ABSTRACT
High-throughput screening is a strategy to identify potential adverse outcome pathways (AOP) for thousands of per- and polyfluoroalkyl substances (PFAS) if the specific effects can be distinguished from nonspecific effects. We hypothesize that baseline toxicity may serve as a reference to determine the specificity of the cell responses. Baseline toxicity is the minimum (cyto)toxicity caused by the accumulation of chemicals in cell membranes, which disturbs their structure and function. A mass balance model linking the critical membrane concentration for baseline toxicity to nominal (i.e., dosed) concentrations of PFAS in cell-based bioassays yielded separate baseline toxicity prediction models for anionic and neutral PFAS, which were based on liposome-water distribution ratios as the sole model descriptors. The specificity of cell responses to 30 PFAS on six target effects (activation of peroxisome proliferator-activated receptor (PPAR) gamma, aryl hydrocarbon receptor, oxidative stress response, and neurotoxicity in own experiments, and literature data for activation of several PPARs and the estrogen receptor) were assessed by comparing effective concentrations to predicted baseline toxic concentrations. HFPO-DA, HFPO-DA-AS, and PFMOAA showed high specificity on PPARs, which provides information on key events in AOPs relevant to PFAS. However, PFAS were of low specificity in the other experimentally evaluated assays and others from the literature. Even if PFAS are not highly specific for certain defined targets but disturb many toxicity pathways with low potency, such effects are toxicologically relevant, especially for hydrophobic PFAS and because PFAS are highly persistent and cause chronic effects. This implicates a heightened need for the risk assessment of PFAS mixtures because nonspecific effects behave concentration-additive in mixtures.
Subject(s)
Alkanesulfonic Acids , Fluorocarbons , Peroxisome Proliferator-Activated Receptors , Fluorocarbons/toxicity , Propionates , Biological AssayABSTRACT
Per- and polyfluoroalkyl substances (PFAS) are a class of substances for which there are widespread concerns about their extreme persistence in combination with toxic effects. It has been argued that PFAS should only be employed in those uses that are necessary for health or safety or are critical for the functioning of society and where no alternatives are available ("essential-use concept"). Implementing the essential-use concept requires a sufficient understanding of the current uses of PFAS and of the availability, suitability, and hazardous properties of alternatives. To illustrate the information requirements under the essential-use concept, we investigate seven different PFAS uses, three in consumer products and four industrial applications. We investigate how much information is available on the types and functions of PFAS in these uses, how much information is available on alternatives, their performance and hazardous properties and, finally, whether this information is sufficient as a basis for deciding on the essentiality of a PFAS use. The results show (i) the uses of PFAS are highly diverse and information on alternatives is often limited or lacking; (ii) PFAS in consumer products often are relatively easy to replace; (iii) PFAS uses in industrial processes can be highly complex and a thorough evaluation of the technical function of each PFAS and of the suitability of alternatives is needed; (iv) more coordination among PFAS manufacturers, manufacturers of alternatives to PFAS, users of these materials, government authorities, and other stakeholders is needed to make the process of phasing out PFAS more transparent and coherent.
Subject(s)
FluorocarbonsABSTRACT
Despite decades of research on per- and polyfluoroalkyl substances (PFAS), fundamental obstacles remain to addressing worldwide contamination by these chemicals and their associated impacts on environmental quality and health. Here, we propose six urgent questions relevant to science, technology, and policy that must be tackled to address the "PFAS problem": (1) What are the global production volumes of PFAS, and where are PFAS used? (2) Where are the unknown PFAS hotspots in the environment? (3) How can we make measuring PFAS globally accessible? (4) How can we safely manage PFAS-containing waste? (5) How do we understand and describe the health effects of PFAS exposure? (6) Who pays the costs of PFAS contamination? The importance of each question and barriers to progress are briefly described, and several potential paths forward are proposed. Given the diversity of PFAS and their uses, the extreme persistence of most PFAS, the striking ongoing lack of fundamental information, and the inequity of the health and environmental impacts from PFAS contamination, there is a need for scientific and regulatory communities to work together, with cooperation from PFAS-related industries, to fill in critical data gaps and protect human health and the environment.
