Biomedical subjects

Andrew J Sweetman

Publications and source records attributed to Andrew J Sweetman.

16 recordsLinked to original sources

PubMed2006

Continental scale passive air sampling of persistent organic pollutants using rapidly equilibrating thin films (POGs).

A novel design of rapidly equilibrating passive air sampler was deployed at 38 sites across 19 European countries to investigate short-term spatial variability of persistent organic pollutants (POPs). Devices were sealed in airtight containers to eliminate the possibility of contamination during transit and couriered to recipients with deployment instructions. Exposure times of 7days permitted the use of back trajectory analysis to further understand the factors responsible for influencing the large-scale spatial distribution of PCBs, PBDEs, PCNs, PAHs, lindane and HCB. Following sampler harvest, devices were sealed and returned for analysis. Comparison of sequestered levels showed that PAHs exhibited the greatest spatial variability (by a factor of 30) with higher levels often associated with greater population density. In contrast, HCB values were much more uniform, reflecting its well mixed distribution in the atmosphere. Spatial variation was strongly influenced by air mass origin, with lower levels being observed at most sites impacted by maritime air masses.

Air Movements↗

PubMed2006

Passive air sampling for persistent organic pollutants: introductory remarks to the special issue.

There have been a number of developments in the need, design and use of passive air samplers (PAS) for persistent organic pollutants (POPs). This article is the first in a Special Issue of the journal to review these developments and some of the data arising from them. We explain the need and benefit of developing PAS for POPs, the different approaches that can be used, and highlight future developments and needs.

Aerosols↗

PubMed2005

Passive air sampling of polychlorinated biphenyls, organochlorine compounds, and polybrominated diphenyl ethers across Asia.

Asia is of global importance economically, yet data on ambient persistent organic pollutant levels are still sparse for the region, despite international efforts under the Stockholm Convention to identify and reduce emissions. A large-scale passive air sampling survey was therefore conducted in Asia, specifically in China, Japan, South Korea, and Singapore. Polyurethane foam disks were deployed simultaneously at 77 sites, between Sept 21 and Nov 16, 2004, and analyzed for polychlorinated biphenyls (PCBs), organochlorine compounds (hexachlorobenzene (HCB), dichlorodiphenyltrichloroethanes (DDTs), chlordane), and polybrominated diphenyl ethers (PBDEs). The meteorological conditions prevailing in the region at this time facilitated the assessment of local/regional differences in atmospheric emissions, because large-scale advection effects due to monsoons or dust storms did not occur. Air concentrations estimated assuming an average sampler uptake rate of 3.5 m3/day ranged as follows (pg m(-3)): PCBs, 5-340; HCB, 10-460; DDTs, 0.4-1800; chlordanes, 1-660; PBDEs, < 0.13-340. South Korea and Singapore generally had regionally low concentrations. Elevated concentrations of PCBs, DDTs, and HCB occurred at sites in China, higher than reported in a similar recent sampling campaign in Europe. Chlordane was highest in samples from Japan (which also had elevated levels of PCBs and DDTs) and was also elevated in some Chinese locations. PBDE levels were generally low in the region.

Air Pollutants↗

PubMed2005

Hexachlorobenzene in the global environment: emissions, levels, distribution, trends and processes.

Hexachlorobenzene (HCB) is considered here as a 'model persistent organic pollutant.' Data on its sources, emissions, environmental levels and distributions and trends are compiled and used to assess its fate and behaviour in the global environment. Consideration is given as to the extent to which it has undergone repeated air-surface exchange or 'hopping' to become globally dispersed, the balance between primary and secondary sources in maintaining ambient levels, and its ultimate sinks in the environment. Global production exceeded 100,000 tonnes and primary emissions to atmosphere probably peaked in the 1970s. There has been a consistent downward trend in the environment over the past 20 years. Temporal trends of HCB in the environment vary, dependent on time period measured, media studied and study location, but the average half-life from all the studies is approximately 9 years. Estimates are made of the contemporary burden in the environment; these range between 10,000 and 26,000 tonnes and are dominated by the loadings in treated and background soils, sediments and oceans. Estimates of the trends of HCB emissions from treated soils are derived. At its peak, the amount of HCB emitted from soil to air may have been in the hundreds to thousands of tonnes per year, which would have made it a significant source of HCB to the environment. Whilst the amount of HCB being emitted from contemporary soil is much lower, only a small amount of re-emission of HCB from soil to air is required to maintain contemporary air concentrations under the current primary emission scenario.

