The Global Monitoring Plan of the Stockholm Convention on Persistent Organic Pollutants (POPs) was established to generate long-term data necessary for evaluating the effectiveness of regulatory measures at a global scale. After 15 years of passive air monitoring (2003-2019), MONET is the first network to produce sufficient data for the analysis of continuous long-term temporal trends of POPs in air across the entire European continent. This study reports long-term concentrations of 20 POPs monitored at 32 sites in 27 European countries. As of January 1, 2019, the concentration ranges (pg/m3) were 1.1-52.8 (∑6PCB), 0.3-8.5 (∑12dl-PCB), 0.007-0.175 (∑17PCDD/F), 0.02-2.2 (∑9PBDE), 0.4-24.7 (BDE 209), 0.5-247 (∑6DDT), 1.7-818 (∑4HCH), 15.8-74.7 (HCB), and 5.9-21.5 (PeCB). Temporal trends indicate that concentrations of most POPs have declined significantly over the past 15 years, with median annual decreases ranging from -8.0 to -11.5% (halving times of 6-8 years) for ∑6PCB, ∑17PCDD/F, HCB, PeCB, and ∑9PBDE. Furthermore, no statistically significant differences were observed in either the trends or the concentrations of specific POPs at sites in Western Europe (WEOG) compared to sites in Central and Eastern Europe (CEE), which suggests relatively uniform compound-specific distribution and removal at the continental scale.

Institute of Biogeochemistry and Pollutant Dynamics ETH Zürich 8092 Zürich Switzerland

RECETOX Masaryk University 625 00 Brno Czech Republic

Zobrazit více v PubMed

Halse A. K.; Schlabach M.; Eckhardt S.; Sweetman A.; Jones K. C.; Breivik K. Spatial Variability of POPs in European Background Air. Atmos. Chem. Phys. 2011, 11, 1549–1564. 10.5194/acp-11-1549-2011. DOI

Pribylova P.; Kares R.; Boruvkova J.; Cupr P.; Prokes R.; Kohoutek J.; Holoubek I.; Klanova J. Levels of Persistent Organic Pollutants and Polycyclic Aromatic Hydrocarbons in Ambient Air of Central and Eastern Europe. Atmos. Pollut. Res. 2012, 3, 494–505. 10.5094/APR.2012.057. DOI

Tørseth K.; Aas W.; Breivik K.; Fjæraa A. M.; Fiebig M.; Hjellbrekke A.-G.; Lund Myhre C.; Solberg S.; Yttri K. E. Introduction to the European Monitoring and Evaluation Programme (EMEP) and Observed Atmospheric Composition Change during 1972-2009. Atmos. Chem. Phys. 2012, 12, 5447–5481. 10.5194/acp-12-5447-2012. DOI

Halvorsen H. L.; Bohlin-Nizzetto P.; Eckhardt S.; Gusev A.; Moeckel C.; Shatalov V.; Pedersen Skogeng L.; Breivik K. Spatial Variability and Temporal Changes of POPs in European Background Air. Atmos. Environ. 2023, 299, 119658.10.1016/j.atmosenv.2023.119658. DOI

Wong F.; Hung H.; Dryfhout-Clark H.; Aas W.; Bohlin-Nizzetto P.; Breivik K.; Mastromonaco M. N.; Lundén E. B.; Ólafsdóttir K.; Sigurd̵sson Á.; Vorkamp K.; Bossi R.; Skov H.; Hakola H.; Barresi E.; Sverko E.; Fellin P.; Li H.; Vlasenko A.; Zapevalov M.; Samsonov D.; Wilson S. Time Trends of Persistent Organic Pollutants (POPs) and Chemicals of Emerging Arctic Concern (CEAC) in Arctic Air from 25 Years of Monitoring. Sci. Total Environ. 2021, 775, 145109.10.1016/j.scitotenv.2021.145109. PubMed DOI