Subject(s)
Fluorocarbons , HumansABSTRACT
Fluoropolymers are a group of polymers within the class of per- and polyfluoroalkyl substances (PFAS). The objective of this analysis is to evaluate the evidence regarding the environmental and human health impacts of fluoropolymers throughout their life cycle(s). Production of some fluoropolymers is intimately linked to the use and emissions of legacy and novel PFAS as polymer processing aids. There are serious concerns regarding the toxicity and adverse effects of fluorinated processing aids on humans and the environment. A variety of other PFAS, including monomers and oligomers, are emitted during the production, processing, use, and end-of-life treatment of fluoropolymers. There are further concerns regarding the safe disposal of fluoropolymers and their associated products and articles at the end of their life cycle. While recycling and reuse of fluoropolymers is performed on some industrial waste, there are only limited options for their recycling from consumer articles. The evidence reviewed in this analysis does not find a scientific rationale for concluding that fluoropolymers are of low concern for environmental and human health. Given fluoropolymers' extreme persistence; emissions associated with their production, use, and disposal; and a high likelihood for human exposure to PFAS, their production and uses should be curtailed except in cases of essential uses.
Subject(s)
Fluorocarbons , Environmental Health , Fluorocarbons/analysis , Humans , PolyethyleneABSTRACT
Chlorinated paraffins are industrial chemicals that can be subdivided into short-chain (SCCP), medium-chain (MCCP), and long-chain (LCCP) chlorinated paraffins. The global production volumes of MCCPs are nowadays suspected to be much higher than those of S- and LCCPs, and the few available studies on the environmental occurrence of chlorinated paraffins report often higher MCCP concentrations than S- or LCCP concentrations in the environment. The present review focuses, therefore, on MCCPs specifically and provides a literature overview and a data analysis of the production volumes, PBT properties (persistence, bioaccumulation potential, and toxicity), and the worldwide measured concentrations of MCCP in environmental samples, biota, and humans. Furthermore, we include our own measurements of technical CP formulations from China, the major global producing country, to estimate the global production amounts of MCCPs. The key findings from this review are that (1) MCCPs are toxic to the aquatic environment, and the available data suggest that they are also persistent; (2) available time trends for MCCPs in soil, biota, and most of the sediment cores show increasing time trends over the last years to decades; and (3) MCCP concentrations in sediment close to local sources exceed toxicity thresholds (i.e., the PNEC). Our study shows that overall, MCCPs are of growing concern, and regulatory actions should be considered seriously.
Subject(s)
Hydrocarbons, Chlorinated , Paraffin , China , Environmental Monitoring , Humans , SoilABSTRACT
Ambient air concentrations of polychlorinated biphenyls (PCBs) in Zurich, Switzerland, are reported for the years 2011-2013. These measurements reveal a distinct seasonal trend with PCB concentrations in air during the summer that were three to five times higher than in the winter. We used a long-term dynamic multimedia model to analyze the seasonal trend and to back-calculate urban emissions of PCBs. In contrast to previous short-term studies that considered time periods of several days to months to extrapolate annual emissions, the use of long-term field data and the corresponding model reduces the uncertainty in these extrapolations. Comparison with measured PCB concentrations in air shows that our model is able to reproduce seasonal trends of the six indicator PCBs (iPCBs). The good agreement of the model results with measurements over a time period of three years provides confidence in model outputs and allows us to estimate the total annual PCB emissions of Zurich (86 µg capita(-1) d(-1)). The resulting summer emissions are nine times higher than emissions during winter. Interestingly, this factor corresponds to the expected increase in PCB volatilization due to the effect of temperature on vapor pressure. This finding implies that PCBs in Zurich are probably released mainly by volatilization from sources that are directly exposed to ambient air temperature (i.e., outdoor sources). The derived emissions are in accordance with previous studies performed at the same location and are also in agreement with an existing emission inventory.
