Atmospheric Deposition Fluxes Research Articles

Modeling global surface dust deposition using physics-informed neural networks

Paleoclimatic measurements serve to understand Earth System processes and evaluate climate model performances. However, their spatial coverage is generally sparse and unevenly distributed across the globe. Statistical interpolation methods are the prevalent techniques to grid such data, but these purely data-driven approaches sometimes produce results that are incoherent with our knowledge of the physical world. Physics-Informed Neural Networks follow an innovative approach to data analysis and physical modeling through machine learning, as they incorporate physical principles into the data-driven learning process. Here, we develop a machine-learning algorithm to reconstruct global maps of atmospheric dust surface deposition fluxes from paleoclimatic archives for the Holocene and Last Glacial Maximum periods. We design an advection-diffusion equation that prevents dust particles from flowing upwind. Our physics-informed neural network improves on kriging interpolation by allowing variable asymmetry around data points. The reconstructions display realistic dust plumes from continental sources towards ocean basins following prevailing winds.

δ26Mg, δ44Ca and 87Sr/86Sr isotope ratios constrain Mg and Ca input–output mass balances in a heavily acidified headwater catchment

A Central European catchment underlain by base-poor orthogneiss was studied using mass budgets and Mg–Ca–Sr isotope systematics. For 50 years, the catchment received large amounts of partly soluble dust from a nearby cluster of coal-burning power plants, while suffering from acid rain and severe spruce die-back. Our objective was to investigate to what extent anthropogenic dust contributes to Mg and Ca in runoff and to identify fractionations affecting Mg and Ca isotope composition of 13 ecosystem pools and fluxes. We hypothesized that if Mg and Ca runoff fluxes were significantly larger than their atmospheric inputs, Mg and Ca isotope ratios in runoff would converge to those of bedrock Mg and Ca. This relationship could be obscured by isotope fractionations. Strontium characterized by negligible isotope fractionations served as a Ca proxy. There was a strong positive correlation between Mg and Ca fluxes via spruce throughfall and catchment runoff. Monitoring of rainfall, canopy throughfall and runoff fluxes revealed a 20-, 15- and 15-fold excess of Mg, Ca and Sr in runoff, respectively, compared to atmospheric deposition fluxes. This sizeable excess per se would indicate predominance of geogenic base cations in runoff. The behavior of Mg and Ca isotopes was de-coupled. Petrographic study indicated that 92% of bedrock Mg was bound to easily dissolving biotite, 97% Ca was present in plagioclase, and nearly all Sr was in orthoclase. While Mg isotope ratios in bedrock and runoff were indistinguishable, corroborating predominantly geogenic Mg in runoff, Ca and Sr isotope ratios in bedrock and runoff were significantly different, consistent with a non-negligible contribution of atmospheric Ca and Sr to runoff. Previous study of sites underlain by felsic rocks indicated that the δ44Ca value of apatite was often higher than the δ44Ca value of plagioclase. Should weathering of apatite and/or plagioclase preferentially release Ca that is isotopically heavier than bulk rock, the geogenic Ca source at JEZ would converge to the mean δ44Ca value of runoff. Calcium isotope data would then become more consistent with a major role of geogenic Ca in JEZ runoff indicated by mass balance data.

On the use of lithogenic tracer measurements in aerosols to constrain dust deposition fluxes to the ocean southeast of Australia

Abstract. Australia contributes a significant amount of dust-borne nutrients (including iron) to the Southern Ocean, which can stimulate marine primary productivity. A quantitative assessment of the variability in dust fluxes from Australia to the surrounding ocean is therefore important for investigating the impact of atmospheric deposition on the Southern Ocean's carbon cycle. In this study, lithogenic trace metals (aluminium, iron, thorium, and titanium) contained in aerosols collected between 2016 and 2021 from kunanyi / Mount Wellington in lutruwita / Tasmania (Australia) were used to estimate dust deposition fluxes. Lithogenic fluxes were calculated using each tracer individually, as well as an average using all four tracers. This latter approach enabled an assessment of the uncertainty associated with flux calculations using only individual tracers. Elemental ratios confirmed the lithogenic nature of each tracer in aerosols when compared with both Australian soil samples and the average Earth's upper continental crust. Lithogenic flux estimates showed annual dust deposition maxima during the austral summer, following the Australian dust storm season, and annual minimum deposition flux over winter. The data provided here will help to constrain model estimates of Southern Hemisphere atmospheric deposition fluxes and their subsequent impact on global ocean biogeochemical cycles.