Wong F.; Shoeib M.; Katsoyiannis A.; Eckhardt S.; Stohl A.; Bohlin-Nizzetto P.; Li H.; Fellin P.; Su Y.; Hung H. Assessing Temporal Trends and Source Regions of Per- and Polyfluoroalkyl Substances (PFASs) in Air under the Arctic Monitoring and Assessment Programme (AMAP). Atmos. Environ. 2018, 172, 65–73. 10.1016/j.atmosenv.2017.10.028. DOI

Graf C.; Katsoyiannis A.; Jones K. C.; Sweetman A. J. The TOMPs Ambient Air Monitoring Network – Continuous Data on UK Air Quality for over 20 Years. Environ. Pollut. 2016, 217, 42–51. 10.1016/j.envpol.2016.01.033. PubMed DOI

Wöhrnschimmel H.; Scheringer M.; Bogdal C.; Hung H.; Salamova A.; Venier M.; Katsoyiannis A.; Hites R. A.; Hungerbuhler K.; Fiedler H. Ten Years after Entry into Force of the Stockholm Convention: What Do Air Monitoring Data Tell about Its Effectiveness?. Environ. Pollut. 2016, 217, 149–158. 10.1016/j.envpol.2016.01.090. PubMed DOI

Hung H.; Katsoyiannis A. A.; Guardans R. Ten Years of Global Monitoring under the Stockholm Convention on Persistent Organic Pollutants (POPs): Trends, Sources and Transport Modelling. Environ. Pollut. 2016, 217, 1–3. 10.1016/j.envpol.2016.05.035. PubMed DOI

Anttila P.; Brorström-Lundén E.; Hansson K.; Hakola H.; Vestenius M. Assessment of the Spatial and Temporal Distribution of Persistent Organic Pollutants (POPs) in the Nordic Atmosphere. Atmos. Environ. 2016, 140, 22–33. 10.1016/J.ATMOSENV.2016.05.044. DOI

Kong D.; Macleod M.; Hung H.; Cousins I. T. Statistical Analysis of Long-Term Monitoring Data for Persistent Organic Pollutants in the Atmosphere at 20 Monitoring Stations Broadly Indicates Declining Concentrations. Environ. Sci. Technol. 2014, 48, 12492.10.1021/es502909n. PubMed DOI

Becker S.; Halsall C. J.; Tych W.; Kallenborn R.; Schlabach M.; Manø S. Changing sources and environmental factors reduce the rates of decline of organochlorine pesticides in the Arctic atmosphere. Atmos. Chem. Phys. 2012, 12, 4033–4044. 10.5194/acp-12-4033-2012. DOI

Birgul A.; Katsoyiannis A.; Gioia R.; Crosse J.; Earnshaw M.; Ratola N.; Jones K. C.; Sweetman A. J. Atmospheric Polybrominated Diphenyl Ethers (PBDEs) in the United Kingdom. Environ. Pollut. 2012, 169, 105–111. 10.1016/j.envpol.2012.05.005. PubMed DOI

Kalina J.; Scheringer M.; Borůvková J.; Kukučka P.; Přibylová P.; Bohlin-Nizzetto P.; Klánová J. Passive Air Samplers As a Tool for Assessing Long-Term Trends in Atmospheric Concentrations of Semivolatile Organic Compounds. Environ. Sci. Technol. 2017, 51, 7047–7054. 10.1021/acs.est.7b02319. PubMed DOI

Klánová J.; Kohoutek J.; Kostrhounová R.; Holoubek I. Are the Residents of Former Yugoslavia Still Exposed to Elevated PCB Levels Due to the Balkan Wars?. Part 1: Air Sampling in Croatia, Serbia, Bosnia and Herzegovina. Environ. Int. 2007, 33, 719–726. 10.1016/j.envint.2007.02.004. PubMed DOI

Klánová J.; Kohoutek J.; Čupr P.; Holoubek I. Are the Residents of Former Yugoslavia Still Exposed to Elevated PCB Levels Due to the Balkan Wars? Part 2: Passive Air Sampling Network. Environ. Int. 2007, 33, 727–735. 10.1016/j.envint.2007.02.005. PubMed DOI

