Volume-weighted Mean Concentrations Research Articles

Factors governing the chemical composition of rain at a regional site in South Africa

Precipitation chemistry is influenced by a number of complex processes, which include the temporal and spatial evolution of air masses. Previous wet deposition studies in South Africa could not distinctly relate the influence of air mass history on rain chemistry in order to substantiate the influence of different sources. The Welgegund atmospheric monitoring station in South Africa measures several atmospheric parameters, which include vertical profiling of the atmosphere that could assist in relating rain chemistry to air mass history. Therefore, the aim of this study was to conduct an advanced assessment on factors influencing chemical composition of rain in the South African interior by relating individual rain events at Welgegund to air mass history at cloud base height (CBH) and arrival heights below clouds, as well as supplementary in situ measurements conducted at the site. Hierarchical cluster analysis was performed through two approaches, i.e. clustering based on the chemical composition of rain, as well as grouping based on air masses arriving at CBH and 100 m above ground level (a.g.l.). Although statistical analyses highlighted the complexity associated with correlating rain chemistry to sources of chemical species, it proved useful to determine some correlations between rain chemistry and air mass history. Clustering according to the chemical composition of rain events grouped rain events from high to low volume weighted mean (VWM) concentrations. Correlation of air mass histories to these clusters indicated that higher VWM concentrations were associated with air masses at 100 m a.g.l. passing over anthropogenic source regions. Air mass history clustering grouped air masses passing predominantly over predefined source regions. The rain chemistry of clusters determined for air masses at 100 m a.g.l. arrival heights could be related to the influence of different source regions, with the impact of large point sources, the clean western background region and oceans especially evident. No significant correlations between air mass histories at CBH and ionic composition were evident. It was concluded that below-cloud atmospheric chemical composition was more significant to the chemical composition of rain in this part of South Africa. A few case studies were also conducted in order to further explore factors influencing the chemical composition of rain.

Atmospheric Deposition around the Industrial Areas of Milazzo and Priolo Gargallo (Sicily–Italy)—Part B: Trace Elements

The concentrations of trace elements in atmospheric bulk depositions (wet plus dry) were investigated from two highly industrialised areas of Sicily (southern Italy) from June 2018 to July 2019, in order to recognise the main natural and anthropogenic sources. A side objective of this study was to improve the common sampling procedures and analytical methods used for monitoring trace elements in atmospheric deposition. The trace element VWM (Volume-Weighted Mean) concentrations ranged from less than 0.01 μg L−1 for trace elements such as Cs, Tl, and U, up to 24 μg L−1 for minor elements (Al, Zn, Sr), in the filtered aliquot, while they reached concentrations up to 144 μg L−1 for the same elements, in the unfiltered aliquot. Therefore, significant differences in concentrations between these two aliquots were found, particularly for Al, Fe, Ti, Zn, Cr, Pb, Se, Cs, and U. This implies that filtering operations may produce a consistent underestimation of concentrations of certain ‘constituents’ of the atmospheric deposition. Natural (marine spray, local and regional geogenic input, volcanic emanations) and anthropogenic sources (industrial emissions, auto vehicular traffic, and diffuse background pollution) which influence rainwater chemistry were identified. Enrichment factors (EFs), with respect to the upper crust composition, provided clear evidence of the different sources above mentioned: Ti, Fe, Al, Cs, Cr, Rb, and Co have low EFs (<1), and are referable to the (local and/or regional) geogenic input, while Se, Sb, Zn, B, Cd, Cu, Mo, Sr, As, with high EFs (>10), highlight the influence of marine and/or industrial sources. The study produced a novel dataset on the atmospheric deposition rate of several trace elements, which had never been studied in the investigated areas. Finally, a comparison of trace element deposition rates in the studied areas with the atmospheric deposition reported for 53 different sites, belonging to 20 different European nations, was made. The comparison showed that some elements, such as Al, V, Zn, and Mo had higher median deposition fluxes in the Sicilian sites than in European monitoring sites.