Subject(s)
Air Pollutants/analysis , Environmental Monitoring/methods , Models, Theoretical , Polychlorinated Biphenyls/analysis , Cities , Environmental Monitoring/statistics & numerical data , Seasons , Switzerland , VolatilizationABSTRACT
Short-chain chlorinated paraffins (SCCPs) are of concern due to their potential for adverse health effects, bioaccumulation, persistence, and long-range transport. Data on concentrations of SCCPs in urban areas and underlying emissions are still scarce. In this study, we investigated the levels and spatial distribution of SCCPs in air, based on two separate, spatially resolved sampling campaigns in the city of Zurich, Switzerland. SCCP concentrations in air ranged from 1.8 to 17 ng·m(-3) (spring 2011) and 1.1 to 42 ng·m(-3) (spring 2013) with medians of 4.3 and 2.7 ng·m(-3), respectively. Both data sets show that atmospheric SCCP levels in Zurich can vary substantially and may be influenced by a number of localized sources within this urban area. Additionally, continuous measurements of atmospheric concentrations performed at one representative sampling site in the city center from 2011 to 2013 showed strong seasonal variations with high SCCP concentrations in summer and lower levels in winter. A long-term dynamic multimedia environmental fate model was parametrized to simulate the seasonal trends of SCCP concentrations in air and to back-calculate urban emissions. Resulting annual SCCP emissions in the city of Zurich accounted for 218-321 kg, which indicates that large SCCP stocks are present in urban areas of industrialized countries.
Subject(s)
Air Pollutants/analysis , Atmosphere/chemistry , Cities , Environmental Monitoring/methods , Halogenation , Paraffin/analysis , Models, Theoretical , Seasons , SwitzerlandABSTRACT
Fluoropolymers are a group of fluorinated polymers within the broad class of substances known as per- and polyfluoroalkyl substances (PFASs). During their production, a wide array of additional fluorinated organic substances (many PFASs and some not defined as PFASs) are used, formed and emitted to air and water. This study aims to assess, and make an inventory of, all emissions of PFASs and other fluorinated organic substances by the fluoropolymer production industry in Europe using available emission databases and permits. Air emissions of the fluorinated gases (i.e., chlorofluorocarbons, hydrofluorocarbons, hydrochlorofluorocarbons and perfluorocarbons (CFCs, H(C)FCs and PFCs)) by this industry have reportedly decreased between 2007 and 2021 from roughly 500 to 150 tonnes per year. Emissions of fluorosurfactants to air and water have also been reduced significantly. However, large uncertainties remain regarding the emissions of substances that are neither fluorinated gases nor fluorosurfactants but are classified as PFASs, such as polymerization by-products, chain transfer agents and fluorinated solvents. The available data indicate that the release of these substances is not decreasing but remains relatively stable. As this inventory probably underestimates emissions, further research, improved data availability and more harmonized reporting of emissions are necessary to obtain more accurate emission data for these substances. Nevertheless, based on the available data, it is clear that the emissions from fluoropolymer production plants to air and water are still significant and that the production of fluoropolymers continues to introduce persistent substances to the environment.
Subject(s)
Fluorocarbon Polymers , Fluorocarbons , Fluorocarbons/analysis , Europe , Water , GasesABSTRACT
Per- and polyfluoroalkyl substances (PFASs) are a class of synthetic organic chemicals of global concern. A group of 36 scientists and regulators from 18 countries held a hybrid workshop in 2022 in Zürich, Switzerland. The workshop, a sequel to a previous Zürich workshop held in 2017, deliberated on progress in the last five years and discussed further needs for cooperative scientific research and regulatory action on PFASs. This review reflects discussion and insights gained during and after this workshop and summarizes key signs of progress in science and policy, ongoing critical issues to be addressed, and possible ways forward. Some key take home messages include: 1) understanding of human health effects continues to develop dramatically, 2) regulatory guidelines continue to drop, 3) better understanding of emissions and contamination levels is needed in more parts of the world, 4) analytical methods, while improving, still only cover around 50 PFASs, and 5) discussions of how to group PFASs for regulation (including subgroupings) have gathered momentum with several jurisdictions proposing restricting a large proportion of PFAS uses. It was concluded that more multi-group exchanges are needed in the future and that there should be a greater diversity of participants at future workshops.