Kalina J.; Scheringer M.; Boruvkova J.; Kukucka P.; Přibylová P.; Sáňka O.; Melymuk L.; Vana M.; Klánová J. Characterizing Spatial Diversity of Passive Sampling Sites for Measuring Levels and Trends of Semivolatile Organic Chemicals. Environ. Sci. Technol. 2018, 52, 10599–10608. 10.1021/acs.est.8b03414. PubMed DOI

White K. B.; Sáňka O.; Melymuk L.; Přibylová P.; Klánová J. Application of Land Use Regression Modelling to Describe Atmospheric Levels of Semivolatile Organic Compounds on a National Scale. Sci. Total Environ. 2021, 793, 148520.10.1016/j.scitotenv.2021.148520. PubMed DOI

Pozo K.; Harner T.; Wania F.; Muir D. C. G.; Jones K. C.; Barrie L. A. Toward a Global Network for Persistent Organic Pollutants in Air: Results from the GAPS Study. Environ. Sci. Technol. 2006, 40, 4867–4873. 10.1021/es060447t. PubMed DOI

Pozo K.; Harner T.; Lee S. C.; Wania F.; Muir D. C. G.; Jones K. C. Seasonally Resolved Concentrations of Persistent Organic Pollutants in the Global Atmosphere from the First Year of the GAPS Study. Environ. Sci. Technol. 2009, 43, 796–803. 10.1021/es802106a. PubMed DOI

Shunthirasingham C.; Oyiliagu C. E.; Cao X.; Gouin T.; Wania F.; Lee S. C.; Pozo K.; Harner T.; Muir D. C. G. Spatial and Temporal Pattern of Pesticides in the Global Atmosphere. J. Environ. Monit. 2010, 12, 1650–1657. 10.1039/c0em00134a. PubMed DOI

Rauert C.; Schuster J. K.; Eng A.; Harner T. Global Atmospheric Concentrations of Brominated and Chlorinated Flame Retardants and Organophosphate Esters. Environ. Sci. Technol. 2018, 52, 2777–2789. 10.1021/acs.est.7b06239. PubMed DOI

Rauert C.; Shoieb M.; Schuster J. K.; Eng A.; Harner T. Atmospheric Concentrations and Trends of Poly- and Perfluoroalkyl Substances (PFAS) and Volatile Methyl Siloxanes (VMS) over 7 Years of Sampling in the Global Atmospheric Passive Sampling (GAPS) Network. Environ. Pollut. 2018, 238, 94–102. 10.1016/j.envpol.2018.03.017. PubMed DOI

Schuster J. K.; Harner T.; Eng A.; Rauert C.; Su K.; Hornbuckle K. C.; Johnson C. W. Tracking POPs in Global Air from the First 10 Years of the GAPS Network (2005 to 2014). Environ. Sci. Technol. 2021, 55, 9479–9488. 10.1021/acs.est.1c01705. PubMed DOI PMC

Klánová J.; Harner T. The Challenge of Producing Reliable Results under Highly Variable Conditions and the Role of Passive Air Samplers in the Global Monitoring Plan. TrAC, Trends Anal. Chem. 2013, 46, 139–149. 10.1016/j.trac.2012.07.021. DOI

Kalina J.; White K. B.; Scheringer M.; Přibylová P.; Kukučka P.; Audy O.; Klánová J. Comparability of Long-Term Temporal Trends of POPs from Co-Located Active and Passive Air Monitoring Networks in Europe. Environ. Sci.: Processes Impacts 2019, 21, 1132–1142. 10.1039/C9EM00136K. PubMed DOI

Bohlin-Nizzetto P.; Melymuk L.; White K. B.; Kalina J.; Madadi V. O.; Adu-Kumi S.; Prokeš R.; Přibylová P.; Klánová J. Field- and Model-Based Calibration of Polyurethane Foam Passive Air Samplers in Different Climate Regions Highlights Differences in Sampler Uptake Performance. Atmos. Environ. 2020, 238, 117742.10.1016/j.atmosenv.2020.117742. DOI