Spatio‐temporal variability and intra‐event variation of throughfall ammonium and nitrate in a pine plantation

AbstractForest canopies are the functional interface between ecosystem and the atmospheric nitrogen (N) deposition. However, the sources of spatio‐temporal variability and intra‐event variation of N deposition via throughfall (TF) remain ambiguous. Here, we analysed TF samples for concentrations and fluxes of ammonium (NH4+) and nitrate (NO3−) using an array of 20 fixed‐position collectors on an event and within event basis throughout the 2019 growing season in a Chinese pine plantation, Northern China. Results showed that the volume weighted mean concentrations of NH4+ and NO3− in TF were significantly higher than those in bulk precipitation (BP) during the study period. A canopy budget model indicated that canopy uptake was more dominant than dry deposition for NH4+, while the reverse was true for NO3−. This caused a comparable TF NH4+ flux but an enhanced TF NO3− fluxes compared to BP. The intra‐event trend and magnitude of TF NH4+ and NO3− concentrations were influenced by the antecedent dry period and rainfall intensity, and indicated that biological nitrification may occur in the canopies. In addition, due to the larger of canopy NH4+ uptake that counteracted the amplifying effect of dry deposition, the spatial variability of TF NH4+ concentration was significantly lower than that of TF NO3− concentration, and exhibited more temporal persistence. No relationship was found between the spatial distribution of TF NH4+ concentration and the TF amount, the distance to the nearest trunk, nor the canopy cover, whereas the TF NO3− concentration was significantly related to the TF amount and the canopy cover. These findings can enhance our understanding of N processes within canopies, and have important implications for evaluating the impacts of N deposition in forest ecosystems.

Fluxes and sources of metals deposited in dew in Changchun, China

Because of the recent expansion of industrialization and urbanization, the concentration of metals in the atmosphere has significantly increased. Considering the threats of wet metal deposition to the water and soil quality, many studies have primarily focused on wet metal deposition in rain or snow, but there are few reports considering dew. As an important factor of wet deposition, dew cannot be ignored when assessing wet metal deposition. To analyze the fluxes and sources of metals deposited on Hemiptelea davidii (Hance) Planch via dew, dew samples were collected over six months in Changchun from May to October 2021, and the concentrations of 12 metals were measured. The order of both the volume-weighted mean (VWM) concentrations and fluxes of the measured metals were Ca > Na > Mg > K > Al > Fe > Zn > Pb > As > Mn > Cu > Ni. Ca was the most abundant metal, with a VWM concentration and wet flux of 6156.74 ± 1807.69 μg/L and 218.87 mg/m2·y, respectively, which were 3 orders of magnitude higher than those of Pb, As, Mn, Cu, and Ni. Based on correlation and principal component analysis, the metals in dew originated from both natural sources (Ca, Na, Mg, Al, Mn, Fe, and K) and anthropogenic activities (Cu, Ni, Pb, Zn, and As). Combined with the analysis of air mass trajectories, fire maps and microstructure characteristics of particles within dew, it was determined that the metals in dew were mainly sourced from crustal dust, straw burning, vehicle exhaust and coal combustion. Additionally, the determined metals could be attributed to a mixture of long range transport and local sources.

Investigation of the chemical nature of precipitation and source apportionment of its constituents in Tehran metropolis, Iran

Precipitation is a key process for purifying the atmosphere of pollutants. However, precipitation chemistry is also a significant environmental catastrophe on a global scale. Tehran Metropolitan Area, Iran's capital, is one of the world's most polluted cities. Nonetheless, little effort has been paid to determining the chemical composition of precipitation in this polluted metropolis. The chemical components and likely sources of trace metals and water-soluble ions in precipitation samples collected from 2021 to 2022 at an urban location in Tehran, Iran, were investigated in this study. The pH of the rainwater samples varied from 6.330 to 7.940 (mean 7.313, volume weighted mean (VWM) 7.523). The following is the order of the VWM concentration of main ions: Ca2+ > HCO3- > Na+ >SO42- > NH4+ > Cl− > NO3- > Mg2+> K+> F−. Furthermore, we discovered that VWM concentrations for trace elements are modest, with the exception of Sr (39.104 eq L−1). The primary neutralizing species for precipitation acidity were Ca2+ and NH4+. Vertical feature mask (VFM) diagrams derived from cloud-aerosol lidar and infrared pathfinder satellite observation (CALIPSO) track data indicated that polluted dust was the most common pollutant in the Tehran sky that might contribute significantly to the neutralization of precipitation. A study of species concentration ratios in seawater and the earth's crust indicated that virtually all Se, Sr, Zn, Mg2+, NO3-, and SO42- were anthropogenic. While Cl− was largely obtained from sea salt, K+ was obtained from both the earth's crust and the sea, with the earth's crust playing a larger role in K+. The earth's crust, aged sea salt, industry, and combustion processes were all verified as sources of trace metals and water-soluble ions by positive matrix factorization analysis.

