsing the contribution made by natural sources and traffic.     

Carboxylic acids in the troposphere, occurrence, sources, and sinks: A review

Carboxylic acids are ubiquitous and important components of the troposphere; they are currently measured in different environments. They are thought to have several sources comprising primary biogenic and anthropogenic emissions, hydrocarbons gas-phase oxidations, and some carbonyl compounds aqueous-phase oxidations. In the present review we make a synthesis of the concentrations of low molecular weight carboxylic acids in tropospheric aqueous and gaseous phases and in aerosol particles for different environments. We also successively examine the major sources of carboxylic acids and discuss their relative contribution to tropospheric concentrations for various environments as well as the principal sinks of these compounds.     

Polychlorinated biphenyls (PCBs) in the British environment: sinks, sources and temporal trends

This paper estimates the present UK environmental loading of polychlorinated biphenyls (PCBs). Of the estimated approximately 40,000 t SigmaPCB sold in the UK since 1954, only an estimated 1% (400 t) are now present in the UK environment. Comparisons of estimated production and current environmental loadings of congeners 28, 52, 101, 138, 153 and 180 suggest that PCB persistence broadly increases with increasing chlorination. Those PCBs that are not now present in the UK environment are considered to have been destroyed--by natural or anthropogenic mechanisms, to be still in use, to reside in landfills or to have undergone atmospheric and/or pelagic transport from the UK. The dramatic fall in PCB levels in archived UK soils and vegetation between the mid-1960s and the present is evidence that the latter mechanism is the most important and that a significant proportion of PCBs released into the UK environment in the 1960s have subsequently undergone environmental transport away from the UK. The bulk (93.1%) of the estimated contemporary UK environmental burden of SigmaPCBs is associated with soils, with the rest found in seawater (3.5%) and marine sediments (2.1%). Freshwater sediments, vegetation, humans and sewage sludge combined account for 1.4% of the present burden, whilst PCB loadings in air and freshwater are insignificant. Although consideration of individual congeners does not reveal any major deviations from the relative partitioning of Sigma PCBs, the importance of sinks other than soils is enhanced for individual congeners, particularly 138 and 180. In particular, around 2% of the total UK burden of congener 180 is present in humans, implying that biodata as a whole may constitute an important sink for the higher chlorinated congeners. The contemporary flux of SigmaPCBs to the UK surface is estimated at 19 t yr(-1), compared with an estimated annual flux to the atmosphere of 44-46 t. This implies that the major sources of PCBs to the UK atmosphere have been identified and that there is currently a net loss of these compounds from the UK. These sources are: volatilisation from soils (88.1%), leaks from large capacitors (8.5%), the production of refuse-derived fuel (RDF) (2.2%), leaks from transformers (0.6%), the recovery of contaminated scrap metal (0.5%) and volatilisation from sewage sludge-amended land (0.2%). Interestingly, whilst large excesses of estimated annual fluxes to the atmosphere over deposition fluxes for individual congeners exist for congeners 28, 52 and 101, estimates of fluxes in both directions across the soil-atmosphere interface agree closely for congeners 138, 153 and 180. This suggests that lower chlorinated congeners are more susceptible to both long-range environmental transport beyond the UK and to atmospheric degradation. Retrospective analysis of dated sediment cores, vegetation and soils indicates that environmental transport from North America and continental Europe introduced PCBs into the British environment well before the onset of their commercial production in the UK in 1954. Since that time, the input of PCBs to the UK environment has essentially reflected temporal trends in UK use. After peaking in the 1960s they declined rapidly through the 1970s following restrictions on PCB use. Recent evidence, however, is that the rate of decrease has diminished and that further significant reductions in fresh environmental input will take some time to occur. Such reductions will be especially slow for humans and other biota with long life-spans. This stems partly from cross-generational transfer from parents to offspring and also because the persistence of PCBs in biota means that present body burdens will reflect past as well as current exposure.     