Seasonal variation and inhalation health risk of atmospheric polyfluoroalkyl and perfluoroalkyl substances in a metropolitan city centre of southwest China

Fifty-six total suspended particle (TSP) samples, covering four seasons from April 2022 to January 2023, were collected from the centre of Chongqing, a metropolitan city of southwest China, using an aerosol sampler. The samples were analyzed for 20 targeted poly- and per-fluoroalkyl substances (PFAS) by HPLC-MS/MS. The concentrations of PFAS ranged from 125 pg/m3 to 200 pg/m3 and were dominated by perfluorobutanoic acid (PFBA), perfluorooctanoic acid (PFOA), 2-perfluorohexyl ethanoic acid (6:2 FTCA) and perfluorooctane sulfonate (PFOS). Seasonal variations of PFAS were distinct, with the highest concentrations in winter, followed by autumn, and with lowest levels in summer. Positive matrix factorization (PMF) and a dry deposition model were used to apportion sources and to estimate the dry deposition fluxes of the 20 PFAS, respectively. PMF analysis indicated that, based on the annual average, paper packaging production (28.1%) and the degradation of precursor compounds and emissions from PFCA production (27.8%) were the two major sources, followed by electronic product manufacturing (24.0%) and textile production (20.1%), although there were significant differences in sources between seasons. The average annual dry deposition flux of PFAS was estimated to be 18.0 ng/m2/day. However, the wet deposition of PFAS was estimated to account for 82.2% of the total atmospheric deposition flux, suggesting it plays a more important role. Estimated daily intakes (EDI) and hazard quotients (HQ) were utilized to evaluate the risks to humans via exposure to PFAS through inhalation and were found to be insignificant (HQ ≪1). This study provides important information on the contamination status and exposure risk for atmospheric PFAS in a mountainous megacity, and for similar urban centers across China.

Study of seasonal variation of accident-derived atmospheric radiocesium in Koriyama City, Fukushima Prefecture, Japan during 2011-2014.

This study measured the atmospheric concentration and deposition flux of radiocesium in Koriyama City, Fukushima Prefecture, Japan, from November 2011 to October 2014. The results show synchronous seasonal change in atmospheric concentration and deposition flux of radiocesium, which is high during winter to early spring and low during summer to autumn. These seasonal variations are similar to those observed in Fukushima City but differ from those in Namie Town, Fukushima Prefecture, comprising a larger contaminated forest area. The evaluation of the relationship between atmospheric 137Cs concentration or 137Cs specific activity in atmospheric particulate matter (PM) and deposition density of 137Cs in PM source area suggest that stronger winds blowing from areas with relatively large 137Cs deposition (west of Koriyama City) toward the study site affect the site's atmospheric 137Cs concentrations.

Marine and terrestrial contributions to atmospheric deposition fluxes of methylated arsenic species

Arsenic, a toxic element from both anthropogenic and natural sources, reaches surface environments through atmospheric cycling and dry and wet deposition. Biomethylation volatilizes arsenic into the atmosphere and deposition cycles it back to the surface, affecting soil-plant systems. Chemical speciation of deposited arsenic is important for understanding further processing in soils and bioavailability. However, the range of atmospheric transport and source signature of arsenic species remain understudied. Here we report significant levels of methylated arsenic in precipitation, cloud water and aerosols collected under free tropospheric conditions at Pic du Midi Observatory (France) indicating long-range transport, which is crucial for atmospheric budgets. Through chemical analyses and moisture source diagnostics, we identify terrestrial and marine sources for distinct arsenic species. Estimated atmospheric deposition fluxes of methylated arsenic are similar to reported methylation rates in soils, highlighting atmospheric deposition as a significant, overlooked source of potentially bioavailable methylated arsenic species impacting plant uptake in soils.

