Knut Breivik

Towards a global historical emission inventory for selected PCB congeners - a mass balance approach: 3. An update

Previously published estimates of the global production, consumption and atmospheric emissions of 22 individual PCB congeners [Breivik K, Sweetman A, Pacyna JM, Jones KC. Towards a global historical emission inventory for selected PCB congeners - a mass balance approach. 1. Global production and consumption. Sci Total Environ 2002a; 290: 181-198.; Breivik K, Sweetman A, Pacyna JM, Jones KC. Towards a global historical emission inventory for selected PCB congeners--a mass balance approach. 2. Emissions. Sci Total Environ 2002b; 290: 181-198.] have provided useful information for later studies attempting to interpret contaminant levels in remote areas as well as in the global environment. As a result of the need for more contemporary emission data (following the year 2000), an update of this emission database is presented. This exercise takes into account new information on PCB production in Poland, as well as new data on the chemical composition of various technical mixtures for which less information had been available. The methodology to estimate temporal trends of PCB emissions associated with various types of PCB usage is improved. Projected emissions up to year 2100 are presented to facilitate predictions of future environmental exposure. The national emission data for each of the 114 countries considered is spatially resolved on a 1 degrees x1 degrees grid for each congener and year, using population density as a surrogate.

Towards a global historical emission inventory for selected PCB congeners--a mass balance approach. 1. Global production and consumption.

Information on the historical global production and consumption of polychlorinated biphenyls (PCBs) is urgently needed for estimating PCB fluxes to the environment and for interpreting global contamination patterns by these pollutants. This study presents the methodology, principal uncertainties and selected results from an inventory, aiming to quantify the global production and consumption of total PCBs as well as 22 PCB congeners. The available data on the historical production of PCBs and the chemical composition of various technical mixtures have been compiled from the literature. For some producers with less detailed information, the production of individual PCB constituents has been estimated to derive a global estimate for individual homologues and selected congeners. Information on imports, exports and consumption, as well as restrictions on production and imports, has further been compiled for individual countries. These data, along with assumptions on the trade between countries and regions, have been utilised to derive an estimate of the global historical consumption pattern. Although there are substantial uncertainties involved in these estimates, important aspects governing the large scale temporal and spatial patterns are most likely captured in these estimates. In particular, the information on imports and exports for the principal users of PCBs around the time of peak production is considered to be fairly reliable. The estimates account for a reported historical global production of approximately 1.3 million t PCBs, more than 70% of which are tri-, tetra- and pentachlorinated biphenyls. The results further suggest that almost 97% of the global historical use of PCBs have occurred in the Northern Hemisphere.

Atmospheric monitoring of organic pollutants in the Arctic under the Arctic Monitoring and Assessment Programme (AMAP): 1993-2006.

Continuous and comparable atmospheric monitoring programs to study the transport and occurrence of persistent organic pollutants (POPs) in the atmosphere of remote regions is essential to better understand the global movement of these chemicals and to evaluate the effectiveness of international control measures. Key results from four main Arctic research stations, Alert (Canada), Pallas (Finland), Storhofdi (Iceland) and Zeppelin (Svalbard/Norway), where long-term monitoring have been carried out since the early 1990s, are summarized. We have also included a discussion of main results from various Arctic satellite stations in Canada, Russia, US (Alaska) and Greenland which have been operational for shorter time periods. Using the Digital Filtration temporal trend development technique, it was found that while some POPs showed more or less consistent declines during the 1990s, this reduction is less apparent in recent years at some sites. In contrast, polybrominated diphenyl ethers (PBDEs) were still found to be increasing by 2005 at Alert with doubling times of 3.5 years in the case of deca-BDE. Levels and patterns of most POPs in Arctic air are also showing spatial variability, which is typically explained by differences in proximity to suspected key source regions and long-range atmospheric transport potentials. Furthermore, increase in worldwide usage of certain pesticides, e.g. chlorothalonil and quintozene, which are contaminated with hexachlorobenzene (HCB), may result in an increase in Arctic air concentration of HCB. The results combined also indicate that both temporal and spatial patterns of POPs in Arctic air may be affected by various processes driven by climate change, such as reduced ice cover, increasing seawater temperatures and an increase in biomass burning in boreal regions as exemplified by the data from the Zeppelin and Alert stations. Further research and continued air monitoring are needed to better understand these processes and its future impact on the Arctic environment.

Relationships between organic matter, black carbon and persistent organic pollutants in European background soils: Implications for sources and environmental fate.

