Understanding the role of atmospheric deposition on the environmental load of per- and polyfluoroalkyl substances: A case study in Three Gorges Reservoir, China.

Sixty-nine total suspended particle (TSP) samples, paired with forty-eight surface soil samples, covering four seasons from January 2021 to November 2021, were collected from the Three Gorges Reservoir Region (TGRR). Twenty per- and poly-fluoroalkyl substances (PFASs) were analyzed to evaluate their contamination characteristics and understand the role of atmospheric deposition on the environmental loads in TGRR. The annual average concentrations of PFASs in TSP and soil were 37.2 ± 1.22 pg·m-3 and 0.798 ± 0.134 ng·g-1, respectively. For TSP, concentrations were highest in spring and lowest in summer. For soil, it was in autumn and winter, respectively. The seasonality was more influenced by anthropogenic activities than by meteorological conditions or physicochemical parameters of the soil. Positive matrix fractionation (PMF) indicated that, based on annual averages, PFOA-based products (40.2 %) were the major sources of PFASs in TSP, followed by PFOS-based products (25.2 %) and precursor degradation (34.6 %). The highest source contributor for PFASs in spring was precursor degradation (40.9 %), while in other three seasons, it was PFOA-based products (39.9 %, 40.9 % and 52.0 %, respectively). The mean atmospheric dry and wet deposition fluxes of PFASs were estimated at 4.38 ng·m-2·day-1 and 23.5 ng·m-2·day-1, respectively. The contribution of atmospheric deposition to the inventory mass of PFASs in the surface soil was 22.3 %. These findings fill a gap in knowledge regarding the processes and mechanisms of the occurrence, sources and atmospheric deposition of PFASs in the TGRR.

Air-plant interaction and air-soil exchange of polycyclic aromatic hydrocarbons in a large human-influenced reservoir in southwest China.

The Three Gorges Reservoir (TGR) is totally manmade, strongly influenced by anthropogenic activity, and lies on the upper reaches of Yangtze River. The periodic storage and discharge of water from the Three Gorges Dam could have altered the original air-plant/soil interactions of contaminants in TGR. Herein, paired atmospheric gas-particle, air-plant, and air-soil samples were collected to investigate the air-plant interaction and air-soil exchange of 16 USEPA priority polycyclic aromatic hydrocarbons (PAHs). The air-plant interaction based on McLachlan's framework to our datasets suggests that PAHs were absorbed via gaseous deposition that was restricted by the plant-gas dynamic equilibrium. The equilibrium indicates a dynamic balance between the gaseous phase and plant surface in PAH absorption. The main limiting factor influencing the PAH uptake was the plant species rather than the atmospheric PAH concentration. The air-soil exchange of PAHs exhibited a net volatilization flux of 16.71 ng/m2/d from the soil to the air based on annual average. There was more volatilization and less deposition in summer and more deposition and less volatilization in autumn and winter. The soil serves as a secondary source of atmospheric PAHs. As the first attempt on probing the multi-interface geochemical process of PAHs, this study highlights the influence of manual water level manipulation from the TGD and environmental factors (such as temperature, humidity, and soil properties) on the regional fate of PAHs in the TGR.

Probing the occurrence, sources and cancer risk assessment of polycyclic aromatic hydrocarbons in PM2.5 in a humid metropolitan city in China.

Fifty-two consecutive PM2.5 samples from December 2021 to February 2022 (the whole winter) were collected in the center of Chongqing, a humid metropolitan city in China. These samples were analysed for the 16 USEPA priority polycyclic aromatic hydrocarbons (16 PAHs) to explore their composition and sources, and to assess their cancer risks to humans. The total concentrations of the 16 PAHs (ng m-3) ranged from 16.45 to 174.15, with an average of 59.35 ± 21.45. Positive matrix factorization (PMF) indicated that traffic emissions were the major source (42.4%), followed by coal combustion/industrial emission (31.3%) and petroleum leakage/evaporation (26.3%). The contribution from traffic emission to the 16 PAHs increased from 40.0% in the non-episode days to as high as 46.2% in the air quality episode during the sampling period. The population attributable fraction (PAF) indicates that when the unit relative risk (URR) is 4.49, the number of lung cancer cases per million individuals under PAH exposure is 27 for adults and 38 for seniors, respectively. It was 5 for adults and 7 for seniors, when the URR is 1.3. The average incremental lifetime cancer risk (ILCR) for children, adolescents, adults and seniors was 0.25 × 10-6, 0.23 × 10-6, 0.71 × 10-6, and 1.26 × 10-6, respectively. The results of these two models complemented each other well, and both implied acceptable PAH exposure levels. Individual genetic susceptibility and exposure time were identified as the most sensitive parameters. The selection and use of parameters in risk assessment should be further deepened in subsequent studies to enhance the reliability of the assessment results.

Microplastic burden in invasive signal crayfish (Pacifastacus leniusculus) increases along a stream urbanization gradient.

