Water-soluble main ions in precipitation over the southeastern Adriatic region: chemical composition and long-range transport

Background, aim and scope  

Precipitation samples collected from 1995 to 2000 at meteorological station in the eastern outskirts of Herceg Novi (Montenegro) were analysed on Na⁺, K⁺, Mg²⁺, Ca²⁺, Cl^–, SO₄ ^2–, NO₃ ^– and NH₄ ⁺. Four-day backward trajectory simulations were conducted during the precipitation period to investigate the regional transport of main ions and their deposition in the region of the southeastern Adriatic Sea. The air mass trajectories were classified into six trajectory categories by the origin and direction of their approach to Herceg Novi.     

Nonlinear regression and ARIMA models for precipitation chemistry in East Central Florida from 1978 to 1997

Continuous monitoring of precipitation in East Central Florida has occurred since 1978 at a sampling site located on the University of Central Florida (UCF) campus. Monthly volume-weighted average (VWA) concentration for several major analytes that are present in precipitation samples was calculated from samples collected daily. Monthly VWA concentration and wet deposition of H(+), NH(4)(+), Ca(2+), Mg(2+), NO(3)(-), Cl(-) and SO(4)(2-) were evaluated by a nonlinear regression (NLR) model that considered 10-year data (from 1978 to 1987) and 20-year data (from 1978 to 1997). Little change in the NLR parameter estimates was indicated among the 10-year and 20-year evaluations except for general decreases in the predicted trends from the 10-year to the 20-year fits. Box-Jenkins autoregressive integrated moving average (ARIMA) models with linear trend were considered as an alternative to the NLR models for these data. The NLR and ARIMA model forecasts for 1998 were compared to the actual 1998 data. For monthly VWA concentration values, the two models gave similar results. For the wet deposition values, the ARIMA models performed considerably better.     

Study of aerosol transport through precipitation chemistry over Arabian Sea during winter and summer monsoons

Precipitation samples over the Arabian Sea collected during Arabian Sea Monsoon Experiment (ARMEX) in 2002–2003 were examined for major water soluble components and acidity of aerosols during the period of winter and summer monsoon seasons. The pH of rain water was alkaline during summer monsoon and acidic during winter monsoon. Summer monsoon precipitation showed dominance of sea-salt components (∼90%) and significant amounts of non-sea salt (nss) Ca²⁺ and SO₄²⁻. Winter monsoon precipitation samples showed higher concentration of NO₃⁻ and NH₄⁺ compared to that of summer monsoon, indicating more influence of anthropogenic sources. The rain water data is interpreted in terms of long-range transport and background pollution. In summer monsoon, air masses passing over the north African and Gulf continents which may be carrying nss components are advected towards the observational location. Also, prevailing strong southwesterly winds at surface level produced sea-salt aerosols which led to high sea-salt contribution in precipitation. While in winter monsoon, it was observed that, air masses coming from Asian region towards observational location carry more pollutants like NO₃⁻and nss SO₄²⁻ that acidify the precipitation.     

Implications for long-range atmospheric transport of polycyclic aromatic hydrocarbons in Lhasa, China

The Tibetan Plateau is suggested to be an important indicator region to study the global long-range atmospheric transport of persistent organic pollutants. In this study, atmospheric polycyclic aromatic hydrocarbons (PAHs) were studied in Lhasa City in the Tibetan Plateau, China. Air samples in gas and particle phases were concurrently collected by a modified high-volume air sampler from 5 August 2008 to 13 July 2009. The concentration of ∑₁₆PAHs ranged from 18 to 160 ng?m^?3 (with a geometric mean of 68 ng?m^?3). The most abundant PAHs were phenanthrene and benzo(b)fluoranthene in gas and particle phases, respectively. Compared with other two similar studies in Beijing and Harbin, different temporal trends were found between gas and particle phases PAHs in Lhasa. The influences of meteorological parameters (ambient temperature and relative humidity) and air masses from China, India, Southeast Asia, and West Asia were the two important reasons for explaining the difference, which was confirmed by the 5-day backward trajectories. This is the first comprehensive study to provide the evidence for the different influences of long-range atmospheric transport on gas and particle phases PAHs pollution in the Tibetan Plateau.     