Seven-year monitoring of mercury in wet precipitation and atmosphere at the Amsterdam Island GMOS station

Mercury (Hg) fate and transport research requires more effort to obtain a deep knowledge of its biogeochemical cycle, particularly in the Southern Hemisphere and Tropics that are still missing of distributed monitoring sites.Continuous monitoring of atmospheric Hg concentrations and trend worldwide is relevant for the effectiveness evaluation of the Minamata Convention on Mercury (MCM) actions. In this context, Gaseous Elemental Mercury (GEM) and total mercury (THg) in precipitations were monitored from 2013 to 2019 at the Amsterdam Island Observatory (AMS - 37°48′S, 77°34′E) to provide insights into the Hg pathway in the remote southern Indian Ocean, also considering ancillary dataset of Rn-222, CO2, CO, and CH4. GEM average concentration was 1.06 ± 0.07 ng m−3, with a slight increase during the austral winter due to both higher wind speed over the surface ocean and contributions from southern Africa. In wet depositions, THg average concentration was 2.39 ± 1.17 ng L−1, whereas the annual flux averaged 2.04 ± 0.80 μg m−2 year−1. In general, both GEM and Volume-Weighted Mean Concentration (VWMC) of THg did not show an increasing/decreasing trend over the seven-year period, suggesting a substantial lack of evolution about emission of Hg reaching AMS.Air masses Cluster Analysis and Potential Source Contribution Function showed that oceanic evasion was the main Hg contributor at AMS, while further contributions were attributable to long-range transport events from southern Africa, particularly when the occurrence of El Niño increased the frequency of wildfires.

Atmospheric wet deposition of mercury in urban Jinan, eastern China: Speciation, scavenging process and potential sources

Understanding the speciation and related influence factors of Hg in wet deposition is important to predict the fate and transport of mercury in the atmosphere. In this study, event-based samples of rainwater were collected for one year in Jinan, a northern city in eastern China. The volume-weighted mean concentration of total mercury (THg) in rainwater was 34.8 ng L−1, comparable to levels in some inland cities in China and were significantly higher than those in North America, Korea and Japan. Most of the Hg in rainwater was associated with particulates, accounted for 15.2–92.9% of THg with a mean of 66.9%, which might be attributed to the scavenging effects of high particulate-bound mercury concentrations in ambient air in urban Jinan. Dissolved mercury (DHg) accounted for 33.1% of THg, in which Hg(OH)2, HgClOH, HgCl2 and Hg(NH3)22+ are the dominant species based on the chemical equilibrium modeling simulations. THg concentrations in rainwater decreased as the rainfall amount increased owing to the dilution effect and 5 mm rainfall might be a threshold for the full wash-out capability of atmospheric Hg. For a continuous rain event, the proportion of DHg in THg could increase from 7.1% to 84.8% with the rainfall processing, especially for the species of HgClOH and HgCl2 under the influence of rainwater pH. Positive matrix factorization (PMF) analysis suggested that the major sources of Hg in rainwater were combustion emissions, marine sources, industrial emissions, as well as complexation process, which contributed to 51.4%, 24.7%, 12.2%, and 11.7% of the THg, respectively. For the specific species, the main sources varied with different Hg species, in which combustion emissions contributed one third to one half of each species sum to particulate mercury (PHg), HgClOH, HgCl2, HgBrOH and HgBrCl followed by marine sources and industrial emissions. Cluster analysis of backward trajectories revealed that polluted air masses, transported from southeast Shandong, Anhui and Jiangsu Provinces, as well as Beijing-Tianjin-Hebei region, contributed to high Hg concentration in rainwater in Jinan.