ABSTRACT
The EU is planning to restrict the manufacture, placing on the market and use of per- and polyfluoroalkyl substances (PFASs) as a class. For such a broad regulatory approach, a lot of different data are required, including data on the hazardous properties of PFASs. Here, we analyze substances that fulfill the OECD definition of PFASs and that are registered under the regulation on Registration, Evaluation, Authorization, and Restriction of Chemicals (REACH) in the EU to obtain a better data basis for PFASs and to elucidate the range of PFASs on the market in the EU. As of September 2021, at least 531 PFASs had been registered under REACH. Our hazard assessment of the PFASs registered under REACH shows that the currently available data are not sufficient to identify those PFASs that are persistent, bioaccumulative and toxic (PBT) or very persistent and very bioaccumulative (vPvB). Using some basic assumptions - which are 1) PFASs or their metabolites do not mineralize, 2) neutral hydrophobic substances bioaccumulate unless they are metabolized and 3) all chemicals exhibit baseline toxicity, and effect concentrations cannot be above effect concentrations for baseline toxicity - shows that at least 17 of the 177 PFASs with full registration are PBT substances, 14 more than currently identified. Moreover, if mobility is considered as a hazard criterion, at least 19 additional substances will need to be considered hazardous. The regulation of persistent, mobile and toxic (PMT) and very persistent and very mobile (vPvM) substances would therefore also affect PFASs. However, many of the substances that have not been identified as PBT, vPvB, PMT or vPvM are either persistent and toxic, persistent and bioaccumulative or persistent and mobile. The planned PFASs restriction will therefore be important for a more effective regulation of these substances.
Subject(s)
Environmental Pollutants , Fluorocarbons , Environmental Pollutants/analysis , Risk Assessment , Bioaccumulation , Fluorocarbons/toxicity , Fluorocarbons/chemistryABSTRACT
Bioaccumulation is one of the three criteria for the PBT assessment of chemicals, where P stands for persistence, B for bioaccumulation, and T for toxicity, which is a cornerstone for the "Registration, Evaluation, Authorization, and Restriction of Chemicals" (REACH) in the EU. Registrants are required by REACH to submit data on bioaccumulation if the chemical is manufactured in and/or imported to the European Economic Area at more than 100 t/year. Most of the experimental bioaccumulation studies submitted were on the bioconcentration factor (BCF) and were conducted prior to 2012, before the OECD Test Guideline 305 on Bioaccumulation in Fish was updated. An analysis of the submitted data revealed that many of the experimental data, but also the data from QSARs and other calculation methods, underestimate the actual bioaccumulation potential of hydrophobic substances considerably. One of the main reasons in the nonexperimental studies is that the BCF is related there to the total concentration of the chemical in water and not to the dissolved chemical concentration. There is therefore an urgent need to reassess the bioaccumulation potential of the hydrophobic substances registered under REACH. Based on the model calculations in the present study, between 332 and 584 substances that are registered under REACH are likely to bioaccumulate in the aquatic environment-many more than have so far been identified in the B assessment. Integr Environ Assess Manag 2023;19:792-803. © 2022 The Authors. Integrated Environmental Assessment and Management published by Wiley Periodicals LLC on behalf of Society of Environmental Toxicology & Chemistry (SETAC).