Black carbon (BC) and total organic carbon (TOC) contents of UK and Norwegian background soils were determined and their relationships with persistent organic pollutants (HCB, PAHs, PCBs, co-planar PCBs, PBDEs and PCDD/Fs) investigated by correlation and regression analyses, to assess their roles in influencing compound partitioning/retention in soils. The 52 soils used were high in TOC (range 54-460 mg/g (mean 256)), while BC only constituted 0.24-1.8% (0.88%) of the TOC. TOC was strongly correlated (p<0.001) with HCB, PCBs, co-PCBs and PBDEs, but less so with PCDD/Fs (p<0.05) and PAHs. TOC explained variability in soil content, as follows: HCB, 80%; PCBs, 44%; co-PCBs, 40%; PBDEs, 27%. BC also gave statistically significant correlations with PBDEs (p<0.001), co-PCBs (p<0.01) and PCBs, HCB, PCDD/F (p<0.05); TOC and BC were correlated with each other (p<0.01). Inferences are made about possible combustion-derived sources, atmospheric transport and air-surface exchange processes for these compounds.

Tracking the global generation and exports of e-waste:do existing estimates add up?

The transport of discarded electronic and electrical appliances (e-waste) to developing regions has received considerable attention, but it is difficult to assess the significance of this issue without a quantitative understanding of the amounts involved. The main objective of this study is to track the global transport of e-wastes by compiling and constraining existing estimates of the amount of e-waste generated domestically in each country MGEN, exported from countries belonging to the Organization for Economic Cooperation and Development (OECD) MEXP, and imported in countries outside of the OECD MIMP. Reference year is 2005 and all estimates are given with an uncertainty range. Estimates of MGEN obtained by apportioning a global total of ∼ 35,000 kt (range 20,000-50,000 kt) based on a nations gross domestic product agree well with independent estimates of MGEN for individual countries. Import estimates MIMP to the countries believed to be the major recipients of e-waste exports from the OECD globally (China, India, and five West African countries) suggests that ∼ 5,000 kt (3,600 kt-7,300 kt) may have been imported annually to these non-OECD countries alone, which represents ∼ 23% (17%-34%) of the amounts of e-waste generated domestically within the OECD. MEXP for each OECD country is then estimated by applying this fraction of 23% to its MGEN. By allocating each countrys MGEN, MIMP, MEXP and MNET = MGEN + MIMP - MEXP, we can map the global generation and flows of e-waste from OECD to non-OECD countries. While significant uncertainties remain, we note that estimated import into seven non-OECD countries alone are often at the higher end of estimates of exports from OECD countries.

Are Reductions in Industrial Organic Contaminants Emissions in Rich Countries Achieved Partly by Export of Toxic Wastes

Recent studies show that PCB (polychlorinated biphenyl) air concentrations remain surprisingly high in parts of Africa and Asia. These are regions where PCBs were never extensively used, but which are implicated as recipients of obsolete products and wastes containing PCBs and other industrial organic contaminants, such as halogenated flame retardants (HFRs). We hypothesize that there may be different trends in emissions across the globe, whereby emissions of some industrial organic contaminants may be decreasing faster in former use regions (due to emission reductions combined with uncontrolled export), at the expense of regions receiving these substances as obsolete products and wastes. We conclude that the potential for detrimental effects on the environment and human health due to long-range transport by air, water, or wastes should be of equal concern when managing and regulating industrial organic contaminants. This calls for a better integration of life-cycle approaches in the management and regulation of industrial organic contaminants in order to protect environmental and human health on a global scale. Yet, little remains known about the amounts of industrial organic contaminants exported outside former use regions as different types of wastes because of the often illicit nature of these operations.

CoZMo-POP 2 - A fugacity-based dynamic multi-compartmental mass balance model of the fate of persistent organic pollutants

CoZMo-POP 2, a dynamic multimedia fate and transport model (MFTM) for describing the long-term fate of persistent organic pollutants (POPs) in a coastal environment or the drainage basin of a large lake is described. The modelled environment, consisting of up to 19 compartments, includes the forest, soils and fresh water bodies of the drainage basin, and a variable number of sequentially arranged marine water units, representing estuarine, coastal, open and deep water environments. Two sediment compartments in each water basin allow to account for the possibility of the simultaneous occurrence of eroding and accumulating bottoms in a water basin. As the movement of POPs in the environment is closely associated with the movement of air, water and organic matter, the model constructs complete steady state mass budgets for air, water and particulate organic carbon (POC) between the model compartments from the environmental parameters supplied by the user. This assures that these input parameters, which can be stored in a database, are all mutually compatible and internally consistent. The CoZMo-POP 2 model takes into account seasonably variable wind speeds, temperatures, canopy developments and OH radical concentrations, and allows for the definition of time-variant emission scenarios. CoZMo-POP 2 is a flexible, dynamic MFTM that can be used for detailed investigation of a particular fate process using a generic environmental scenario, as well as for simulations of the behaviour of a particular POP in a particular environment. All of the model equations, which are expressed in fugacity notation, are provided.