Organic Acids in Sequential Volume-Based Rainwater Samples in Shanghai: Seasonal Variations and Origins

Organic acids were investigated in the rain sequence. Samples were collected in Shanghai (East China) over a one-year period using an automatic volume-based sequential rain sampler designed by ourselves. Organic acids significantly contributed (17.8 ± 10.2%) to the acidity of rainfall events in Shanghai. We observed that the concentration of each water-soluble ion in the sequential volume-based rainwater samples did not change significantly after the cumulative rainfall reached ~1.2 mm, on average. The volume-weighted mean (VWM) concentrations of formic acid, acetic acid, and oxalic acid were 13.54 μeq L−1, 8.32 μeq L−1, and 5.85 μeq L−1, respectively. Organic acids might mostly come from fine particles, which was the reason for the differences in acid concentrations in rainfall events, cloud water, and early sequences of rainfall events. The VWM concentrations of organic acids in rainfall events, cloud water, and early sequences of rainfall events were highest in spring and lowest in winter. Further analysis, including positive matrix factorization (PMF), suggested that vehicle exhaust and secondary emission sources were dominant contributors of organic acids in rainfall events (40.5%), followed by biological emission sources (37.3%), and biomass combustion sources (18.6%). The overall results not only reveal the critical role of organic acids in cloud water and rainfall events but also indicate organic acids might pose an ecological threat to the local surface ecosystem.

A long-term overview of nitrogen in tropical rainwater and wet deposition fluxes in southern Brazil

This work reports inorganic and organic nitrogen concentrations in rainwater and estimates wet deposition fluxes in an agro-industrial region of São Paulo State (Brazil) impacted by biomass burning and vehicular public policies, spanning the period from 2005 to 2020. The overall volume weighted mean (VWM) concentration of nitrate in rainwater was 13.1 ± 0.5 μmol L−1 (n = 696). Despite decreasing vehicular emissions of NOx over the study period, there was no clear trend of nitrate concentrations in rainwater, possibly due to biomass burning emission sources. The overall ammonium VWM concentration was 24.3 ± 1.1 (n = 696). In contrast to nitrate, there was a 94% increase of ammonium in 16 years, attributed to increased emissions from vehicles and fertilizer use, together with variable biomass burning emissions. Dissolved organic nitrogen (DON) concentrations in individual samples ranged from 0.2 to 153 μmol N L−1, corresponding to between 1 and 73% of the total dissolved nitrogen, with VWM of 18.9 ± 0.9 μmol N L−1 (n = 377). Amino acids corresponded, on average, to 15% of the DON. For the majority of the years, the VWM concentrations of nitrate, ammonium, and DON were higher for the pool of samples collected during the dry season, compared to the wet season. These results highlighted the importance of biomass burning sources of reactive nitrogen in drier months, when wildfires are common. The wet deposition flux of total dissolved nitrogen was ∼12 kg N ha−1 yr−1, with ammonium corresponding to 43%, followed by DON (33%) and nitrate (23%). These results demonstrated the importance of including DON when modeling the biogeochemical cycle of nitrogen, especially in a world where wildfires may become more frequent and intense.

Wet season chemical composition of atmospheric wet deposition at Cape Point

The measurement of precipitation chemistry enables the assessment of the temporal and spatial evolution of the chemical composition of the atmosphere associated with atmospheric physical and chemical mechanisms. The aims of this study were to report the chemical composition of rainwater collected at a marine environment, i.e. the Cape Point Global Atmosphere Watch (CPT GAW) station from 2004 to 2012. As expected, the volume weighted mean (VWM) concentrations of Na+ (298.64 μEq.L-1) and Cl- (354.18 μEq.L-1) were significantly higher compared to the VWM concentrations of other ionic species, as well as compared to the VWM concentrations thereof at the sites in the South African interior. The average pH of rainwater was slightly lower than the pH of unpolluted rainwater, mainly due to NO3- associated with the occasional influence of the Cape Town metropole. In contrast to the sites situated in the north-eastern South African interior, where anthropogenic SO42- was the major constituent in rainwater, SO42- at CPT GAW was entirely associated with marine air with no anthropogenic contribution. It was also indicated that 94% of the chemical content at CPT GAW can be attributed to the marine source.