Characterization of atmospheric arsenic wet deposition transport pathways and potential sources areas in the Pearl River Delta region

This study tracked the characteristics of atmospheric wet deposition of the toxic element arsenic (As) at both urban (Guangzhou (GZ)) and forested (Dinghushan Natural Reserve (DHS)) sites within the Pearl River Delta (PRD) region between 2016 and 2019, examining its correlation with rainfall patterns. Additionally, by employing backward trajectory analysis and the potential source contribution function (PSCF) in conjunction with pertinent emission inventories, we pinpointed the main pathways of atmospheric arsenic transport and evaluated the emission contributions from priority source areas. The study revealed that the atmospheric arsenic wet deposition fluxes at the GZ and DHS sites exhibited a trend of increase followed by a decrease over the four-year period. Wet season deposition fluxes were more than triple those of the dry season, with urban site showing a difference of over four times. Notably, wet season As deposition at both sites was predominantly affected by heavy rainfall from marine air masses, constituting 31% of the total deposition. The predominant trajectory directions contributing to arsenic deposition at GZ and DHS were northeast (55%) and south (53%), respectively. The primary source areas for both sites were largely outside the PRD region, with the GZ site having 80% to 95% of its source area in the non-PRD region, compared to 69% to 88% at the DHS site. Furthermore, non-PRD areas contributed approximately 65% to arsenic emissions for both sites, with the industrial sector being the dominant emission source, exceeding 97% of the total emissions.

High atmospheric dissolved organic nitrogen deposition in southeast Tibet

Nitrogen deposition has been highlighted in the last decades because it was considered as one control factor of global change. The Yarlung Tsangpo Grand Canyon acts as a major passage of monsoonal moisture transport from the Bay of Bengal into the Tibetan Plateau. However, the characteristics of nitrogen(N) deposition in this area are still unclear. Here, we established five N deposition monitoring sites and quantification the bulk N deposition fluxes from 2200 to 4600m above sea level in southeast Tibet. Results showed that the average precipitation amount of the five sites was 1127.7 mm. The dissolved organic nitrogen (DON) was the dominant species, and the deposition flux was 16.80 kg N ha−1 yr−1. The averaged NH4+-N deposition flux was 4.92 kg N ha−1 yr−1, whereas the NO3−-N deposition flux was 1.49 kg N ha−1 yr−1. In addition, the deposition fluxes of TDN, DON and NH4+-N were all significantly positive to precipitation amounts at all five sampling sites. However, the deposition flux of NO3−-N was significantly correlated with precipitation amount in the remote environment, and there was no correlation between precipitation amounts and NO3−-N deposition fluxes in human concentrated areas. TDN, DON and NH4+-N deposition were all concentrated in the plant growing season at all five sampling sites. In conclusion, the atmospheric TDN deposition flux in the Yarlung Zangbo Grand Canyon in southeast Tibet is mainly controlled by precipitation, and DON was the dominant species, followed by NH4+-N, and NO3−-N contribution was limited.

On the contribution of atmospheric reactive nitrogen deposition to nitrogen burden in a eutrophic Lake in eastern China

