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FULLTEXT01.Pdf http://www.diva-portal.org This is the published version of a paper published in Science of the Total Environment. Citation for the original published paper (version of record): Arp, H P., Morin, N A., Andersson, P L., Hale, S E., Wania, F. et al. (2020) The presence, emission and partitioning behavior of polychlorinated biphenyls in waste, leachate and aerosols from Norwegian waste-handling facilities Science of the Total Environment, 715: 1-12 https://doi.org/10.1016/j.scitotenv.2020.136824 Access to the published version may require subscription. N.B. When citing this work, cite the original published paper. Permanent link to this version: http://urn.kb.se/resolve?urn=urn:nbn:se:umu:diva-169377 Science of the Total Environment 715 (2020) 136824 Contents lists available at ScienceDirect Science of the Total Environment journal homepage: www.elsevier.com/locate/scitotenv The presence, emission and partitioning behavior of polychlorinated biphenyls in waste, leachate and aerosols from Norwegian waste- handling facilities Hans Peter H. Arp a,b,⁎, Nicolas A.O. Morin a,c,PatrikL.Anderssond, Sarah E. Hale a, Frank Wania e, Knut Breivik f,g, Gijs D. Breedveld a,h a Norwegian Geotechnical Institute (NGI), P.O. Box 3930, Ullevål Stadion, N-0806 Oslo, Norway b Department of Chemistry, Norwegian University of Science and Technology (NTNU), N-7491 Trondheim, Norway c Environmental and Food Laboratory of Vendée (LEAV), Department of Chemistry, Rond-point Georges Duval CS 80802, 85021 La Roche-sur-Yon, France d Department of Chemistry, Umeå University, SE-90187 Umeå, Sweden e Department of Physical and Environmental Sciences, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario M1C 1A4, Canada f Norwegian Institute for Air Research, P.O. Box 100, NO-2027 Kjeller, Norway g Department of Chemistry, University of Oslo, P.O. Box 1033, NO-0315 Oslo, Norway h Department of Geosciences, University of Oslo, P.O. Box 1047, NO-0316 Oslo, Norway HIGHLIGHTS GRAPHICAL ABSTRACT • Despite the 1980s phase out, PCBs are still found in plastic waste in the mg/kg range. • Waste recycling in Norway leads to en- vironmental emissions of PCBs. • Particles in leachate exhibit PCB partitioning similar to waste on site. • Air emissions of PCB are mostly in the gas-phase, BFRs in the particle-phase. • Air PCB concentrations in Norwegian and Chinese WEEE facilities are comparable. article info abstract Article history: Even though production and open use of polychlorinated biphenyls (PCBs) have been phased out in Western Received 23 November 2019 industrialised countries since the 1980s, PCBs were still present in waste collected from different waste handling Received in revised form 17 January 2020 facilities in Norway in 2013. Sums of seven indicator-PCBs (I-PCB7: PCB-28, -52, -101, -118, -138, -153 and -180) Accepted 18 January 2020 were highest in plastic waste (3700 ±1800 μg/kg, n=15), waste electrical and electronic equipment (WEEE) Available online 21 January 2020 (1300 ± 400 μg/kg, n=12) and fine vehicle fluff (1800 ± 1400 μg/kg, n=4) and lowest in glass waste, combus- fl μ Editor: Damia Barcelo tibles, bottom ash and y ash (0.3 to 65 g/kg). Concentrations in leachate water varied from 1.7 to 2900 ng/L, with higher concentrations found at vehicle and WEEE handling facilities. Particles in leachate water exhibited Keywords: similar PCB sorption properties as solid waste collected on site, with waste-water partitioning coefficients rang- 5 7 3 Waste ing from 10 to 10 . I-PCB7 in air samples collected at the sites were mostly in the gas phase (100–24000 pg/m ), Recycling compared to those associated with particles (9–1900 pg/m3). In contrast, brominated flame retardants (BFRs) in Leachate the same samples were predominantly found associated with particles (e.g. sum of 10 brominated diethyl ethers, ⁎ Corresponding author at: Norwegian Geotechnical Institute (NGI), P.O. Box 3930, Ullevål Stadion, N-0806 Oslo, Norway. E-mail address: [email protected] (H.P.H. Arp). https://doi.org/10.1016/j.scitotenv.2020.136824 0048-9697/© 2020 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). 2 H.P.H. Arp et al. / Science of the Total Environment 715 (2020) 136824 3 3 Gas-particle ΣBDE10, associated with particles 77–194,000 pg/m )comparedtothegasphase(ΣBDE10 6–473 pg/m ). Mea- Emissions sured gas-phase I-PCB7 concentrations are less than predicted, assuming waste-air partitioning in equilibrium WEEE with predominant waste on site. However, the gas-particle partitioning behavior of PCBs and BFRs could be pre- Plastic dicted using an established partitioning model for ambient aerosols. PCB emissions from Norwegian waste han- dling facilities occurred primarily in the form of atmospheric vapor or leachate particles. © 2020 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http:// creativecommons.org/licenses/by/4.0/). 