Mercury wet depositions study during plum rain, regular precipitations and near typhoon periods

This study analyzed the rainwater collected in Central Taiwan during the near typhoon period. Mercury (Hg) was analyzed and the Hg volume weighted mean concentrations (VWM) and wet depositions were calculated during the near typhoon period. In addition, the Hg wet depositions, VWM and precipitation values obtained were compared with Plum rain and regular precipitation periods. The relationship between wet Hg depositions, VWM and precipitations were also discussed. Wet Hg depositions, VWM and precipitations were also compared with the precipitation collected from other parts of the world during 2009 to 2021. The results indicated that the precipitations, VWM and wet Hg depositions in the near typhoon period were 152.5 mm, 0.82 ng/L, and 0.29 μg/m2, respectively. The Hg precipitation ratio values of this study to the plum rain and regular precipitation periods were 3.70 and 6.63, respectively. The Hg VWM ratios values of this study to the plum rain and regular precipitation periods were 12,852.56 and 1.56, respectively. Moreover, the wet Hg deposition ratios values of this study to the plum rain and regular precipitation periods (near typhoon period) were 105.97 and 9.90, respectively. The results further indicated that the Hg VWM and wet depositions obtained in the near typhoon period showed the lowest values when compared with plum rain and regular precipitations periods. Compared with Hg(p) VWM and Fw values obtained from plum season, regular precipitation, this study (typhoon period) demonstrated it has the average lowest VWM and Fw values among these three sampling periods. The correlation coefficient of precipitation and the mercury wet deposition was 0.72051 which was significant in this study. The correlation coefficient for the VWM of mercury was 0.0826 which displayed insignificant relationship in this study. Finally, when comparing the Hg VWM, wet deposition and precipitation values from various studies, the results further indicated that the near typhoon period has the lowest average Hg VWM, wet deposition and precipitation values.

Up-to-date monitoring data of wastewater and stormwater quality in Germany

A comprehensive dataset of pollutant concentrations in German urban wastewater systems is available from recently completed monitoring projects. It contains up to 1000 concentration values for each of 79 substances in wastewater treatment plant (WWTP) effluents from 49 sites, and up to 157 values for each of 95 substances in combined sewer overflows (CSOs) from 12 sites. WWTP influents and stormwater outfalls were sampled to a lesser extent. All sampling methods were harmonised and aimed at collecting event or multi-day composite samples over periods of ≥1 year. Among the substances analysed were biocides and pesticides, polycyclic aromatic hydrocarbons, perfluorinated alkyl substances, metals, pharmaceuticals, benzotriazoles, phenols, acesulfame, di-(2-ethylhexyl)phthalate, and hexabromocyclododecanes. Occurrence, concentration ranges, and removal rates of selected WWTPs are presented. CSOs can be confirmed as an important pathway of metals and PAH to receiving waters when compared to WWTPs on the basis of annual per capita loads. The derived volume-weighted site mean concentrations are qualified to be used as representative input data for estimation of average substance emissions in large areas, e.g. on river basin scale, if no site-specific data are available. As such, they will contribute to the development of strategies to reduce substance emissions, taking into account not only WWTPs but also stormwater-related discharges.

Levels and Compositions of Polycyclic Aromatic Hydrocarbons in Rainwater and Their Implication for Aquatic Environments in Urban Area in Saitama, Japan

In this study, we investigated concentrations and profiles of polycyclic aromatic hydrocarbons (PAHs) in rainwater and surface water samples collected in Saitama, an urban city located in Japan. The volume-weighted mean concentration of total PAHs in rainwater samples (dissolved + particulate) was 108.8 ng L−1 with a range of 17.6–192.9 ng L−1. Two and three benzene ring PAHs were predominantly detected, occupying 67.0% of the total concentration in rainwater samples. Individual PAH concentrations were negatively correlated with their K ow, suggesting that low-molecular-weight PAHs are preferentially scavenged owing to the higher hydrophilicity. The toxic equivalent calculated based on the relative potencies of individual PAHs showed high toxic contributions by chrysene and benz[a]anthracene in the rainwater samples. Those PAHs levels in rainwater were comparable or higher than those in adjacent river water. Correlation coefficient of PAH signatures between rainwater and surface water samples was high particularly in the dissolved phase, supporting the source/sink relationships of PAHs between wet deposition samples and receiving waters. The mean deposition flux of PAHs was 2000 ng m−2 and considered to increase with precipitation amounts.