Although it has been demonstrated that atmospheric reactive nitrogen (i.e., Nr mainly including NH3, NH4+, NOx, NO3− and etc.) deposition has substantial impacts on nitrogen pools in remote and/or sensitive lakes, there is a scarcity of systematic evaluations regarding the impact on nitrogen burden in eutrophic lakes with riverine input as primary nitrogen source. Utilizing a regional atmospheric chemical transport model, combined with observation-based estimates of atmospheric nitrogen deposition fluxes and riverine nitrogen inputs, we investigate the contribution of atmospheric Nr deposition to the fifth largest freshwater lake located in eastern China, i.e., the Chaohu Lake which is facing frequent outbreaks of algal bloom. The results indicate that in the studied year of 2022, riverine total nitrogen (TN) input to the lake was 11553.3 t N yr−1 and atmospheric TN deposition was 2326.0 t N yr−1. For Nr species which are directly available for the biosphere supporting algae and plant growth, riverine NH4+ input was 1856.1 t N yr−1 and atmospheric NHx (NH3 and NH4+) deposition was 824.5 t N yr−1. The latter accounts for 30.8% of total NHx input to the lake. For NOy (HNO3 and NO3−), riverine NO3− input was estimated as 2621.7 t N yr−1, while atmospheric NOy deposition was 629.3 t N yr−1, accounting for 19.4%. In all, atmospheric Nr deposition accounts for 24.5 % of total Nr input to the lake. Our results suggest that even in regions with dense human activities with primary riverine N input, atmospheric deposition of Nr could also contribute significantly to the bio-available nitrogen in lake systems, and addressing eutrophication in Lake Chaohu and other eutrophic lakes will also need to consider the influence of atmospheric Nr deposition which is related to NH3 and NOx (i.e., NO + NO2, the precursor of NOy) emissions, in addition to the mitigation of riverine N input.

Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas

Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas

Phytoavailability, translocation, and accompanying isotopic fractionation of cadmium in soil and rice plants in paddy fields

Rice consumption is a major pathway for human cadmium (Cd) exposure. Understanding Cd behavior in the soil-rice system, especially under field conditions, is pivotal for controlling Cd accumulation. This study analyzed Cd concentrations and isotope compositions (δ114/110Cd) in rice plants and surface soil sampled at different times, along with urinary Cd of residents from typical Cd-contaminated paddy fields in Youxian, Hunan, China. Soil water-soluble Cd concentrations varied across sampling times, with δ114/110Cdwater lighter under drained than flooded conditions, suggesting supplementation of water-soluble Cd by isotopically lighter Cd pools, increasing Cd phytoavailability. Both water-soluble Cd and atmospheric deposition contributed to rice Cd accumulation. Water-soluble Cd’s contribution increased from 28‐52% under flooded to 58‐87% under drained conditions due to increased soil Cd phytoavailability. Atmospheric deposition’s contribution (12‐72%) increased with potential atmospheric deposition flux among sampling areas. The enrichment of heavy Cd isotopes occurred from root-stem-grain to prevent rice Cd accumulation. The different extent of enrichment of heavy isotopes in urine indicated different Cd exposure sources. These findings provide valuable insights into the speciation and phytoavailability changes of Cd in the soil-rice system and highlight the potential application of Cd isotopic fingerprinting in understanding the environmental fate of Cd.

Assessing the impact of rainfall on water quality in a coastal urban river utilizing the environmental fluid dynamics code

The Haihe River, flowing through Tianjin City, grapples with pollution challenges, notably high levels of nitrogen (N) and phosphorus (P) leading to eutrophication and unpleasant odors, particularly aggravated by rainfall. This study used Environmental Fluid Dynamics Code to comprehensively analyze the water environment under three scenarios: low flow year, normal flow year, and high flow year. The investigation delves into N and P concentrations, computes atmospheric deposition fluxes, and evaluates the loads and retention ratios of N and P in the urban river network of Tianjin City. Scenario analysis reveals distinct trends, with high flow years associated with elevated N and hydrodynamics levels, while low flow years exhibit contrasting patterns. Key findings include 1) wet deposition fluxes contributing 21% of NH4+-N and 9% of TP river loads, 2) continuous rainfall and runoff resulting in immediate or delayed increases in NH4+-N, TN, and TP concentrations in surface water, 3) an increase in average N:P mole ratios downstream along the Haihe River, and 4) N and P mean retention ratios were 48% and 63%, respectively. The study suggests that implementing sponge city construction and sustainable drainage systems may improve water quality by mitigating the direct discharge of rainfall runoff into the river.