1. Introduction Hence, how various materials and wastes that contain PCBs are being recycled and/or disposed of is likely to remain an issue for con- Polychlorinated biphenyls (PCBs) are among the initial “dirty dozen” temporary waste management strategies now and well into the future substances regulated under the Stockholm Convention on Persistent Or- (Bergsdal et al., 2014). Even though new uses of PCBs were banned in ganic Pollutants (POPs) (UNEP, 2001) because they are persistent, Norway in 1980, there are still approximately 100 t of PCB estimated bioaccumulative, toxic, prone to long-range transport and pose a poten- to be present in products and building structures (Miljøstatus, 2018). tial risk to environmental and human health. PCBs were extensively The PCB problem may not be solved without a better understanding of produced in major industrialized countries as technical mixtures from the occurrence and fate of PCBs during recycling and disposal. ~1930 until 1994. During this time N1.3 million tonnes were produced, In this work, the fate of PCBs was studied at 12 different sites with peak production occurring around 1970 (Breivik et al., 2007). throughout Norway and compared with that of the brominated flame The cumulative historical consumption in Norway has been estimated retardants (BFRs) at the same facilities reported previously (Morin at 1307 t (Miljødirektoratet, 2010). PCBs proved to be versatile et al., 2017). Whereas atmospheric concentrations of BFRs were higher chemicals and therefore found use in a large variety of applications. at WEEE/vehicle collecting facilities (e.g. total air concentration of the However, concerns about the potential environmental hazards emerg- sum of 10 brominated diethyl ethers, Σ BDE10,of ing first in the late 1960s eventually terminated the usage of PCBs 9000–195,000 pg/m3) compared to incineration and landfilling facilities within applications where there was no or limited possibility for recol- (80–90 pg/m3), leachate concentrations were not significantly different lection. For example, open usage such as in plastics as plasticisers and between these facilities (ranging from 1 to 3500 ng/L). Samples were flame retardants, within carbonless copy paper and several other such collected over a period of one year using both active and passive sam- applications ended within the member countries of the Organisation pling techniques. Concentrations in solid waste handled at the facilities for Economic Co-operation and Development (OECD) by 1973 (de were measured along with air and leachate concentrations. These data Voogt and Brinkman, 1989). Usage of PCBs within closed electrical sys- were in turn used to quantify the partitioning behaviour of PCBs be- tems, such as capacitors and transformers, however, was discontinued tween waste, leachate and aerosol particles present at these sites. This later than open usages (Breivik et al., 2002). A characteristic feature of study tested the following hypotheses: (a) waste handling facilities the historical use pattern of PCBs is its application in many long-lived are inherently contaminated by PCBs, thereby contaminating waste products, including building materials like paints (Jartun et al., 2009), sorted for recycling and the environment around the waste-handling fa- sealants (Kohler et al., 2005), as well as electrical equipment. Storage cility, (b) the fate and transport of PCBs released to air and leachate of obsolete equipment may further delay recycling and disposal water is affected by particulate matter generated from the waste, (Saphores et al., 2009). For example, small capacitors containing PCBs, (c) the fate and transport behavior from waste handling facilities of which were used in cars and various electrical household appliances PCBs deviates from that of BFRs. (Harrad et al., 1994), have an estimated average use-life expectancy of about 10 to 15 years, with larger electrical equipment (larger capacitors 2. Materials and methods and transformers) of up to 30 years (NTIS, 1972). For PCBs used in closed electrical systems, significant releases may not occur as long as 2.1. PCBs investigated the electrical equipment is kept intact during use or storage, but rather occur if those systems are improperly managed at the waste and The analysis was limited to seven indicator congeners I-PCB7, that recycling stage, as is evident from elevated emissions at informal e- were 2,4,4′-trichlorobiphenyl (PCB-28), 2,2′,5,5′-tetrachlorobiphenyl waste recycling areas within developing regions (Han et al., 2010; (PCB-52), 2,2′,4,5,5′-pentachlorobiphenyl (PCB-101), 2,3′,4,4′,5- Breivik et al., 2011). In the case of PCBs in building materials, the poten- pentachlorobiphenyl (PCB-118), 2,2′,3,4,4′,5′-hexachlorobiphenyl tial for continued releases call for even longer time perspectives (PCB-138), 2,2′,4,4′,5,5′-hexachlorobiphenyl (PCB-153), and (Bergsdal et al., 2014). These persistent PCB emission sources have the 2,2′,3,4,4′,5,5′-heptachlorobiphenyl (PCB-180).
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