Levels and speciation of arsenic in the atmosphere in Beijing, China

Arsenic levels and speciation in the total suspended particles (TSPs) were quantitatively determined by high performance liquid chromatography on-line coupled with hydride generation atomic fluorescence spectrometry in Beijing, China from February 2009 to March 2011. The high TSP levels fluctuated between 0.07 and 0.79 mg m⁻³, with a mean level of 0.32 ± 0.17 mg m⁻³. The total arsenic concentrations ranged from 0.03 to 0.31 μg m⁻³ (mean: 0.13 ± 0.06 μg m⁻³) in Beijing‘s air. The concentrations of As(III) and As(V) ranged from 0.73 to 20 ng m⁻³ (mean: 4.7 ± 3.6 ng m⁻³) and from 14 to 2.5 × 10² ng m⁻³ (mean: 67 ± 35 ng m⁻³), respectively. As levels and speciation demonstrated relative higher levels in spring and autumn and lower values in summer and winter. As(V) accounted for 81-99% of the extractable species in the TSP samples which showed that As(V) was the major fraction of the extractable As. Organoarsenic species, monomethylarsonate (MMA) and dimethylarsinate (DMA) were not found in all samples. Higher values of enrichment factors demonstrated that arsenic in TSP mainly come from anthropogenic sources. High As and its species levels in air and respiratory exposure (0.30-0.84 μg d⁻¹) attributed to higher excess cancer risk ((4.2 ± 2.0) × 10⁻⁴) for people in Beijing.     

Origin of polluted air masses in the Alps. An overview and first results for MONARPOP

The contribution of ZAMG to MONAROP consists of special weather forecasts to control the SOCs sampling procedure and of the analysis of the specific transport processes for SOCs, which is still in progress.In this paper, air pollutant transport into the Alps is demonstrated by examples of inorganic pollutants: Measurements of NO_x and ozone provide evidence for air pollutant transport by local wind systems (valley and slope winds), especially at low elevated sites of the Alps. In addition, trajectory analyses for the high elevation sites demonstrate the importance of large scale synoptic air pollutant transport. The effects of these transport processes with different spatial and temporal scales are governed by the physical and chemical properties of the particular pollutant.First results for the high alpine MONARPOP stations show that air masses from east Europe influence mostly Sonnblick (Austria), whereas the influence of the Po basin is strongest at Weissfluhjoch (Switzerland).     

Detecting and Coping with Disruptive Shocks in Arctic Marine Systems: A Resilience Approach to Place and People

It seems inevitable that the ongoing and rapid changes in the physical environment of the marine Arctic will push components of the region’s existing social-ecological systems—small and large—beyond tipping points and into new regimes. Ongoing changes include warming, freshening, acidification, and alterations to food web structure. In anticipation we pose three distinct but interrelated challenges: (1) to explore existing connectivities within components of the marine system; (2) to seek indicators (if they exist) of approaching regime change through observation and modeling; and (3) to build functional resilience into existing systems through adaptation-oriented policy and to have in hand transformative options when tipping points are crossed and new development trajectories are required. Each of the above challenges is scale dependent, and each requires a much deeper understanding than we currently have of connectivity within existing systems and their response to external forcing. Here, we argue from a global perspective the need to understand the Arctic’s role in an increasingly nonlinear world; then describe emerging evidence from new observations on the connectivity of processes and system components from the Canada Basin and subarctic seas surrounding northern North America; and finally posit an approach founded in “resilience thinking” to allow northern residents living in small coastal communities to participate in the observation, adaption and—if necessary—transformation of the social-ecological system with which they live.     

Spatial and temporal variations and mobile source emissions of polycyclic aromatic hydrocarbons in Quito, Ecuador

Motor vehicles are a major source of air pollution in Quito, Ecuador; however, little work has been done to characterize spatial and temporal variations in traffic-related pollutants, or to measure pollutants in vehicle emissions. We measured PAH continuously for one year at two residential sites in Quito, and PAH and traffic patterns for one week near a busy roadway. Morning rush-hour traffic and temperature inversions caused daily PAH maxima between 06:00 and 08:00. SO₂, NO_x, CO, and PM_2.5 behaved similarly. At the residential sites PAH levels during inversions were 2-3-fold higher than during the afternoon, and 10-16-fold higher than 02:00-03:00 when levels were lowest. In contrast, at the near-roadway site, PAH concentrations were 3-6-fold higher than at the residential sites, and the effects of inversions were less pronounced. Cars and buses accounted for >95% of PAH at the near-roadway site. Near-roadway PAH concentrations were comparable to other polluted cities.     

Chemical compositions and radiative properties of dust and anthropogenic air masses study in Taipei Basin, Taiwan, during spring of 2004