Subject(s)
Water Pollutants, Chemical , Animals , Bioaccumulation , Water Pollutants, Chemical/analysis , Ecotoxicology/methods , Hydrophobic and Hydrophilic Interactions , Risk AssessmentABSTRACT
Background: The NORMAN Association (https://www.norman-network.com/) initiated the NORMAN Suspect List Exchange (NORMAN-SLE; https://www.norman-network.com/nds/SLE/) in 2015, following the NORMAN collaborative trial on non-target screening of environmental water samples by mass spectrometry. Since then, this exchange of information on chemicals that are expected to occur in the environment, along with the accompanying expert knowledge and references, has become a valuable knowledge base for "suspect screening" lists. The NORMAN-SLE now serves as a FAIR (Findable, Accessible, Interoperable, Reusable) chemical information resource worldwide. Results: The NORMAN-SLE contains 99 separate suspect list collections (as of May 2022) from over 70 contributors around the world, totalling over 100,000 unique substances. The substance classes include per- and polyfluoroalkyl substances (PFAS), pharmaceuticals, pesticides, natural toxins, high production volume substances covered under the European REACH regulation (EC: 1272/2008), priority contaminants of emerging concern (CECs) and regulatory lists from NORMAN partners. Several lists focus on transformation products (TPs) and complex features detected in the environment with various levels of provenance and structural information. Each list is available for separate download. The merged, curated collection is also available as the NORMAN Substance Database (NORMAN SusDat). Both the NORMAN-SLE and NORMAN SusDat are integrated within the NORMAN Database System (NDS). The individual NORMAN-SLE lists receive digital object identifiers (DOIs) and traceable versioning via a Zenodo community (https://zenodo.org/communities/norman-sle), with a total of > 40,000 unique views, > 50,000 unique downloads and 40 citations (May 2022). NORMAN-SLE content is progressively integrated into large open chemical databases such as PubChem (https://pubchem.ncbi.nlm.nih.gov/) and the US EPA's CompTox Chemicals Dashboard (https://comptox.epa.gov/dashboard/), enabling further access to these lists, along with the additional functionality and calculated properties these resources offer. PubChem has also integrated significant annotation content from the NORMAN-SLE, including a classification browser (https://pubchem.ncbi.nlm.nih.gov/classification/#hid=101). Conclusions: The NORMAN-SLE offers a specialized service for hosting suspect screening lists of relevance for the environmental community in an open, FAIR manner that allows integration with other major chemical resources. These efforts foster the exchange of information between scientists and regulators, supporting the paradigm shift to the "one substance, one assessment" approach. New submissions are welcome via the contacts provided on the NORMAN-SLE website (https://www.norman-network.com/nds/SLE/). Supplementary Information: The online version contains supplementary material available at 10.1186/s12302-022-00680-6.
ABSTRACT
The essential-use concept is a tool that can guide the phase-out of per- and polyfluoroalkyl substances (PFAS) and potentially other substances of concern. This concept is a novel approach to chemicals management that determines whether using substances of concern, such as PFAS, is truly essential for a given functionality. To assess the essentiality of a particular use case, three considerations need to be addressed: (1) the function (chemical, end use and service) that the chemical provides in the use case, (2) whether the function is necessary for health and safety and critical for the functioning of society and (3) if the function is necessary, whether there are viable alternatives for the chemical for this particular use. A few illustrative examples of the three-step process are provided for use cases of PFAS. The essential-use concept takes chemicals management away from a substance-by-substance approach to a group approach. For PFAS and other substances of concern, it offers a more rapid pathway toward effective management or phase-out. Parts of the concept of essential use have already been widely applied in global treaties and international regulations and it has also been recently used by product manufacturers and retailers to phase out substances of concern from supply chains. Herein some of the common questions and misinterpretations regarding the practical application of the essential-use concept are reviewed, and answers and further clarifications are provided.
Subject(s)
Fluorocarbons , HumansABSTRACT
Per- and polyfluoroalkyl substances (PFAS) are a class of synthetic organic substances with diverse structures, properties, uses, bioaccumulation potentials and toxicities. Despite this high diversity, all PFAS are alike in that they contain perfluoroalkyl moieties that are extremely resistant to environmental and metabolic degradation. The vast majority of PFAS are therefore either non-degradable or transform ultimately into stable terminal transformation products (which are still PFAS). Under the European chemicals regulation this classifies PFAS as very persistent substances (vP). We argue that this high persistence is sufficient concern for their management as a chemical class, and for all "non-essential" uses of PFAS to be phased out. The continual release of highly persistent PFAS will result in increasing concentrations and increasing probabilities of the occurrence of known and unknown effects. Once adverse effects are identified, the exposure and associated effects will not be easily reversible. Reversing PFAS contamination will be technically challenging, energy intensive, and costly for society, as is evident in the efforts to remove PFAS from contaminated land and drinking water sources.