Air Pollutants↗

PubMed2005

The role of soil organic carbon in the global cycling of persistent organic pollutants (POPs): interpreting and modelling field data.

Soil is an important global reservoir for persistent organic pollutants (POPs). The interaction between air (which often receives the majority of emissions) and soil plays a key role in the long term environmental cycling and fate of these chemicals. Soil surveys have been carried out to try and estimate regional and global distribution/inventory of POPs. A correlation between soil POPs concentration and soil organic carbon (SOC) has been observed in background soils [Meijer et al., 2003. Global distribution and budget of PCBs and HCB in background surface soils: implications for sources and environmental processes. Environ. Sci. Technol., 37, 667], provoking discussion about whether POPs will approach steady-state (or equilibrium) between air and SOC, on a global scale. This manuscript investigates this relationship and in particular how soil concentrations can be influenced by factors such as temperature, SOC content and physicochemical properties. A simple two box model designed to investigate parameters that are likely to affect air-soil exchange revealed that more volatile chemicals such as HCB are likely to achieve steady-state conditions between air and soil relatively quickly whilst relatively involatile chemicals, such as heavy PCBs, may take considerably longer and other compounds (e.g. OCDD) may never achieve it. These model calculations provide an insight into which fate processes (e.g. volatilisation or degradation) may control a chemicals fate in the terrestrial environment. A different modelling exercise was used to explore the complex interaction of environmental parameters, representative of 'real world' conditions to study their potential influence on POPs cycling at the European scale. Results from the model suggested that compound degradation rates in soil (linked to SOC content), temperature, vegetation cover and ecosystem C turnover are all likely to significantly influence POP air-soil exchange and fate.

Air↗

PubMed2005

Temporal trends in the sources of PCDD/Fs to and around the Venice Lagoon.

Two salt marsh cores were collected from the Venice Lagoon, Italy, and analysed for PCDD/Fs. The samples were undisturbed and had an approximately constant accumulation rate. Radiochemical chronologies were established for the different core sections. The PCDD/F pattern in the surficial layers was very similar to that of atmospheric deposition measured in the same area. However, the pattern changed with increasing depth and was very different in the deeper sections, where the highest PCDD/F concentrations were measured. This layer was dated around the 1950s. Deeper layers have a profile similar to the surficial one. Undisturbed salt marsh cores appear to be a reliable tool for the reconstruction of temporal trends in the atmospheric deposition of persistent organic pollutants. It is proposed that the trends in the core reflect atmospheric deposition that probably results from the sum of two different contributions: emissions of the industrial district of Porto Marghera on the edge of the lagoon and the regional background.

Air Pollutants↗

PubMed2005

Reconstruction of historical trends of PCDD/Fs and PCBs in the Venice Lagoon, Italy.

Historical trends of PCDD/Fs and PCBs from the year 1900 have been reconstructed for the Venice Lagoon area by using a fugacity-based dynamic multimedia model. A novel approach to estimate the inputs to the system was applied. Emissions to the lagoon were estimated by studying dated sediment cores taken from salt marshes located in the lagoon area. These cores have recently proven to be a suitable tool to reconstruct the temporal trends of atmospheric deposition of POPs. According to the model, concentrations of PCBs and PCDD/Fs in air and water reflect the trends of their production and usage, peaking during the 1960s. The peaks in the sediment were delayed by 5-40 years depending on the congener. Predicted concentrations are in good agreement with experimental results. The most important input parameters, identified by a sensitivity analysis, are the degradation constants, K(ow), the Henry's law constant, vapour pressure, active sediment depth, sediment resuspension, and deposition rates, and water residence time in the lagoon.

Cities↗

PubMed2004

Passive air sampling of PCBs, PBDEs, and organochlorine pesticides across Europe.