Sensitivity study of air trajectory long-range transport modelling

A forward trajectory model for long-term regional scale simulation of transport and deposition of sulphur from a single elevated point source is used for sensitivity tests of the deposition pattern and suspension ratio, subject to a spatial and temporal variable mixing depth, contra constant mixing depth different oxidation rates of SO₂, wet deposition rates and different source heights. The deposition is studied up to 1800 km from the source using meteorological data measured every 6 h covering Europe. For dry conditions, the inclusion of a diurnally variable mixing depth causes longer residence times of the airborne S and larger deposition far from the source. An effective wet deposition rate, however, has a tendency to suppress the change in the dry deposited mass induced by variable mixing height. A change from an oxidation rate of about 1 to 3%h⁻¹ increases both the suspension ratio and the deposition significantly at large distances from the source, while a change to a low value, 0.5 % h⁻¹ has the opposite effect. Halving the wet removal rates results in about 30% larger deposition at remote locations and 30% lower deposition occurs when the removal rates are doubled. Similar changes occur in the suspension ratio. A low source causes about 60% higher local depositions and consequently reduced suspension ratios and distant depositions of about 30%. These results support the assumption that the uncertainty in predictions of total deposition and residence times is within about ±50% when the uncertainty in the parameters considered is taken into account.     

Assessment of the environmental persistence and long-range transport of endosulfan

Concentrations of the insecticide endosulfan (α- and β-isomer) and its degradation product endosulfan sulfate in air, seawater and soil are calculated with the global environmental fate model CliMoChem. As model input, physicochemical properties of all three compounds were assembled and a latitudinally and temporally resolved emission inventory was generated. For concentrations in air, model and measurements are in good agreement; a bimodal seasonality with two peaks in spring and fall as it is observed in Arctic air is reproduced by the model. For seawater, the agreement of model and measurements depends on the values of the hydrolysis activation energy of endosulfan used in the model; with relatively high values around 100 kJ/mol, model results match field data well. The results of this assessment of the levels, persistence, and global distribution of endosulfan are also relevant for the evaluation of endosulfan as a Persistent Organic Pollutant under the Stockholm Convention.     

Stable isotopic characteristics of precipitation related to the environmental controlling factors in Ningbo,East China

Environmental Science and Pollution Research - Hydrogen and oxygen stable isotopes (δ2H and δ18O) in precipitation were analysed from June 2018 to May 2020 in Ningbo and were influenced...     

Acid rain: chemistry and transport

This review describes the more important features of the emission, chemistry, transport and deposition of pollutants involved in acid deposition. Global emissions, both natural and man-made, of sulphur and nitrogen oxides are discussed and examples of spatial distributions and trends over the last century presented. The more significant chemical and physical processes involved in the transformation of the primary emissions into their acidic end products are described, including a summary of the approximate timescales of the processes involved. Measurements and modelled calculations of spatial and temporal patterns in the deposition of acidic pollutants by both wet and dry pathways are presented.     

Analysis of observations relevant to long-range transport and deposition of pollutants

Observations of annual wet deposition of sulfur made during 1980 at 62 stations in northeastern America are interpreted using a statistical long-range transport model. This work is meant to demonstrate the role of an empirical model in the analysis of observations. Our analysis points to the following conclusions:

• 1.(1) The parameters that represent the conversion of SO₂ to SO₄ and the wet and dry removal of sulfur are insensitive to concentration levels,
• 2.(2) the variation of the wet deposition field is closely related to the distribution of sulfur emissions and
• 3.(3) observations demand efficient wet scavenging of SO₂.

     

Chemical characteristics of long-range transport aerosol at background sites in Korea

In this study, background concentration sites of Deokjeok and Gosan, which were deemed suitable for monitoring the impact of long-range transported air pollutants, were selected. An investigation of the source types of pollutants, their locations, and relative quantitative contributions to the particulate concentrations at both sites using appropriate methodologies to make initial estimations was conducted. Episodic measurements of PM_2.5, PM₁₀, and size distribution, along with its ion and carbon components were performed from 2005 to 2007, and a comprehensive analysis of the results was conducted utilizing back trajectory analysis. As for frequency of wind direction, it was quite apparent that the two sites are heavily influenced by air masses originating from the eastern and northern regions of China. For PM_2.5 and PM₁₀, the mass concentrations from north and east China were higher than other cases, originating from the ocean. In the northerly-wind case, meteorological properties for Deokjeok and Gosan and the influence of carbon emissions from northwest Korea resulted in a changing of air mass properties during transport. As was the case with mass concentration, the highest contribution for ionic and carbon components of PM_2.5 and PM₁₀ for both sites appeared for the westerly wind case. A specially high relative contribution, greater than 1.4 times, was apparent in the secondary aerosol case because of a large influence of long-range transported pollutants from east China. Carbon components exhibited different behaviors for the northerly and westerly wind cases compared with secondary aerosol. The major reason for this discrepancy appears to be the carbon emissions from northwest Korea.     