Kalina J.; White K. B.; Scheringer M.; Přibylová P.; Kukučka P.; Audy O.; Martinik J.; Klánová J. Comparability of Semivolatile Organic Compound Concentrations from Co-Located Active and Passive Air Monitoring Networks in Europe. Environ. Sci.: Processes Impacts 2022, 24, 898–909. 10.1039/d2em00007e. PubMed DOI

Kirchner M.; Freier K. P.; Denner M.; Ratz G.; Jakobi G.; Körner W.; Ludewig E.; Schaub M.; Schramm K. W.; Weiss P.; Moche W. Air Concentrations and Deposition of Chlorinated Dioxins and Furans (PCDD/F) at Three High Alpine Monitoring Stations: Trends and Dependence on Air Masses. Atmos. Environ. 2020, 223, 117199.10.1016/j.atmosenv.2019.117199. DOI

Kirchner M.; Jakobi G.; Körner W.; Levy W.; Moche W.; Niedermoser B.; Schaub M.; Ries L.; Weiss P.; Antritter F.; Fischer N.; Henkelmann B.; Schramm K. W. Ambient Air Levels of Organochlorine Pesticides at Three High Alpine Monitoring Stations: Trends and Dependencies on Geographical Origin. Aerosol Air Qual. Res. 2016, 16, 738–751. 10.4209/aaqr.2015.04.0213. DOI

Roscales J. L.; Muñoz-Arnanz J.; Ros M.; Vicente A.; Barrios L.; Jiménez B. Assessment of POPs in Air from Spain Using Passive Sampling from 2008 to 2015. Part I: Spatial and Temporal Observations of PBDEs. Sci. Total Environ. 2018, 634, 1657–1668. 10.1016/j.scitotenv.2018.03.043. PubMed DOI

Muñoz-Arnanz J.; Roscales J. L.; Vicente A.; Ros M.; Barrios L.; Morales L.; Abad E.; Jiménez B. Assessment of POPs in Air from Spain Using Passive Sampling from 2008 to 2015. Part II: Spatial and Temporal Observations of PCDD/Fs and Dl-PCBs. Sci. Total Environ. 2018, 634, 1669–1679. 10.1016/j.scitotenv.2018.04.164. PubMed DOI

White K. B.; Kalina J.; Scheringer M.; Přibylová P.; Kukučka P.; Kohoutek J.; Prokeš R.; Klánová J. Temporal Trends of Persistent Organic Pollutants across Africa after a Decade of MONET Passive Air Sampling. Environ. Sci. Technol. 2021, 55, 9413–9424. 10.1021/acs.est.0c03575. PubMed DOI

Borůvková J.; Gregor J.; Šebková K.; Bednářová Z.; Kalina J.; Hůlek R.; Dušek L.; Holoubek I.; Klánová J.. GENASIS—Global Environmental Assessment and Information System. http://www.genasis.cz (accessed July 24, 2019).

Wania F.; Shunthirasingham C. Passive Air Sampling for Semi-Volatile Organic Chemicals. Environ. Sci.: Processes Impacts 2020, 22, 1925–2002. 10.1039/d0em00194e. PubMed DOI

Saini A.; Clarke J.; Harner T. Direct Measurements of Polyurethane Foam (PUF) – Air Partitioning Coefficients for Chemicals of Emerging Concern Capable of Equilibrating in PUF Disk Samplers. Chemosphere 2019, 234, 925–930. 10.1016/j.chemosphere.2019.06.134. PubMed DOI

Gelaro R.; McCarty W.; Suárez M. J.; Todling R.; Molod A.; Takacs L.; Randles C. A.; Darmenov A.; Bosilovich M. G.; Reichle R.; Wargan K.; Coy L.; Cullather R.; Draper C.; Akella S.; Buchard V.; Conaty A.; da Silva A. M.; Gu W.; Kim G. K.; Koster R.; Lucchesi R.; Merkova D.; Nielsen J. E.; Partyka G.; Pawson S.; Putman W.; Rienecker M.; Schubert S. D.; Sienkiewicz M.; Zhao B. The Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2). J. Clim. 2017, 30, 5419–5454. 10.1175/JCLI-D-16-0758.1. PubMed DOI PMC