Subject(s)
Drinking Water , Fluorocarbons , Water Pollutants, Chemical , Drinking Water/analysis , Fluorocarbons/analysis , Fluorocarbons/toxicity , Water Pollutants, Chemical/analysisABSTRACT
Per- and polyfluoroalkyl substances (PFAS) are of concern because of their high persistence (or that of their degradation products) and their impacts on human and environmental health that are known or can be deduced from some well-studied PFAS. Currently, many different PFAS (on the order of several thousands) are used in a wide range of applications, and there is no comprehensive source of information on the many individual substances and their functions in different applications. Here we provide a broad overview of many use categories where PFAS have been employed and for which function; we also specify which PFAS have been used and discuss the magnitude of the uses. Despite being non-exhaustive, our study clearly demonstrates that PFAS are used in almost all industry branches and many consumer products. In total, more than 200 use categories and subcategories are identified for more than 1400 individual PFAS. In addition to well-known categories such as textile impregnation, fire-fighting foam, and electroplating, the identified use categories also include many categories not described in the scientific literature, including PFAS in ammunition, climbing ropes, guitar strings, artificial turf, and soil remediation. We further discuss several use categories that may be prioritised for finding PFAS-free alternatives. Besides the detailed description of use categories, the present study also provides a list of the identified PFAS per use category, including their exact masses for future analytical studies aiming to identify additional PFAS.
Subject(s)
Fluorocarbons , Water Pollutants, Chemical , Construction Materials , Fluorocarbons/analysis , Humans , Soil , Textiles , Water Pollutants, Chemical/analysisABSTRACT
Grouping strategies are needed for per- and polyfluoroalkyl substances (PFAS), in part, because it would be time and resource intensive to test and evaluate the more than 4700 PFAS on the global market on a chemical-by-chemical basis. In this paper we review various grouping strategies that could be used to inform actions on these chemicals and outline the motivations, advantages and disadvantages for each. Grouping strategies are subdivided into (1) those based on the intrinsic properties of the PFAS (e.g. persistence, bioaccumulation potential, toxicity, mobility, molecular size) and (2) those that inform risk assessment through estimation of cumulative exposure and/or effects. The most precautionary grouping approach of those reviewed within this article suggests phasing out PFAS based on their high persistence alone (the so-called "P-sufficient" approach). The least precautionary grouping approach reviewed advocates only grouping PFAS for risk assessment that have the same toxicological effects, modes and mechanisms of action, and elimination kinetics, which would need to be well documented across different PFAS. It is recognised that, given jurisdictional differences in chemical assessment philosophies and methodologies, no one strategy will be generally acceptable. The guiding question we apply to the reviewed grouping strategies is: grouping for what purpose? The motivation behind the grouping (e.g. determining use in products vs. setting guideline levels for contaminated environments) may lead to different grouping decisions. This assessment provides the necessary context for grouping strategies such that they can be adopted as they are, or built on further, to protect human and environmental health from potential PFAS-related effects.
Subject(s)
Environmental Health , Fluorocarbons , Bioaccumulation , Humans , Risk AssessmentABSTRACT
Persistent organic pollutants (POPs), such as polychlorinated biphenyls (PCBs), are ubiquitous environmental contaminants that have been targeted by national regulations since the 1970-1980s, followed in 2004 by the worldwide regulation under the Stockholm Convention on POPs. However, concerns are growing regarding the emergence of additional POP-like substances, such as chlorinated paraffins (CPs), which have particularly large production volumes. Whereas short-chain CPs (SCCPs) have recently been restricted in Europe and are currently under evaluation for inclusion into the Stockholm Convention, medium-chain CPs (MCCPs) have received little attention. On the one hand, temporal trends of CPs in the environment have hardly been investigated. On the other hand, the effectiveness of the Stockholm Convention on environmental levels of PCBs is still a matter of debate. Here, we reconstructed temporal trends of SCCPs, MCCPs, and PCBs in archived soil samples from six sampling sites in Switzerland, covering the period 1989-2014 (respectively 1988-2013 for one site). Concentrations of SCCPs have decreased in soil since 1994, which indicates positive effects of the reduction of production of SCCPs in Europe and the increasingly stringent regulation. However, the decline in soil is slow with a halving time of 18 years. Concentrations of MCCPs have continuously increased in soil over the entire period 1989-2014, with a doubling between 2009 and 2014. The concentrations of MCCPs have surpassed those of SCCPs, showing their relevance today, partly as replacements for SCCPs. Soil concentrations of PCBs peaked in 1999, i.e. three decades later than worldwide production and use of PCBs, but earlier than the entry into force of the Stockholm Convention. PCBs follow a decline in soil with a halving time of approx. 8 years. This study shows the usefulness of sample archives for the reconstruction and interpretation of time trends of persistent environmental contaminants.