Mesoscale influence on long-range transport — evidence from ETEX modelling and observations

During the first European Tracer Experiment (ETEX) tracer gas was released from a site in Brittany, France, and subsequently observed over a range of 2000 km. Hourly measurements were taken at the National Environmental Research Institute (NERI) located at Risø, Denmark, using two measurement techniques. At this location, the observed concentration time series shows a double-peak structure occurring between two and three days after the release. By using the Danish Emergency Response Model of the Atmosphere (DERMA), which is developed at the Danish Meteorological Institute (DMI), simulations of the dispersion of the tracer gas have been performed. Using numerical weather-prediction data from the European Centre for Medium-Range Weather Forecast (ECMWF) by DERMA, the arrival time of the tracer is quite well predicted, so also is the duration of the passage of the plume, but the double-peak structure is not reproduced. However, using higher-resolution data from the DMI version of the HIgh Resolution Limited Area Model (DMI-HIRLAM), DERMA reproduces the observed structure very well. The double-peak structure is caused by the influence of a mesoscale anti-cyclonic eddy on the tracer gas plume about one day earlier.     

Total gaseous concentrations in mercury in Seoul, Korea: Local sources compared to long-range transport from China and Japan

Total gaseous mercury (TGM) and carbon monoxide (CO) were measured every 5 min and hourly, respectively, in Seoul, Korea, from February 2005 through December 2006. The mean concentrations of TGM and CO were 3.44 ± 2.13 ng m⁻³ and 613 ± 323 ppbv, respectively. TGM and CO concentrations were highest during the winter and lowest during the summer. In total, 154 high TGM concentration events were identified: 86 were classified as long-range transport events and 68 were classified as local events. The TGM and CO concentrations were well correlated during all long-range transport events and were weakly correlated during local events. Five-day backward trajectory analysis for long-range transport events showed four potential source regions: China (79%), Japan (13%), the Yellow Sea (6%), and Russia (2%). Our results suggest that measured ΔTGM/ΔCO can be used to identify long-range transported mercury and to estimate mercury emissions from long-range transport.     

Assessment of long-range transport potential of polychlorinated Naphthalenes based on three-dimensional QSAR models

Environmental Science and Pollution Research - Experimentally determined octanol–air partition coefficients (K OA) for 43 polychlorinated naphthalene (PCN) congeners and experimentally...     

Estimating contribution of precipitation scavenging of atmospheric particulate mercury to mercury wet deposition in Japan

Mercury wet deposition is dependent on both the scavenging of divalent reactive gaseous mercury (RGM) and atmospheric particulate mercury (Hg(p)) by precipitation. Estimating the contribution of precipitation scavenging of RGM and Hg(p) is important for better understanding the causes of the regional and seasonal variations in mercury wet deposition. In this study, the contribution of Hg(p) scavenging was estimated on the basis of the scavenging ratios of other trace elements (i.e., Cd, Cu, Mn, Ni, Pb and V) existing entirely in particulate form. Their wet deposition fluxes and concentrations in air, which were measured concurrently from April 2004 to March 2005 at 10 sites in Japan, were used in this estimation. The monthly wet deposition flux of mercury at each site correlated with the amount of monthly precipitation, whereas the Hg(p) concentrations in air tended to decrease during summer. There was a significant correlation (P<0.001) among the calculated monthly average scavenging ratios of trace elements, and the values in each month at each site were similar. Therefore, it is assumed the monthly scavenging ratio of Hg(p) is equivalent to the mean value of other trace elements. Using this scavenging ratio (W), the wet deposition flux (F) due to Hg(p) scavenging in each month was calculated by F=WKP, where K and P are the Hg(p) concentration and amount of precipitation, respectively. Relatively large fluxes due to Hg(p) scavenging were observed at a highly industrial site and at sites on the Japan Sea coast, which are strongly affected by the local sources and the long-range transport from the Asian continent, respectively. However, on average, at the 10 sites, the contribution of Hg(p) scavenging to the annual mercury deposition flux was 26%, suggesting that mercury wet deposition in Japan is dominated by RGM scavenging. This RGM should originate mainly from the in situ oxidation of Hg⁰ in the atmosphere.     

Analysis of cloud and precipitation chemistry at Whiteface Mountain,NY

Federal and state programs over the past two decades have resulted in the reduction of emissions of precursors of acid rain. Concomitant with these changes, measured concentrations of acidity in precipitation and in watersheds have shown a downward trend or improvement. However, another pathway for these precursors is through cloud and fog events that often tend to occur at high-elevation regions affecting the fauna and flora as well. In this study we report on long-term measurements of cloud water and precipitation chemistry made from 1994 onwards at a high-elevation location, Whiteface Mountain NY, in the northeastern United States. Trends and inter-relationship between the ions were examined along with ambient SO₂ measurements and Adirondack lakes chemistry data.     

