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Sci Rep ; 9(1): 953, 2019 01 30.
Artigo em Inglês | MEDLINE | ID: mdl-30700755


The profound changes in global SO2 emissions over the last decades have affected atmospheric composition on a regional and global scale with large impact on air quality, atmospheric deposition and the radiative forcing of sulfate aerosols. Reproduction of historical atmospheric pollution levels based on global aerosol models and emission changes is crucial to prove that such models are able to predict future scenarios. Here, we analyze consistency of trends in observations of sulfur components in air and precipitation from major regional networks and estimates from six different global aerosol models from 1990 until 2015. There are large interregional differences in the sulfur trends consistently captured by the models and observations, especially for North America and Europe. Europe had the largest reductions in sulfur emissions in the first part of the period while the highest reduction came later in North America and East Asia. The uncertainties in both the emissions and the representativity of the observations are larger in Asia. However, emissions from East Asia clearly increased from 2000 to 2005 followed by a decrease, while in India a steady increase over the whole period has been observed and modelled. The agreement between a bottom-up approach, which uses emissions and process-based chemical transport models, with independent observations gives an improved confidence in the understanding of the atmospheric sulfur budget.

Atmos Chem Phys ; 18(14): 10199-10218, 2018 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-30450115


The evaluation and intercomparison of air quality models is key to reducing model errors and uncertainty. The projects AQMEII3 and EURODELTA-Trends, in the framework of the Task Force on Hemispheric Transport of Air Pollutants and the Task Force on Measurements and Modelling, respectively (both task forces under the UNECE Convention on the Long Range Transport of Air Pollution, LTRAP), have brought together various regional air quality models to analyze their performance in terms of air concentrations and wet deposition, as well as to address other specific objectives. This paper jointly examines the results from both project communities by intercomparing and evaluating the deposition estimates of reduced and oxidized nitrogen (N) and sulfur (S) in Europe simulated by 14 air quality model systems for the year 2010. An accurate estimate of deposition is key to an accurate simulation of atmospheric concentrations. In addition, deposition fluxes are increasingly being used to estimate ecological impacts. It is therefore important to know by how much model results differ and how well they agree with observed values, at least when comparison with observations is possible, such as in the case of wet deposition. This study reveals a large variability between the wet deposition estimates of the models, with some performing acceptably (according to previously defined criteria) and others underestimating wet deposition rates. For dry deposition, there are also considerable differences between the model estimates. An ensemble of the models with the best performance for N wet deposition was made and used to explore the implications of N deposition in the conservation of protected European habitats. Exceedances of empirical critical loads were calculated for the most common habitats at a resolution of 100 × 100 m2 within the Natura 2000 network, and the habitats with the largest areas showing exceedances are determined. Moreover, simulations with reduced emissions in selected source areas indicated a fairly linear relationship between reductions in emissions and changes in the deposition rates of N and S. An approximate 20 % reduction in N and S deposition in Europe is found when emissions at a global scale are reduced by the same amount. European emissions are by far the main contributor to deposition in Europe, whereas the reduction in deposition due to a decrease in emissions in North America is very small and confined to the western part of the domain. Reductions in European emissions led to substantial decreases in the protected habitat areas with critical load exceedances (halving the exceeded area for certain habitats), whereas no change was found, on average, when reducing North American emissions in terms of average values per habitat.

Environ Pollut ; 217: 52-61, 2016 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-26874550


Temporal trends of Persistent Organic Pollutants (POPs) measured in Arctic air are essential in understanding long-range transport to remote regions and to evaluate the effectiveness of national and international chemical control initiatives, such as the Stockholm Convention (SC) on POPs. Long-term air monitoring of POPs is conducted under the Arctic Monitoring and Assessment Programme (AMAP) at four Arctic stations: Alert, Canada; Stórhöfði, Iceland; Zeppelin, Svalbard; and Pallas, Finland, since the 1990s using high volume air samplers. Temporal trends observed for POPs in Arctic air are summarized in this study. Most POPs listed for control under the SC, e.g. polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethanes (DDTs) and chlordanes, are declining slowly in Arctic air, reflecting the reduction of primary emissions during the last two decades and increasing importance of secondary emissions. Slow declining trends also signifies their persistence and slow degradation under the Arctic environment, such that they are still detectable after being banned for decades in many countries. Some POPs, e.g. hexachlorobenzene (HCB) and lighter PCBs, showed increasing trends at specific locations, which may be attributable to warming in the region and continued primary emissions at source. Polybrominated diphenyl ethers (PBDEs) do not decline in air at Canada's Alert station but are declining in European Arctic air, which may be due to influence of local sources at Alert and the much higher historical usage of PBDEs in North America. Arctic air samples are screened for chemicals of emerging concern to provide information regarding their environmental persistence (P) and long-range transport potential (LRTP), which are important criteria for classification as a POP under SC. The AMAP network provides consistent and comparable air monitoring data of POPs for trend development and acts as a bridge between national monitoring programs and SC's Global Monitoring Plan (GMP).