Canopy modification of base cations deposition in a subtropical broadleaved forest: Spatial characteristics, canopy budgets and acid neutralizing capacity

Atmospheric deposition of base cations in contact with the canopy alters their chemical characteristics and plays a vital role in offsetting soil acidification and nutrient imbalance by replenishing the base cationic pool in forest ecosystems. However, the effects of site characteristics on deliveries of base cations fluxes via throughfall (TF) and stemflow (SF) across topographic gradients within a watershed remain less understood. Here, we examined the concentrations and fluxes of base cations (potassium (K+), calcium (Ca2+), magnesium (Mg2+) and sodium (Na+)), acid neutralizing capacities (ANC) and alkalinity (ALK) in bulk precipitation (BP), TF and SF in an upper slope plot (UP) and a lower slope plot (LP) in a subtropical broadleaved montane forest, Southeast China. In addition, a canopy budget model was applied to distinguish the relative contributions of dry deposition (DD) and canopy exchange (CE) to net TF + SF (NTF) flux. Results showed that annual volume weighted mean concentrations of base cations in TF and SF were significantly higher than those in BP in both UP and LP. Annual fluxes of TF or SF base cations had no significant differences between UP and LP, resulting in a comparable of the NTF fluxes. However, the relative contributions of DD and CE to NTF were different at the two slope plots. NTF K+ flux was dominated by CE regardless of slope position. Unlike K+, NTF Ca2+ and Mg2+ fluxes were dominated by DD in UP, while CE in LP. In addition, ANC and ALK of TF and SF were significantly higher compared to BP, suggesting rainwater beneath the canopy became less acidic and may mitigate in part the risk of soil acidification, especially in the dormant season. This study can provide insights into the spatial variability of chemical characteristics of base cations, and improve our understanding of the quantities and controls of external and internal nutrient inputs occurring within the canopy in forest watershed.

Atmospheric wet deposition of major ionic constituents and inorganic nitrogen in Bangladesh: Implications for spatiotemporal variation and source apportionment

The quantitative and qualitative characterization of ions and inorganic nitrogen in precipitation assists in understanding the accompanying sources and chemistry of regional precipitation. A total of 212 event-based precipitation samples were collected from four sites in Bangladesh in 2017 to investigate the physicochemical characteristics, sources, and deposition of atmospheric ionic constituents and inorganic nitrogen. During the entire monitoring period, 5.7% of the total samples were acidic (i.e., pH < 5.6), indicating that Bangladesh does not suffer severely from acid rain. The electrical conductivity (EC) and total dissolved solids (TDS) values indicate the inverse relationship between the amount of precipitation on the spatiotemporal scale. Ca2+ was the dominant neutralizing factor at four sites, which was demonstrated by the equivalent ratio of the neutralization potential to the acidifying potential and fractional acidity. Moreover, it had the highest volume-weighted mean concentration of all the sites, validating the calcareous nature of the soil aerosolized into the atmosphere. Distinct seasonality was observed for the majority of the ions with higher concentrations in the non-monsoon climate. Sea salt species displayed the pattern of Satkhira > Cox's Bazar > Dinajpur > Sylhet, whereas the anthropogenic species exhibited the order of Dinajpur > Satkhira > Sylhet > Cox's Bazar, underlining the local and regional impacts of these species in Bangladesh. Based on the source apportionment, the sources were categorized as marine (Na+ and Cl−), terrigenous (Ca2+, Mg2+, and HCO3−), fossil fuel combustion (NO3− and SO42−), agriculture (NH4+), and biomass burning (K+). The Cl− in Sylhet and Satkhira suggests additional sources associated with anthropogenic activities. The back-trajectory analyses and the National Centers for Environmental Prediction's final (NCEP FNL) datasets illustrate the presence of significantly diverse air masses with contributions from various sources in the monsoon and non-monsoon climates. Both the amount of precipitation and the ionic quantity governs the fluxes in Bangladesh. The Na+ % and SAR lie under the safe category suggesting a good precipitation water quality for agriculture and soil in Bangladesh, while the deposition of inorganic nitrogen has resulted in a value above the threshold line (10 kg ha−1 y−1). Thus, this study conveys a comprehensive picture of the ionic composition, providing a baseline dataset to assess the atmospheric environment in this lowland region.