This study presents concurrently sampled ambient air data for a range of persistent organic pollutants at the continental scale. This was achieved using a passive air sampling system, deploying polyurethane foam disks, which was prepared in one laboratory, sealed to prevent contamination, sent out by courier to volunteers participating in different countries, exposed for 6 weeks, collected, resealed, and returned to the laboratory for analysis. Europe was the study area--a region with a history of extensive POPs usage and emission and with marked national differences in population density, the degree of urbanization and industrial/agricultural development. Samplers were deployed at remote/rural/urban locations in 22 countries and analyzed for PCBs, a range of organochlorine pesticides (HCB, alpha-HCH, gamma-HCH, ppDDT, ppDDE), and PBDEs. Calculated air concentrations were in line with those obtained by conventional active air sampling techniques. The geographical pattern of all compounds reflected suspected regional emission patterns and highlighted localized hotspots. PCB and PBDE levels varied by over 2 orders of magnitude; the highest values were detected in areas of high usage and were linked to urbanized areas. HCB was relatively uniformly distributed, reflecting its persistence and high degree of mixing in air. Higher gamma-HCH, ppDDT, and ppDDE levels generally occurred in South and East Europe.

Agriculture↗

PubMed2004

Modelling the atmospheric fate and seasonality of polycyclic aromatic hydrocarbons in the UK.

This paper presents the results from an exercise in atmospheric contaminant fate modelling, which had three main objectives: (1) to investigate the balance between estimated national atmospheric emissions of six selected PAHs and observed ambient measurements for the UK, as a means of testing the current emission estimates; (2) to investigate the potential influence of seasonally dependent environmental fate processes on the observed seasonality of air concentrations; and (3) after undertaking the first two objectives, to make inferences about the likely magnitude of seasonal differences in sources. When addressing objective 1 with annually averaged emissions data, it appeared that the UK PAH atmospheric emissions inventory was reasonably reliable for fluorene, fluoranthene, pyrene, benzo[a]pyrene and benzo[ghi]perylene--but not so for phenanthrene. However, more detailed analysis of the seasonality in environmental processes which may influence ambient levels, showed that the directions and/or magnitudes of the predicted seasonality did not coincide with field observations. This indicates either that our understanding of the environmental fate and behaviour of PAHs is still limited, and/or that there are uncertainties in the emissions inventories. It is suggested that better quantification of PAH sources is needed. For 3- and 4-ringed compounds, this should focus on those sources which increase with temperature, such as volatilisation from soil, water, vegetation and urban surfaces, and possible microbially-mediated formation mechanisms. The study also suggests that the contributions of inefficient, diffusive combustion processes (e.g. domestic coal/wood burning) may be underestimated as a source of the toxicologically significant higher molecular weight species in the winter. It is concluded that many signatory countries to the UNECE POPs protocol (which requires them to reduce national PAH emissions to 1990 levels) will experience difficulties in demonstrating compliance, because source inventories for 1990 and contemporary situations are clearly subject to major uncertainties.

Air Pollutants↗

PubMed2004

Seasonal and long-term trends in atmospheric PAH concentrations: evidence and implications.

Atmospheric monitoring data for selected polynuclear aromatic hydrocarbons (PAHs) were compiled from remote, rural and urban locations in the UK, Sweden, Finland and Arctic Canada. The objective was to examine the seasonal and temporal trends, to shed light on the factors which exert a dominant influence over ambient PAH levels. Urban centres in the UK have concentrations 1-2 orders of magnitude higher than in rural Europe and up to 3 orders of magnitude higher than Arctic Canada. Interpretation of the data suggests that proximity to primary sources 'drives' PAH air concentrations. Seasonality, with winter (W) > summer (S), was apparent for most compounds at most sites; high molecular weight compounds (e.g. benzo[a]pyrene) showed this most clearly and consistently. Some low molecular weight compounds (e.g. phenanthrene) sometimes displayed S>W seasonality at some rural locations. Strong W>S seasonality is linked to seasonally-dependent sources which are greater in winter. This implicates inefficient combustion processes, notably the diffusive domestic burning of wood and coal. However, sometimes seasonality can also be strongly influenced by broad changes in meteorology and air mass origin (e.g. in the Canadian Arctic). The datasets examined here suggest a downward trend for many PAHs at some sites, but this is not apparent for all sites and compounds. The inherent noise in ambient air monitoring data makes it difficult to derive unambiguous evidence of underlying declines, to confirm the effectiveness of international source reduction measures.