Sulfate in precipitation as observed by the European atmospheric chemistry network

The temporal variation in sulfur concentration/deposition involves long term fluctuations which show striking similarities within certain areas but are different between areas in different positions relative to major sulfur emission areas in Europe. As an example, the deposition has been constant or decreasing during the last ten years in most of the area covered by the network, indicating that an increasing amount of the sulfur emitted in Europe is transported and deposited elsewhere, possibly in an eastward direction.The seasonal variation in deposition resembles that for amount of precipitation and shows a maximum during the summer or autumn for most areas. The concentration shows a maximum in the spring and a minimum in the autumn at most stations.The concentration field has a maximum approximately over Belgium and Holland with decreasing concentrations towards SW to NE (over W) but with comparatively high levels extending up over Finland. (Areas to the east and south are not covered by the network.)The deposition field was, based on a brief discussion of the relation between concentration and amount of precipitation, obtained as the product of these latter fields. High deposition rates are found in the south of Norway and in the middle of Britain in addition to the areas with high concentration.Sulfur and hydrogen ion are the dominating ions in precipitation followed by ammonium and nitrate except in coastal areas and in places where the soil is bare.Sources of errors in the data base are discussed and the results from a large number of additional sampling sites around and between the regular network sampling sites are most helpful in this regard. These latter measurements also permit an estimate of the uncertainty in areal concentration averages which are due to local and mesoscale variability.Finally, past and future importance of continuous measurements (as in the EACN) is discussed briefly.     

Analysis of long-range transport influences on urban PM10 using two-stage atmospheric trajectory clusters

There is evidence that long-range transport of natural and/or anthropogenic particles can have a negative impact on urban air quality. Certain European cities may fail to comply with the currently implemented 24-h PM₁₀ limit value due to the additional impact of remote sources of particles, which are not controllable at local level. For that reason, reliable methodologies identifying long-range transport patterns and quantifying their contribution to urban PM₁₀ levels are required. In this study, a two-stage clustering methodology was developed and applied to back trajectories arriving in three European cities: Athens, Madrid and Birmingham, which experience large, moderate and small numbers of daily PM₁₀ episodes, respectively. The atmospheric trajectories used in this analysis were computed with HYSPLIT model (NOAA) for a 3-year period. The two-stage cluster analysis has the advantage of providing highly disaggregated trajectory clusters, which proved to correspond to significantly different PM₁₀ levels. In the case of Madrid and Birmingham, clusters of trajectories originating from North Africa and continental Europe, respectively, were strongly associated with the highest PM₁₀ levels recorded in selected monitoring stations. In Athens, long-range transport patterns and trans-boundary influences were less evident, which highlighted the more substantial impact of local emission sources. Finally, two simple statistical indexes were proposed for assessing PM₁₀ episodes associated with different clusters of trajectories. This study has established a practical methodology for examining the impact of long-range atmospheric transport on local air quality, without resorting to high resource-demanding source apportionment techniques.     

Acid neutralization of precipitation in Northern China

There is an increasing concern over the impact of human-related emissions on the acid precipitation in China. However, few measurements have been conducted so far to clarify the acid-neutralization of precipitation on a regional scale. Under a network of 10 sites across Northern China operated during a 3-year period from December 2007 to November 2010, a total of 1118 rain and snow samples were collected. Of this total, 28% was acid precipitation with pH < 5.6. Out of these acid samples, 53% were found heavily acidic with pH value below 5.0, indicating significantly high levels of acidification of precipitation. Most of the acidity of precipitation was caused by H2SO4 and HNO3, their relative contribution being 72% and 28%, respectively. However; the contribution of HNO3 to precipitation acidity will be enhanced due to the increasing NO(x) and stable SO2 emissions in future. Neutralization factors for K+, NH4+, Ca2+, Na+, and Mg2+ were estimated as 0.06, 0.71, 0.72, 0.15, and 0.13, respectively. The application of multiple regression analysis further quantified higher NH4+ and Ca2+ contribution to the neutralization process, but the dominant neutralizing agent varied from site to site. The neutralization was less pronounced in the rural than urban areas, probably due to different levels of alkaline species, which strongly buffered the acidity. Presence of high concentrations of basic ions was mainly responsible for high pH of precipitation with annual volume-weighted mean (VWM) values larger than 5.6 at several sites. It was estimated that in the absence of buffering ions, for the given concentration of SO4(2-) and NO3-, the annual VWM pH of precipitation would have been recorded around 3.5 across Northern China. This feature suggested that emissions of particles and gaseous NH3 played very important role in controlling the spatial variations of pH of precipitation in the target areas.