Poluentes Atmosféricos/análise , Monitoramento Ambiental , Cooperação Internacional , Regiões Árticas , Atmosfera/química , Canadá , Clordano/análise , Finlândia , Éteres Difenil Halogenados/análise , Hexaclorobenzeno/análise , Islândia , Bifenilos Policlorados/análise , Avaliação de Programas e Projetos de Saúde , Svalbard , Fatores de Tempo
Environ Pollut ; 176: 71-9, 2013 May.
Artigo em Inglês | MEDLINE | ID: mdl-23416271


High air concentrations of ammonium were detected at low and high altitude sites in Sweden, Finland and Norway during the spring 2006, coinciding with polluted air from biomass burning in eastern Europe passing over central and northern Fennoscandia. Unusually high values for throughfall deposition of ammonium were detected at one low altitude site and several high altitude sites in north Sweden. The occurrence of the high ammonium in throughfall differed between the summer months 2006, most likely related to the timing of precipitation events. The ammonia dry deposition may have contributed to unusual visible injuries on the tree vegetation in northern Fennoscandia that occurred during 2006, in combination with high ozone concentrations. It is concluded that long-range transport of ammonium from large-scale biomass burning may contribute substantially to the nitrogen load at northern latitudes.

Poluentes Atmosféricos/análise , Poluição do Ar/estatística & dados numéricos , Monitoramento Ambiental , Incineração/estatística & dados numéricos , Compostos de Amônio Quaternário/análise , Biomassa , Países Escandinavos e Nórdicos
J Environ Monit ; 11(6): 1276-83, 2009 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-19513460


A comprehensive field intercomparison at four different types of European sites (two rural, one urban and one industrial) comparing three different collectors (wet only, bulk and Bergerhoff samplers) was conducted in the framework of the European Committee for Standardization (CEN) to create an European standard for the deposition of the four elements As, Cd, Ni and Pb. The purpose was to determine whether the proposed methods lead to results within the uncertainty required by the EU's daughter directive (70%). The main conclusion is that a different sampling strategy is needed for rural and industrial sites. Thus, the conclusions on uncertainties and sample approach are presented separately for the different approaches. The wet only and bulk collector ("bulk bottle method") are comparable at wet rural sites where the total deposition arises mainly from precipitation, the expanded uncertainty when comparing these two types of sampler are below 45% for As, Cd and Pb, 67% for Ni. At industrial sites and possibly very dry rural and urban sites it is necessary to use Bergerhoff samplers or a "bulk bottle+funnel method". It is not possible to address the total deposition estimation with these methods, but they will give the lowest estimate of the total deposition. The expanded uncertainties when comparing the Bergerhoff and the bulk bottle+funnel methods are below 50% for As and Cd, and 63% for Pb. The uncertainty for Ni was not addressed since the bulk bottle+funnel method did not include a full digestion procedure which is necessary for sites with high loads of undissolved metals. The lowest estimate can however be calculated by comparing parallel Bergerhoff samplers where the expanded uncertainty for Ni was 24%. The reproducibility is comparable to the between sampler/method uncertainties. Sampling and sample preparation were proved to be the main factors in the uncertainty budget of deposition measurements.

Poluentes Atmosféricos/análise , Arsênico/análise , Monitoramento Ambiental/métodos , Metais Pesados/análise , Cádmio/análise , Cidades , Monitoramento Ambiental/instrumentação , Europa (Continente) , Humanos , Chumbo/análise , Níquel/análise , Saúde da População Rural , Estações do Ano , Saúde da População Urbana
Environ Pollut ; 154(3): 448-61, 2008 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-18336973


We analyze trends of some nitrogen compounds using long-term measurements and results from the EMEP (co-operative programme for monitoring and evaluation of the long-range transmissions of air pollutants in Europe) chemical transport model at EMEP sites. We find statistically significant declines at the majority of sites for NH(x) (sum of ammonia and ammonium) in air and for nitrate and ammonium in precipitation, but only at a few sites for xNO3 (sum of nitrate and nitric acid) in air. Model calculations and measurements give similar results. We demonstrate that the lack of trends for xNO3 in air at least partly can be attributed to a shift in the equilibrium between nitric acid and ammonium nitrate towards particulate phase, caused by reductions in the sulfur dioxide emissions.

Poluentes Atmosféricos/análise , Poluição do Ar/estatística & dados numéricos , Modelos Estatísticos , Nitrogênio/análise , Poluição do Ar/análise , Amônia/análise , Precipitação Química , Monitoramento Ambiental/métodos , Monitoramento Ambiental/estatística & dados numéricos , Europa (Continente) , Nitratos/análise , Ácido Nítrico/análise , Compostos de Amônio Quaternário/análise , Estações do Ano , Dióxido de Enxofre/análise