Agriculture↗

PubMed2004

Modelling the fate of persistent organic pollutants in Europe: parameterisation of a gridded distribution model.

A regionally segmented multimedia fate model for the European continent is described together with an illustrative steady-state case study examining the fate of gamma-HCH (lindane) based on 1998 emission data. The study builds on the regionally segmented BETR North America model structure and describes the regional segmentation and parameterisation for Europe. The European continent is described by a 5 degrees x5 degrees grid, leading to 50 regions together with four perimetric boxes representing regions buffering the European environment. Each zone comprises seven compartments including; upper and lower atmosphere, soil, vegetation, fresh water and sediment and coastal water. Inter-regions flows of air and water are described, exploiting information originating from GIS databases and other georeferenced data. The model is primarily designed to describe the fate of Persistent Organic Pollutants (POPs) within the European environment by examining chemical partitioning and degradation in each region, and inter-region transport either under steady-state conditions or fully dynamically. A test case scenario is presented which examines the fate of estimated spatially resolved atmospheric emissions of lindane throughout Europe within the lower atmosphere and surface soil compartments. In accordance with the predominant wind direction in Europe, the model predicts high concentrations close to the major sources as well as towards Central and Northeast regions. Elevated soil concentrations in Scandinavian soils provide further evidence of the potential of increased scavenging by forests and subsequent accumulation by organic-rich terrestrial surfaces. Initial model predictions have revealed a factor of 5-10 underestimation of lindane concentrations in the atmosphere. This is explained by an underestimation of source strength and/or an underestimation of European background levels. The model presented can further be used to predict deposition fluxes and chemical inventories, and it can also be adapted to provide characteristic travel distances and overall environmental persistence, which can be compared with other long-range transport prediction methods.

Climate↗

PubMed2004

Passive air sampling of polycyclic aromatic hydrocarbons and polychlorinated naphthalenes across Europe.

This study presents concurrently sampled ambient air data for a range of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated naphthalenes (PCNs) at the continental scale. This was achieved with a passive air sampling system, by deploying polyurethane foam disks, which were prepared in one laboratory, sealed to prevent contamination, sent out by courier to volunteers participating in different countries, exposed for six weeks, collected, resealed, and returned to the laboratory for analysis. The study area was Europe, a region with a history of extensive persistent organic pollutants usage and emission, and with marked national differences in population density, the degree of urbanization and industrial and agricultural development. Samplers were deployed at remote, rural, and urban locations in 22 countries. Calculated air concentrations were broadly in line with those obtained by conventional active air sampling techniques, for both compound classes and for compounds existing predominantly in the gas and particle phases. The geographical compound distribution reflected suspected regional emission patterns and highlighted localized source areas. Both PAH and PCN levels varied by more than two orders of magnitude. The implications for sources are discussed.

Air Pollutants↗

PubMed2003

Estimation of PCDD/F distribution and fluxes in the Venice Lagoon, Italy: combining measurement and modelling approaches.

The available experimental information on the occurrence of PCDD/Fs in the Venice Lagoon, Italy, was compiled and used to calculate fugacities for the environmental compartments of sediment, suspended particulate matter (SPM), water and air and then used to estimate fugacity ratios and assess the likely net direction of flux between media. The bottom sediment: SPM fugacity ratios for different PCDD/Fs indicate conditions close to equilibrium, suggestive of the close coupling of SPM with re-suspended sediment. Sediment/water and the sediment/air fugacity ratios suggest that net flux directions vary depending on the congener and the location within the lagoon. Net sediment-water-air movement (i.e. re-mobilisation/volatilisation) is suggested for the lighter congeners from the industrial canals, where the highest PCDD/F concentrations in the lagoon occur. The tendency to volatilise increases with decreasing congener molecular weight. In contrast, net deposition (air-water-sediment) appears to be occurring for the heaviest (hepta- and octa-) substituted PCDD/Fs. OCDF represents a marker of the industrial district of the lagoon, decreasing in concentration and as a fraction of total PCDD/Fs with increasing distance. The fugacity-based quantitative water air sediment interaction (QWASI) mass-balance model was applied to the central part of the lagoon. The key parameters for the determination of the model output, identified by a sensitivity analysis, were: the sediment active depth, the sediment re-suspension and deposition rates, and the total input of PCDD/Fs to the system. The QWASI model also indicates the tendency for the lighter PCDD/Fs to be released from surface sediment to the water column.