Temporal-spatial characteristics and sources of heavy metals in bulk deposition across China

With the rapid development of industries, agriculture, and urbanization (including transportation and population growth), there has been a significant alteration in the emission and atmospheric deposition of heavy metal pollutants. This has consequently given rise to a range of ecological and environmental health issues. In this study, we conducted a comprehensive two-year investigation on the temporal and spatial distribution characteristics of heavy metals in atmospheric deposition across China based on the Nationwide Nitrogen Deposition Monitoring Network (NNDMN). The atmospheric bulk deposition of Lead (Pb), Arsenic (As), Nickel (Ni), Selenium (Se), Chromium (Cr) and Cadmium (Cd) were 6.32 ± 1.59, 4.49 ± 0.57, 1.31 ± 0.21, 1.05 ± 0.16, 0.60 ± 0.06 and 0.21 ± 0.03 mg m−2 yr−1, respectively, with a large variation among the different regions of China. The order for atmospheric deposition flux was Southwest China > Southeast China > North China > Northeast China > Qinghai-Tibet Plateau and rural area > urban area > background area. The concentrations of heavy metals in bulk deposition exhibit seasonal variation with higher levels observed during winter compared to summer and spring, which are closely associated with anthropogenic activities. The Positive Matrix Factorization (PMF) results indicated that combustion, industrial emissions and traffic are the primary contributors to atmospheric deposition of heavy metals. The single factor pollution index (Pi) of heavy metals is consistently below 1, and the composite pollution index (Ni) is 0.16 across China, indicating that atmospheric heavy metal deposition is at a pollution-free level. The comprehensive potential ecological risk index of heavy metals is 11.8, with Cd exhibiting the highest single factor potential ecological risk index at 7.09, suggesting that more attention should be paid to Cd deposition in China. The present study reveals the spatial-temporal distribution pattern of atmospheric heavy metals deposition in China, identifying regional source characteristics and providing a theoretical foundation and strategies for reducing emissions of atmospheric pollutants.

Emissions and Atmospheric Dry and Wet Deposition of Trace Metals from Natural and Anthropogenic Sources in Mainland China

Trace metals from natural and anthropogenic sources impact the atmospheric environment and enter the soil through dry and wet atmospheric deposition, ultimately affecting human health. In this study, we established an emission inventory of Pb, As, Cr, and Cd in East Asia (80° E–140° E, 15° N–50° N) for the year 2017, including dust and anthropogenic sources from both land and marine. We modified the Community Multiscale Air Quality (CMAQ) model to provide gridded data on concentrations, as well as dry and wet atmospheric deposition fluxes of metals, with a focus on mainland China. The emissions of Pb, As, Cr, and Cd in East Asia were 19,253, 3415, 3332, and 9379 tons, respectively, in 2017, with 55%, 69%, 25%, and 58% distributed in the fine mode. The spatial distribution of atmospheric concentrations and dry deposition of trace metals was similar to that of emissions, while the spatial distribution of precipitation-related wet deposition was further east and greater in the south than in the north. In mainland China, the average bulk-deposition fluxes of Pb, As, Cr, and Cd were 1036.5, 170.3, 465.9, and 185.0 μg·m−2·year−1, respectively. Our study provides gridded data on trace metals in mainland China, which can be used for assessing air quality, human exposure risks, and metal inputs to soils.

Performance evaluation of four sampling techniques and source apportionment for the atmospheric deposition fluxes of polycyclic aromatic hydrocarbons