Potential sources, scavenging processes, and source regions of mercury in the wet deposition of South Korea

In this study, the potential sources, scavenging processes, and emission regions for Hg in wet deposition were investigated in rural (Jeju), suburban (Gwangju), and urban sites (Incheon and Seoul) of South Korea. The annual volume-weighted mean concentrations of Hg in wet deposition were four to five times higher in Incheon (16.6 ng L−1) and Seoul (22.5 ng L−1) than in Jeju (4.0 ng L−1) and Gwangju (4.1 ng L−1). The variations in the Hg concentrations in wet deposition of Jeju and Gwangju were related to Cl−, Na+, Mg2+, and K+ originating from marine and crustal sources, and those in Incheon and Seoul were related to SO42−, NO3−, and NH4+ emitted from anthropogenic sources. The below-cloud scavenging was considered a major inclusion process of Hg in Jeju and Gwangju, while the within-cloud scavenging was suggested in Incheon and Seoul, based on the results of correlation analysis with Hg and major ions in wet deposition, and meteorological data. The cluster analysis of backward trajectories demonstrated that the Hg concentration in wet deposition was highest in the cluster transported from Hebei and Shandong of China in Gwangju, but in Seoul, the Hg concentrations of each cluster were comparable. This suggests that regional transport is the major source of Hg in the wet deposition of Gwangju while local transport provides substantial amount of Hg in the wet deposition of Seoul. This was further supported by the results of concentration-weighted trajectories: the most probable source region was east China for Gwangju, and the mid-west of South Korea and east China for Seoul. It is noted that the peak methylmercury concentrations were found every spring with simultaneous increases in atmospheric Al, Ca, Mg, and Fe concentrations, indicating a concurrence with Asian dust. The formation process of methylmercury in Asian dust should be confirmed in future studies.

Wet Inorganic Nitrogen Deposition at the Daheitin Reservoir in North China: Temporal Variation, Sources, and Biomass Burning Influences

Atmospheric nitrogen deposition is of great concern to both air quality and the ecosystem, particularly in northern China, which covers one-quarter of China’s cultivated land and has many heavily air polluted cities. To understand the characteristics of wet N deposition at rural sites in northern China, one-year wet deposition samples were collected in the Daheitin reservoir region. Due to the intense emissions of gaseous nitrogen compounds from heating activities during cold seasons and distinct dilution effects under different rainfall intensities and frequencies, the volume weighted mean concentrations of wet N deposition showed higher levels in dry seasons but lower levels in wet seasons. In contrast, the wet N deposition rates varied consistently with precipitation, i.e., high during the wet season and lower during the dry season. The annual wet deposition rate of total inorganic ions (the sum of NO3−–N and NH4+–N) at the rural site in North China from July 2019 to June 2020 was observed at 18.9 kg N ha−1 yr−1, still remained at a relatively high level. In addition, biomass burning activities are ubiquitous in China, especially in northern China; however, studies on its impact on wet N deposition are limited. Non-sea salt potassium ion (nss-K+) was employed as a molecular tracer to investigate the characteristics of biomass burning activities as well as their impact on the chemical properties of wet N deposition. Three precipitation events with high nss-K+ levels were captured during the harvest season (June to July). The variations in the patterns of nss-K+, deposited N species, and ratios of nss-K+ to nitrogen species as well as their relationships all indicated that biomass burning emissions contributed remarkably to NO3−–N but had a minor influence on NH4+–N.

Atmospheric wet deposition of trace elements to forest ecosystem of the Qilian Mountains, northwest China

