Elsevier

Atmospheric Environment

Volume 99, December 2014, Pages 474-484
Atmospheric Environment

Levels, trends and health concerns of atmospheric PAHs in Europe

https://doi.org/10.1016/j.atmosenv.2014.10.011Get rights and content

Highlights

  • Atmospheric PAHs generally have higher levels in the Central/Baltic areas.

  • Marked seasonality of PAH concentration, with winter highs and summer lows.

  • Downward temporal trends are perceived as we approach the higher latitudes.

  • Air quality guidelines for BaP have been surpassed in several areas in the last years.

Abstract

Changes in climate can affect the concentration patterns of polycyclic aromatic hydrocarbons (PAHs) by altering the dispersion (wind speed, mixing layer height, convective fronts), deposition by precipitation, dry deposition, photochemistry, natural emissions and background concentrations. This means the evolution trends of these pollutants have to be studied under a multi-scale perspective, allowing the establishment of transport patterns and distribution of PAHs. In this sense, this work tries to unveil the atmospheric behaviour of these pollutants using temporal data series collected in different stations from the European Monitoring and Evaluation Programme (EMEP) air sampling network. These sites are thought to avoid the direct influence of emitting areas (background stations), allowing the study of long-range transport effects, intra- and trans-annual variability, relationships between concentrations patterns and meteorological variables and latitudinal gradients of PAH levels in Europe. Overall, a typical high concentration pattern was found for the colder months (and an opposite behaviour is found for summertime). Negative trends were detected over high latitudes, for instance, in Svalbard (Norway), whereas for the United Kingdom the pattern is the inverse. Also, negative latitudinal gradients were observed in 4 of the 15 PAHs studied. Finally, air quality parameters revealed concern over human health issues, given the recent increase of BaP levels in Europe.

Introduction

As a result of the industrial development occurred in Europe during the last century, environmental pollution levels have been increasing exponentially. For example, the use of fossil fuels such as coal and petroleum generated increases in the emission of different pollutants into the atmosphere, such as nitrogen oxides, sulphur dioxide, carbon monoxide or organic compounds of different volatilities. The latter group includes the polycyclic aromatic hydrocarbons (PAHs), produced by natural and anthropogenic sources (Srogi, 2007), that can be found not only in the atmosphere associated with the gas or the particulate phase (Kiss et al., 2001, Lammel et al., 2009), but also in other environmental matrices like soil, sediment or vegetation (Wild and Jones, 1995, Chen et al., 2004, Navarro-Ortega et al., 2012). These compounds are widely studied due to their carcinogenic and mutagenic properties. Their high lipid solubility makes them prone to absorption in the lung tissue, skin, breasts or intestines, carrying risks to the human health (Maron and Ames, 1982, Howard et al., 1995, Kim et al., 2013).

However, existing literature on PAHs report that their atmospheric content is reduced comparing to the other environmental matrices. Maliszewska-Kordybach (1999) mentioned an overall presence of only 0.5%, while Wild and Jones (1995) found that the airborne PAHs in the British territory represent only 4% of total anthropogenic emissions in a year. This is evidence that the atmosphere is not a repository for these compounds but rather a pathway for their transport, dilution and transformation (Wild and Jones, 1995).

An important aspect in that in most studies, the areas covered are small (form cities to 50 km wide regions), tendency profiles are often missing and the temporal trends use datasets of less that 10 years (Dimashki et al., 2001, Prevedouros et al., 2004). For instance, Hwang and Wade (2008) and Amador-Muñoz et al. (2013) had time series of 4 and 2 years to obtain the PAHs levels in specific locations of the USA and Mexico, respectively. Hwang and Wade (2008) used pine needles as biomonitors of the airborne PAHs. Also, no detailed analysis was found integrating the entire European continent, essential to assess trans-boundary pollution, except for the information yielded by the EMEP network, a programme which derives from the Geneva Convention of 1977 on transboundary pollution (http://www.emep.int). However, even the EMEP network in its 2012 report on particulate matter applying temporal series, relies on time-frames of less than 10 years and only distinguishes between PM2.5 and PM10, despite having information on individual contaminants (Torseth et al., 2012).

Fuelled by the relatively small amount of related literature (considering the existing databases on atmospheric PAHs), four main objectives are intended for the current study: to conduct a comparative analysis of the concentration of 15 PAHs in the atmosphere throughout the European continent, characterising the temporal variability of the series, including intra-annual patterns, using the Mann–Kendall test to determine statistical significance; to establish correlations with meteorological parameters, in order to explain the influence of climate on the variability of PAH levels, with significance calculated by the Pearson test; to determine possible latitudinal gradients of concentration for each PAH under study; and finally to evaluate if the PAH incidence in the time series considered poses problems concerning human health quality guidelines. With these objectives it is also an aim to estimate the influence of atmospheric transport from the source to remote areas in Europe.

Section snippets

Target pollutants

The study will focus on the dataset available from the EMEP network concerning 15 of the 16 EPA (Environmental Protection Agency) PAHs: acenaphthylene (Acy), acenaphthene (Ace), fluorene (Fluo), phenanthrene (Phen), anthracene (Ant), fluoranthene (Flt), pyrene (Pyr), benzo[a]anthracene (BaA), chrysene (Chry), benzo[b]fluoranthene (BbF), benzo[k]fluoranthene (BkF), benzo[a]pyrene (BaP), indeno[1,2,3-cd]pyrene (IcdP), dibenzo[a,h]anthracene (DahA) and benzo[ghi]perylene (BghiP). Naphthalene was

Results and discussion

As indicated in Table 1, the longer time data series are located in Norway (Svalbard Island), Sweden (Aspvreten), Finland (Pallas) and Czech Republic (Kosetice). Naturally, these are the series where the results supposedly have the highest statistical weight, although it is possible that they contain anomalous years or an intensified effect of statistical noise. In a similar way, there are also individual PAHs with more data available than others (with BaP on top of the list). Taking these

Human health guidelines

Legislation or guidelines for the presence of PAHs in the atmosphere are very scarce. Due to its proven carcinogenic properties, BaP has been taken as a reference to set some legal or reference limits, as the hazardous effects of this chemical can affect human health in a widespread range of ways (Gallo et al., 2008, Kim et al., 2013). According to the EEA, BaP emissions in the EU increased by 11% between 2002 and 2011, linked with a 24% rise in emissions from fuel consumption associated to

Conclusions

After this study, it can be said that the regions with the highest individual concentrations of PAHs within the considered domain are central Europe and the Baltic Sea areas. This reflects a significant presence of local concentration sources. The Finnish and Norwegian stations (located in higher latitudes) are recurrently those with lower levels, particularly Svalbard, where almost all the presence of PAHs is due to the long distance atmospheric transport. Seasonal trends are relatively

Acknowledgements

This work has been partially funded by the European Union Seventh Framework Programme-Marie Curie COFUND (FP7/2007-2013) under UMU Incoming Mobility Programme ACTion (U-IMPACT) Grant Agreement 267143. The Spanish Ministry of Economy and Competitiveness and the “Fondo Europeo de Desarrollo Regional” (FEDER) (project CORWES CGL2010-22158-C02-02) are acknowledged for their partial funded. Dr. Pedro Jiménez-Guerrero acknowledges the Ramón y Cajal programme.

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