Evidence for Major Emissions of PCBs in the West African Region

In previous studies unexpectedly high air concentrations of polychlorinated biphenyls (PCBs) were observed in ship-based measurements made ∼400 km off parts of the West African coast. To investigate further (i) samples were taken on board the RV Polarstern during a cruise from Germany to South Africa in October-November 2007; (ii) samples were obtained on Cape Verde Island during the same period to monitor airflows from Africa; and (iii) passive samplers were deployed in four West African countries to try to characterize potential sources on land. Results were as follows: on Cape Verde and on the ship air masses came predominantly (∼ 95%) from the African continent; the shipboard Σ29PCB concentrations off West Africa ranged from 10 to 360 pg m(-3) and from 6 to 99 pg m(-3) in Cape Verde; the highest land-based concentrations were observed in Ivory Coast and the Gambia (up to 300 pg m(-3)) and the lowest was observed in Ghana (9 pg m(-3)). Taken together, these and previous studies indicate there are more major emission(s) of PCBs and different source types in parts of West Africa than accounted for in current global atmospheric emissions estimates. Results from the FLEXPART model and PAH measurements show that emission inventories and biomass burning cannot fully explain the high PCB concentrations. Potential sources of the high PCB levels to the African regions are discussed, namely illegal dumping of PCB containing waste with release via volatilization and uncontrolled burning, and the storage and breakup of old ships.

Has the Burden and Distribution of PCBs and PBDEs Changed in European Background Soils between 1998 and 2008? Implications for Sources and Processes

Background soils were collected from 70 locations on a latitudinal transect in the United Kingdom and Norway in 2008, ten years after they had first been sampled in 1998. The soils were analyzed for polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), and organochlorine pesticides (OCs), to see whether there had been any change in the loadings or distributions of these persistent organic pollutants (POPs). The same transect has also been used to sample air between the mid-1990s and the present, so the air and soil spatial and temporal trends provide information on air-soil transfers, source-receptor relationships, long-range atmospheric transport (LRAT), and recycling phenomena. Comparisons of the 2008 and 1998 data sets show a general decline for PBDEs in surface soil, and a smaller averaged net decline of PCBs. Changes between the years were observed for total POP concentrations in soil and also for correlations with site and sample characteristics assumed to affect those concentrations. POP concentrations were correlated to distance and strength of possible sources, a relationship that became weaker in the 2008 data. Fractionation, a commonly discussed process for the global cycling of POPs was also lost in the 2008 data. As in 1998, soil organic matter content continues to have a strong influence on the loadings of POPs in surface soils, but changes in the PCB loads were noted. These factors indicate an approach to air-surface soil equilibrium and a lessening of the influence of primary sources on POP concentrations in soil between 1998 and 2008.

Trends in European Background Air Reflect Reductions in Primary Emissions of PCBs and PBDEs

Data are presented for polychlorinated biphenyls (PCBs) and polybrominated diphenyls ethers (PBDEs) in passive air samplers (PAS) collected along a rural/remote latitudinal transect from southern UK to northern Norway during 2004-2008. This study is part of an ongoing campaign, using semipermeable membrane devices (SPMDs) as PAS over two year intervals since 1994. Absolute sequestered amounts of selected PCB congeners have decreased in a first order fashion between 1994-2008, with the average time of 8.4+/-3.2 years for atmospheric concentrations to decline by 50%. PCBs have continued to fractionate with latitude during this period. PBDE concentrations declined by 50% between 2000 and 2008 every 2.2+/-0.4 years. Results are discussed in terms of sources, long-range atmospheric transport, global fractionation, and clearance processes. It is concluded that the spatial and temporal trends in background European air mainly reflect the strength of primary diffusive emissions of these compounds and subsequently their ongoing declines. The direct evidence for this is similar rates of decline at all the sites; similar rates of decline for all congeners; no systematic change in the fractionation pattern since 1994. The latest results indicate a reduction in the rate of decline for PCBs (and hence in primary emissions).