Polycyclic aromatic hydrocarbons (PAHs) are primarily emitted into the atmosphere through anthropogenic activities and can be transported to receptor sites at varying distances. In this study, the atmospheric PAH deposition was investigated using a dry deposition plate (DDP) with Mylar, a dry deposition disk (DDD) with Velcro, a resin bulk deposition sampler (Resin-BDS), and a water bulk deposition sampler (Water-BDS) in Ulsan, South Korea, during May–October 2013. Additionally, ambient PAH concentrations were monitored using high-volume air samplers. The mean deposition fluxes of Σ13 PAHs were 8.62 ± 1.44, 36.9 ± 6.81, 56.9 ± 9.74, and 63.8 ± 8.04 μg/m2/d for the DDP, DDD, Resin-BDS, and Water-BDS, respectively. The DDD was more effective than the DDP because it could collect high molecular weight (HMW) PAHs from dry deposition, which are more toxic than low molecular weight PAHs. The Water-BDS had the highest fluxes of Σ13 PAHs; however, the Resin-BDS may be more suitable for collecting HMW PAHs from both dry and wet deposition due to relatively constant values for the deposition velocity of PAHs. Furthermore, the PAH fluxes in the Resin-BDS samples were significantly positively correlated with the gaseous and total (gaseous + particulate) concentrations of ambient PAHs. Hence, the fluxes obtained by the Resin-BDS were further used to apply principal component analysis, multiple linear regression, and backward air trajectory simultaneously to identify the emission sources of the deposited PAHs. The results indicate that the combustion of fossil fuels and biomass was the major source. In particular, the industrial complexes using petroleum and coal on the city's east coast and vehicular exhausts were the main local sources. Meanwhile, long-range sources may be forest fires, harbors, and industrial activities in nearby countries. Our study suggests that BDS, considering both dry and wet deposition, can be selectively used for research on PAH deposition.

Characteristics of Cd Fluxe in Topsoil Around Typical Mining Area in Hezhou, Guangxi

Guangxi is a typical geological high background area in southwest China, where carbonates, black rock series, basic-ultrabasic rock mass, and metal deposits (mineralized bodies) exhibit strong weathering into loam, resulting in higher cadmium (Cd) content in the soil than that in other areas of China. In order to investigate the degree of influence of mining activities on topsoil environmental quality in the area with high geological background, we chose a mining area and control area in Hezhou for this research and systematically carried out a comparative study on Cd transport routes and transport flux density in topsoil. The results showed that the average atmospheric dry and wet deposition flux densities of Cd in the soil of the mining area and control area were 1.87 g·(hm2·a)-1 and 1.52 g·(hm2·a)-1, accounting for 61.5% and 60.3% of the total input flux density, respectively. The flux density of Cd in the soil by fertilization and irrigation was lower. Surface water infiltration was the main avenue of soil Cd output in both the mining area and control area, accounting for 75.4% and 86.6% of the total output flux density, respectively. The harvest output flux density in the mining area was higher than that in the control area, and the Cd content of rice planted in the mining area was higher than the standard, whereas that of maize was safe. On the whole, the net transport flux densities of soil Cd in the mining area and control area were -3.05 g·(hm2·a)-1 and -4.05 g·(hm2·a)-1, both of which showed Cd leaching in the soil. However, the points of high atmospheric deposition flux density and exceeding Cd content in rice were mainly distributed around the mining area, which may have posed a potential threat to the health of local residents. Therefore, it is suggested to control the soil Cd pollution through monitoring and planting structure adjustment.

Modelled sources of airborne microplastics collected at a remote Southern Hemisphere site

Airborne microplastics have emerged in recent years as ubiquitous atmospheric pollutants. However, data from the Southern Hemisphere, and remote regions in particular, are sparse. Here, we report airborne microplastic deposition fluxes measured during a five-week sampling campaign at a remote site in the foothills of the Southern Alps of New Zealand. Samples were collected over 24-hour periods for the first week and for 7-day periods thereafter. On average, atmospheric microplastic (MP) deposition fluxes were six times larger during the 24-hour sampling periods (150 MP m−2 day−1) than during the 7-day sampling periods (26 MP m−2 day−1), highlighting the importance of sampling frequency and deposition collector design to limit particle resuspension. Previous studies, many of which used weekly sampling frequencies or longer, may have substantially underestimated atmospheric microplastic deposition fluxes, depending on the study design. To identify likely sources of deposited microplastics, we performed simulations with a global dispersion model coupled with an emissions inventory of airborne microplastics. Modelled deposition fluxes are in good agreement with observations, highlighting the potential for this method in tracing sources of deposited microplastics globally. Modelling indicates that sea-spray was the dominant source when microplastics underwent long-range atmospheric transport, with a small contribution from road dust.