Atmospheric deposition is the main pathway by which trace elements (TEs) enter the terrestrial ecosystems, but few studies have investigated atmospheric TE deposition in remote forests. To understand the concentration, fluxes, influencing factors, and sources of TEs in atmospheric wet deposition, 104 samples from 13 rainfall events in two forest stands of the Qilian Mountains between July and September 2018 were collected and analyzed for eight TEs. The order of volume-weighted mean (VWM) concentration of TEs was Cu > Pb > Ni > Cr > Cd > As > Hg. Cu was the most abundant TE, with VWM concentrations of 6.33–10.90 μg L−1 in Qinghai spruce (PiceacrassifoliaKom.) forest and 3.21–7.48 μg L−1 in Qilian juniper (Juniperus przewalskii Kom.) forest, which were 2 or 3 orders of magnitude higher than those of Hg, respectively. The wet deposition fluxes of TEs in Qinghai spruce forest were larger than those in Qilian juniper forest. The rainfall amount, rainfall intensity, rainfall duration, relative humidity, and wind speed were found to be important factors influencing atmospheric TE deposition. Based on correlation analysis, Principal Component Analysis (PCA) and Positive Matrix Factorization (PMF) modeling, three major sources of particulate matter (PM) were identified, namely industrial activities and waste incineration, traffic emissions and coal combustion, and biomass burning. Industrial activities and waste incineration were the dominant contributors, accounting for 79% of PM mass. Our results confirm that long-range transport of TEs has a significant impact on remote forest ecosystems in the Qilian Mountains.

Rainfall partitioning and associated nitrate and sulfate fluxes along a slope gradient in a subtropical broadleaved forest

Forest canopies create a high spatial variability of both canopy interception (Ei) and acid deposition. However, spatial characteristics of these hydrochemical fluxes along a slope gradient in forest watersheds remain unclear. Here we monitored bulk precipitation (BP), throughfall (TF), stemflow (SF), and associated nitrate (NO3−) and sulfate (SO42−) in an upper slope plot (UP) and a lower slope plot (LP) in a subtropical broadleaved forest, Southeast China. Results showed that annual rates of TF, SF and Ei to BP in UP were 85.2%, 2.6%, and 12.2%, respectively. Corresponding values in LP were 88.6%, 2.2%, and 9.2%. There were no significant differences among these rainfall partitioning components between UP and LP. Additionally, annual volume weighted mean concentrations of NO3−-N in TF and SF were significantly lower than in BP, whereas no significant differences were found for SO42−-S among BP, TF and SF. Unlike annual TF NO3−-N fluxes were similar in UP and LP, annual TF SO42−-S fluxes significantly increased along the UP to LP. Net TF + SF (NTF) fluxes were negative for NO3−-N and SO42−-S at the two slope plots, illustrating retained/uptake in the canopy. Dormant season NTF S fluxes were close to zero, indicating that dry deposition does not appear to play a major role, whereas exchange with foliage surfaces should be the dominant factor controlling the spatial patterns of TF N and S fluxes in the watershed. This study can contribute to the evaluation of watershed-scale water and acidifying input into the soil during canopy passage, and further consequent effects on forest ecosystems.

Concentration, sources and wet deposition of dissolved nitrogen and organic carbon in the Northern Indo-Gangetic Plain during monsoon

Precipitation represents an important phenomenon for carbon and nitrogen deposition. Here, the concentrations and fluxes of dissolved organic carbon (DOC) and total dissolved nitrogen (TDN) with their potential sources were analyzed in wet precipitation during summer monsoon from the Northern Indo-Gangetic Plain (IGP), important but neglected area. The volume-weighted mean (VWM) concentration of DOC and TDN were 687.04 and 1210.23 µg/L, respectively. Similarly, the VWM concentration of major ions were in a sequence of NH4+ > Ca2+ > SO42- > Na+ > K+ > NO3− > Cl− > Mg2+ > F− > NO2−, suggesting NH4+ and Ca2+ from agricultural activities and crustal dust played a vital role in precipitation chemistry. Moreover, the wet deposition flux of DOC and TDN were 9.95 and 17.06 kg/(ha⋅year), respectively. The wet deposition flux of inorganic nitrogen species such as NH4+-N and NO3−-N were 14.31 and 0.47 kg/(ha⋅year), respectively, demonstrating the strong influence of emission sources and precipitation volume. Source attribution from different analysis suggested the influence of biomass burning on DOC and anthropogenic activities (agriculture, animal husbandry) on nitrogenous species. The air-mass back trajectory analysis indicated the influence of air masses originating from the Bay of Bengal, which possibly carried marine and anthropogenic pollutants along with the biomass burning emissions to the sampling site. This study bridges the data gap in the less studied part of the northern IGP region and provides new information for policy makers to deal with pollution control.