Subject(s)
Environmental Monitoring/standards , Paraffin/analysis , Paraffin/standards , Polychlorinated Biphenyls/analysis , Polychlorinated Biphenyls/standards , Soil Pollutants/analysis , Soil Pollutants/standards , Environmental Pollution , Europe , Guidelines as Topic , Switzerland , Time FactorsABSTRACT
Polychlorinated biphenyls (PCBs) are persistent organic compounds that are ubiquitously found in the environment. Their use and manufacture were restricted or banned in many countries in the 1970-1980s, however, they still persist in the antroposphere, the environment and in biota worldwide today. Conventions like the Convention on Long-range Transboundary Air Pollution encourage or bind the member parties to annually submit emission inventories of regulated air pollutants. Unfortunately, several member states have not yet reported PCB emissions. The identification and quantification of stocks and emissions sources is, however, an important precondition to handle and remove the remaining reservoirs of PCBs and, thus, to be able to reduce emissions and subsequently environmental exposure. Here, we estimate past, present, and future emissions of PCBs to air in Switzerland and provide emission factors for all relevant emission categories. Switzerland hereby represents a typical developed industrial country, and most of the assumptions and parameters presented here can be used to calculate PCB emission also for other countries. PCB emissions to air are calculated using a dynamic mass flow and emissions model for Switzerland, which is run for the years 1930-2100. The results point out the importance of the use of PCBs in open applications, which have largely been previously overlooked. Additionally, we show that PCBs will persist in applications during the coming decades with ongoing emissions. Especially the use of PCBs in open applications will cause Swiss emissions to remain above 100 kg PCB per year, even after the year 2030. Our developed model is available in Excel/VBA and can be downloaded with this article.
Subject(s)
Air Pollutants/analysis , Air Pollution/analysis , Environmental Monitoring/methods , Polychlorinated Biphenyls/analysis , Models, Theoretical , SwitzerlandABSTRACT
Polychlorinated biphenyls (PCBs) are banned worldwide under the Stockholm Convention on Persistent Organic Pollutants. However, PCBs are still emitted in appreciable amounts from remaining primary sources in urban areas or landfills and are ubiquitous environmental contaminants, inter alia in soil and air. Concentrations of PCBs have been measured in various media by numerous studies worldwide. However, monitoring data do not always provide quantitative information about transport processes between different media, deposition fluxes to ground, or distribution of PCBs between environmental compartments. Also future trends in environmental contamination by PCBs cannot be predicted from monitoring data, but such information is highly relevant for decision-makers. Here, we present a new regionally resolved dynamic multimedia mass balance model for Switzerland to investigate the origin of PCBs in air and to investigate their long-term fate and mass balance in the environment. The model was validated with existing field data for PCBs. We find that advective inflow of PCBs from outside Switzerland into the atmospheric boundary layer is responsible for 80% of PCBs present in air in Switzerland, whereas Swiss emissions cause the remaining 20%. Furthermore, we show that the atmospheric deposition of the higher-chlorinated PCBs is dominated by particle-bound deposition, whereas the deposition of the lower-chlorinated PCBs is a combination of particle-bound and gaseous deposition. The volume fraction of particles in air is in both cases an important factor driving the deposition of PCBs to ground and, thus, contributing to the higher concentrations of PCBs generally observed in populated and polluted areas. Regional emissions influence the deposition fluxes only to a limited extent. We also find that secondary emissions from environmental reservoirs do not exceed primary emissions for all PCB congeners until at least 2036. Finally, we use our model to evaluate the effect of chemical regulation on future environmental contamination by PCBs.