Atmospheric deposition of dicamba herbicide can cause injury to sensitive soybean

ABSTRACT The herbicide dicamba has injured millions of hectares of sensitive plant species in the United States since 2017. This injury has coincided with the commercialization of dicamba-resistant soybean [Glycine max (L.) Merr.] and cotton (Gossypium hirsutum L.). We quantified atmospheric deposition and mass flux of dicamba in 12 soybean production regions of Missouri. Dicamba was routinely detected in weekly deposition samples collected during agriculturally-intensive spray periods. Observed concentrations were indicative of both local (<1 km) and long-distance transport (>1 km) of air-borne dicamba. High deposition events (>100 µg m-2) occurred annually in southeast Missouri, and peak dicamba deposited at these sites (12.5-84.0 µg m-2) was sufficient to injure non-dicamba resistant soybean. Adoption rate of dicamba-resistant crops and atmospheric stability explained much of the variance, and it is difficult for a herbicide product label to address these variables. Overall, these results demonstrated that dicamba was commonly deposited from the atmosphere during the growing season and observed concentrations and fluxes were strongly related to the timing and magnitude of rainfall events, and the amount of dicamba usage near collection sites.

Spatial Distribution and Migration of Heavy Metals in Dry and Windy Area Polluted by Their Production in the North China

We explored the migration and distribution of heavy metal pollution in a dry and windy area in northern China. We collected soil, atmospheric deposition, and water samples, and measured heavy metal concentrations. Cu, Zn, As, and Pb in the 0–10 cm soil layer had a fan-shaped distribution, consistent with their atmospheric deposition fluxes. This indicates that the distribution of these heavy metals was driven by strong winds. The concentration of Cd in the river increased from 0.257 mg/L upstream to 0.460 mg/L downstream, resulting in the same distribution trends as soil near the river. Surface runoff may therefore drive Cd migration. The concentration of Pb in the river exceeded the pollution threshold, resulting in accumulation in the 5–10 cm soil layer. Atmospheric deposition fluxes were consistent with the soil distribution results, and principal component analysis showed that the contribution of surface runoff was high. This suggests that the migration of Pb and Cr is driven by both wind and surface runoff. Six heavy metals showed different migration behaviors, suggesting specific control strategies should be implemented for individual heavy metals.

Gas–particle partitioning and dry deposition of atmospheric parent, alkylated, nitrated and hydroxyl polycyclic aromatic hydrocarbons over the Bohai sea and northern Yellow sea in autumn

To elucidate the gas–particle partitioning characteristics and dry deposition contributions of polycyclic aromatic hydrocarbons (PAHs) in the marine environment, 23 integrated air samples were collected during a research cruise in the northern Yellow Sea (NYS) and Bohai Sea (BS) in mid-autumn 2020. The atmospheric concentrations of 23 parent PAHs (PPAHs), 18 alkylated PAHs (APAHs), five nitrated PAHs (NPAHs), and seven hydroxyl PAHs (OPAHs) in gaseous and particulate phases were measured simultaneously. The total concentrations of 53 PAHs varied from 8.77 to 348 ng/m3. The 2-ring and 3-ring PPAHs and APAHs had lower particle-bound fractions than those of the NPAHs and OPAHs. For the gas–particle partitioning of the PAHs, the gas–particle partitioning coefficients (Kp) estimated using an octanol–air partition coefficient (KOA)–based model and KOA/soot–air partition coefficient (KSA) dual model (KOA–KSA dual model) were lower than the Kp measured in the field. Underestimation of the Kp commonly occurred with these models, but the KOA–KSA dual model was more suitable than the KOA–based model for gas–particle partitioning of the 53 atmospheric PAHs in the BS and NYS. The estimated atmospheric dry deposition fluxes of the 53 PAHs ranged from 631 to 14,345 ng/m2/day. The BS receives a PAHs load of up to 117 tons/year. The study provides background information on the occurrence and environmental fate of PAHs and could be vitally important for environmental safety management for the Northwest Pacific Ocean.