Asia is one of the major sources of not only mineral dust but also anthropogenic aerosols. Continental air masses associated with the East Asian winter monsoon always contain high contents of mineral dust and anthropogenic species and transported southeastward to Taiwan, which have significant influences on global atmospheric radiation transfer directly by scattering and absorbing solar radiation in each spring. However, few measurements for the long-range transported aerosol and its optical properties were announced in this area, between the Western Pacific and the southeastern coast of Mainland China. The overall objective of this work is to quantify the optical characteristics of different aerosol types in the Eastern Asian. In order to achieve this objective, meteorological parameters, concentrations of PM₁₀ and its soluble species, and optical property of atmospheric scattering coefficients were measured continuously with 1 h time-resolved from 11 February to 7 April 2004 in Taipei Basin (25°00′N, 121°32′E). In this work, the dramatic changes of meteorological parameters such as temperature and winds were used to determine the influenced period of each air mass. Continental, strong continental, marine, and stagnant air masses defined by the back-trajectory analysis and local meteorology were further characterized as long-range transport pollution, dust, clean marine, and local pollution aerosols, respectively, according to the diagnostic ratios. The aerosol mass scattering efficiency of continental pollution, dust, clean marine, and local pollution aerosols were ranged from 1.3 to 1.6, 0.7 to 1.0, 1.4 and 1.4 to 2.3 m² g⁻¹, respectively. Overall, there are two distinct populations of aerosol mass scattering efficiencies, one for an aerosol chemical composition dominated by dust (<1.0 m² g⁻¹) and the other for an aerosol chemical composition dominated by anthropogenic pollutants (1.3–2.3 m² g⁻¹), which were similar to the previous measurements with high degree of temporal resolution.     

Correlations between physicochemical properties of PAHs and their distribution in soil, moss and reindeer dung at Ny-Ålesund of the Arctic

Concentrations of 16 polycyclic aromatic hydrocarbons (PAHs) in soil, moss and reindeer dung collected at Ny-Ålesund of the Arctic were measured to investigate their accumulation trends and distribution in the three compartments. Compared with the other regions, the proportions of 2 + 3 ring PAHs to the total PAHs were higher, whereas the proportions of 5 + 6 ring PAHs were lower in the three compartments at Ny-Ålesund. Significant log/log-linear relationship was observed between the sub-cooled liquid vapor pressure and the soil/moss quotient (Q_SM). The relation was similar to the relationship between the gas/particle partition coefficient (K_P) and of PAHs, implying Q_SM would be a “mirror image” of K_P. Excellent log/log-linear relationships were observed between Q_SM and K_OA as well as between the moss/dung quotient (Q_MD) and K_OW. The results presented here indicate the physicochemical properties are suitable for characterizing the distribution of PAHs in soil, moss and reindeer dung.     

Organochlorine pesticides in the atmosphere of Guangzhou and Hong Kong: Regional sources and long-range atmospheric transport

Organochlorine pesticides (OCPs) were measured in the atmosphere over the period of December 2003–December 2004 at four sampling sites in Guangzhou and Hong Kong. Gas phase and particle phase concentrations of 8 OCP species, including trans-chlordane (t-CHL), cis-chlordane (c-CHL), p,p′-DDT, p,p′-DDE, o,p′-DDT, α-endosulfan, α- and γ-hexachlorocyclohexane (HCH), were studied. OCPs were found predominantly in the gas phase in all seasons. t-CHL, c-CHL, o,p′-DDT, p,p′-DDT and α-endosulfan had significantly (p<0.001) higher concentrations than other OCPs, with mean values (gas+particle) typically ranging from 103 to 1440 pg m⁻³. In general, the concentrations of OCPs in summer were higher than that in winter, except for α-HCH which showed no clear seasonal pattern. Higher levels of γ-HCH and o,p′-DDT found in Guangzhou could be attributed to the present usage of lindane and dicofol in the Pearl River Delta (PRD) region. The very high concentrations of p,p′-DDT and α-endosulfan were observed at all sampling sites. The results of 7 days air back trajectory analysis indicated that the unusual high p,p′-DDT levels in summer in both cities could be related to the seasonal usage of DDT containing antifouling paints for fishing ships in the upwind seaports of the region. The high concentrations of α-endosulfan in winter in the study area suggested an atmospheric transport by the winter monsoon from the East China, where endosulfan is being used as insecticide in cotton fields. The consistency of the seasonal variation of concentrations and isomeric ratios of DDTs and α-endosulfan with the alternation of winter monsoon and summer monsoon suggested that the Asian monsoon plays an important role in the long-range atmospheric transport of OCPs.     

Assessment of 2010 air quality in two Alpine valleys from modelling: Weather type and emission scenarios

Alpine valleys are sensitive to anthropogenic emissions. Local atmospheric dynamics are a key factor that may lead to an accumulation of pollutants in the bottom of the Chamonix and Maurienne valleys. Assessment of 2010 pollutant concentrations variability needs to take these specificities into account. A meteorological data classification is combined with different emission scenarios in order to run an air quality model. Using simulations of representative scenarios rather than complete years allows for a fine spatial and temporal representation of local atmospheric dynamics and gives access to detailed chemical breakdowns. Results demonstrate the variability of primary and secondary species due to emissions and the predominance of local effects on pollutant concentrations.