Air↗

PubMed2003

Understanding levels and trends of BDE-47 in the UK and North America: an assessment of principal reservoirs and source inputs.

Despite increasing interest in the occurrence of Polybrominated diphenyl ethers (PBDEs) in the environment, there has been only limited effort expended to identify principal source input reservoirs and pathways into the environment. Taking a single congener BDE-47, an important component of the penta commercial product, we have estimated principal contemporary reservoirs and emissions in two regions with very different historical use patterns. In North America, production and use of the penta-product has been rising steadily for the last 20 years, whilst in the UK, use has been restricted over the last 10 years, and most recently, there has been an EU ban on use. Mass balance models have been applied using our contemporary emission estimates to predict environmental levels. Results highlight that contemporary emissions to air can account for contemporary air concentrations but cannot account for measured concentrations in principal reservoirs such as soils and sediments. Future efforts are needed to improve our knowledge of the stocks of PBDEs in use, and emission factors from those stocks, to better understand/predict past and likely future trends.

Environmental Exposure↗

PubMed2003

The global re-cycling of persistent organic pollutants is strongly retarded by soils.

'Persistent organic pollutants' (POPs) are semi-volatile, mobile in the environment and bioaccumulate. Their toxicity and propensity for long-range atmospheric transport (LRAT) has led to international bans/restrictions on their use/release. LRAT of POPs may occur by a 'single hop' or repeated temperature-driven air-surface exchange. It has been hypothesised that this will result in global fractionation and distillation-with condensation and accumulation in polar regions. Polychlorinated biphenyls (PCBs)--industrial chemicals banned/restricted in the 1970s--provide a classic illustration of POP behaviour. A latitudinally-segmented global PCB inventory has been produced, which shows that approximately 86% of the 1.3 x 10(6) tonnes produced was used in the temperate industrial zone of the northern hemisphere. A global survey of background surface soils gives evidence for 'fractionation' of PCBs. More significantly, however, very little of the total inventory has 'made the journey' via primary emission and/or air-surface exchange and LRAT out of the heavily populated source regions, in the 70 years since PCBs were first produced. Soils generally occlude PCBs, especially soils with dynamic turnover of C/bioturbation/burial mechanisms. This limits the fraction of PCBs available for repeated air-soil exchange. The forested soils of the northern hemisphere, and other C-rich soils, appear to be playing an important role in 'protecting' the Arctic from the advective supply of POPs. Whilst investigations on POPs in remote environments are important, it is imperative that researchers also seek to better understand their release from sources, persistence in source regions, and the significant loss mechanisms/global sinks of these compounds, if they wish to predict future trends.

Arctic Regions↗

PubMed2002

A dynamic level IV multimedia environmental model: application to the fate of polychlorinated biphenyls in the United Kingdom over a 60-year period.

A dynamic or level IV multimedia model is described and illustrated by application to the fate of three polychlorinated biphenyl (PCB) congeners in the United Kingdom over a 60-year period from their introduction into commerce until the present. Models of this type are shown to be valuable for elucidating the time response of environmental systems to increasing, decreasing, or pulse inputs. The suggestion is made that in addition to the outputs of time-dependent concentrations (which can be compared with monitoring data for validation purposes), it is useful to examine masses, fugacities, and fugacity ratios between media? The relative importance of processes is best evaluated by compiling cumulative intermedia fluxes and quantities lost by reaction and advection and examining the corresponding process rate constants or their reciprocals, the characteristic times. The suggestion is made that uncertainty and sensitivity analyses are desirable, but it must be appreciated that relative sensitivities of input parameters may change during the simulation period, so a single sensitivity analysis conducted at one point in time can be misleading. The use of the model for forecasting future trends in concentration is illustrated. Given the uncertainties in emission and advective inflow rates, the simulation of PCB fate in the United Kingdom is regarded as showing time trends that are in satisfactory agreement with monitoring data.

Environmental Monitoring↗