Herkert N. J.; Spak S. N.; Smith A.; Schuster J. K.; Harner T.; Martinez A.; Hornbuckle K. C. Calibration and Evaluation of PUF-PAS Sampling Rates across the Global Atmospheric Passive Sampling (GAPS) Network. Environ. Sci.: Processes Impacts 2018, 20, 210–219. 10.1039/c7em00360a. PubMed DOI PMC

Theil H.A Rank-Invariant Method of Linear and Polynomial Regression Analysis. Henri Theil’s Contributions to Economics and Econometrics; Springer Science & Business Media, 1992; Vol. 3( (1950), ), pp 345–381.

Sen P. K. Estimates of the Regression Coefficient Based on Kendall’s Tau. J. Am. Stat. Assoc. 1968, 63, 1379–1389. 10.1080/01621459.1968.10480934. DOI

Mann H. B.; Whitney D. R. On a Test of Whether One of Two Random Variables Is Stochastically Larger than the Other. Ann. Math. Stat. 1947, 18, 50–60. 10.1214/aoms/1177730491. DOI

Breivik K.; Sweetman A.; Pacyna J. M.; Jones K. C. Towards a Global Historical Emission Inventory for Selected PCB Congeners - A Mass Balance Approach: 1. Global Production and Consumption. Sci. Total Environ. 2002, 290, 181–198. 10.1016/S0048-9697(01)01075-0. PubMed DOI

Breivik K.; Sweetman A.; Pacyna J. M.; Jones K. C. Towards a Global Historical Emission Inventory for Selected PCB Congeners - A Mass Balance Approach: 2. Emissions. Sci. Total Environ. 2002, 290, 199–224. 10.1016/S0048-9697(01)01076-2. PubMed DOI

Schuster J. K.; Gioia R.; Breivik K.; Steinnes E.; Scheringer M.; Jones K. C. Trends in European Background Air Reflect Reductions in Primary Emissions of PCBs and PBDEs. Environ. Sci. Technol. 2010, 44, 6760–6766. 10.1021/es101009x. PubMed DOI

Grama M.; Adams F.; Siretanu L.; Cincilei A.; Bulmaga P.. Analytical Study of Obsolete Pesticides Stockpiles in the Republic of Moldova into Nato Science for Peace Project “Clean-Up Chemicals—Moldova”. Environmental Security Assessment and Management of Obsolete Pesticides in Southeast Europe; Springer, 2013; pp 381–395.

Ivanova A.; Wiberg K.; Ahrens L.; Zubcov E.; Dahlberg A.-K. Spatial Distribution of Legacy Pesticides in River Sediment from the Republic of Moldova. Chemosphere 2021, 279, 130923.10.1016/j.chemosphere.2021.130923. PubMed DOI

Romanić S. H.; Vuković G.; Klinčić D.; Antanasijević D. Self-Organizing Maps for Indications of Airborne Polychlorinated Biphenyl (PCBs) and Organochlorine Pesticide (OCPs) Dependence on Spatial and Meteorological Parameters. Sci. Total Environ. 2018, 628–629, 198–205. 10.1016/j.scitotenv.2018.02.012. PubMed DOI

Tuduri L.; Harner T.; Hung H. Polyurethane Foam (PUF) Disks Passive Air Samplers: Wind Effect on Sampling Rates. Environ. Pollut. 2006, 144, 377–383. 10.1016/j.envpol.2005.12.047. PubMed DOI

Melymuk L.; Nizzetto P. B.; Harner T.; White K. B.; Wang X.; Tominaga M. Y.; He J.; Li J.; Ma J.; Ma W.-L.; Aristizábal B. H.; Dreyer A.; Jimenéz B.; Muñoz-Arnanz J.; Odabasi M.; Dumanoglu Y.; Yaman B.; Graf C.; Sweetman A.; Klánová J. Global Intercomparison of Polyurethane Foam Passive Air Samplers Evaluating Sources of Variability in SVOC Measurements. Environ. Sci. Policy 2021, 125, 1–9. 10.1016/j.envsci.2021.08.003. PubMed DOI PMC