Microplastics are a globally pervasive pollutant with the potential to directly impact species and accumulate in ecosystems. However, there remains a relative paucity of research addressing their accumulation in freshwater ecosystems and a near absence of work in crayfish, despite their high ecological and economic importance. This study investigated the presence of microplastics in the invasive signal crayfish Pacifastacus leniusculus along a stream urbanization gradient. The results demonstrate a ubiquitous presence of microplastics in crayfish digestive tracts at all sites and provide the first evidence of microplastic accumulation in tail tissue. Evidence of a positive linear trend was demonstrated between microplastic concentration in crayfish and upstream urban area size in generalized linear models. Evidence for a positive effect of the upstream urban area and a negative effect of crayfish length on microplastic concentrations in crayfish was demonstrated in multiple generalized linear regression models. Our results extend the current understanding of microplastics presence in freshwater ecosystems and demonstrate their presence in crayfish in the wild for the first time.

The varved succession of Crawford Lake, Milton, Ontario, Canada as a candidate Global boundary Stratotype Section and Point for the Anthropocene series.

An annually laminated succession in Crawford Lake, Ontario, Canada is proposed for the Global boundary Stratotype Section and Point (GSSP) to define the Anthropocene as a series/epoch with a base dated at 1950 CE. Varve couplets of organic matter capped by calcite precipitated each summer in alkaline surface waters reflect environmental change at global to local scales. Spheroidal carbonaceous particles and nitrogen isotopes record an increase in fossil fuel combustion in the early 1950s, coinciding with early fallout from nuclear and thermonuclear testing - 239+240Pu and 14C:12C, the latter more than compensating for the effects of old carbon in this dolomitic basin. Rapid industrial expansion in the North American Great Lakes region led to enhanced leaching of terrigenous elements by acid precipitation during the Great Acceleration, and calcite precipitation was reduced, producing thin calcite laminae around the GSSP that is marked by a sharp decline in elm pollen (Dutch Elm disease). The lack of bioturbation in well-oxygenated bottom waters, supported by the absence of fossil pigments from obligately anaerobic purple sulfur bacteria, is attributed to elevated salinities and high alkalinity below the chemocline. This aerobic depositional environment, highly unusual in a meromictic lake, inhibits the mobilization of Pu, the proposed primary stratigraphic guide for the Anthropocene.

The Searsville Lake Site (California, USA) as a candidate Global boundary Stratotype Section and Point for the Anthropocene series.

Cores from Searsville Lake within Stanford University's Jasper Ridge Biological Preserve, California, USA, are examined to identify a potential GSSP for the Anthropocene: core JRBP2018-VC01B (944.5 cm-long) and tightly correlated JRBP2018-VC01A (852.5 cm-long). Spanning from 1900 CE ± 3 years to 2018 CE, a secure chronology resolved to the sub-annual level allows detailed exploration of the Holocene-Anthropocene transition. We identify the primary GSSP marker as first appearance of 239,240Pu (372-374 cm) in JRBP2018-VC01B and designate the GSSP depth as the distinct boundary between wet and dry season at 366 cm (6 cm above the first sample containing 239,240Pu) and corresponding to October-December 1948 CE. This is consistent with a lag of 1-2 years between ejection of 239,240Pu into the atmosphere and deposition. Auxiliary markers include: first appearance of 137Cs in 1958; late 20th-century decreases in δ15N; late 20th-century elevation in SCPs, Hg, Pb, and other heavy metals; and changes in abundance and presence of ostracod, algae, rotifer and protozoan microfossils. Fossil pollen document anthropogenic landscape changes related to logging and agriculture. As part of a major university, the Searsville site has long been used for research and education, serves users locally to internationally, and is protected yet accessible for future studies and communication about the Anthropocene. Plain Word Summary: The Global boundary Stratotype Section and Point (GSSP) for the proposed Anthropocene Series/Epoch is suggested to lie in sediments accumulated over the last ~120 years in Searsville Lake, Woodside, California, USA. The site fulfills all of the ideal criteria for defining and placing a GSSP. In addition, the Searsville site is particularly appropriate to mark the onset of the Anthropocene, because it was anthropogenic activities-the damming of a watershed-that created a geologic record that now preserves the very signals that can be used to recognize the Anthropocene worldwide.

Earthquake, floods and changing land use history: A 200-year overview of environmental changes in Selenga River basin as indicated by n-alkanes and related proxies in sediments from shallow lakes.

The Selenga River basin, located in southern Siberia, is an important component of the Lake Baikal ecosystem, and comprises approximately 80 % of the Baikal watershed. Within the Selenga River basin, two localized study regions were chosen. The first, the Selenga Delta, is one of the largest inland freshwater floodplains in the world and plays an important role in the ecosystem functioning of Baikal. It purifies the river waters before they enter the lake and acts as a refuge for many of Baikal's endemic species. The second location, the Gusinoozersk region, is southwest of Lake Baikal and the Selenga Delta, and was chosen as a more heavily industrialized region within the Selenga River basin. Anthropogenic activities, including industry, urban settlements, aquaculture and agriculture, have historically increased ecological damage within this area. We assessed possible drivers of changes in sedimentary organic matter (OM) composition within two shallow lakes (SLNG04 and Black Lake), located in the Selenga Delta and the Selenga watershed, respectively. We focused on individual n-alkanes, one of the most abundant and common lipids used to provide information on past vegetation and used multivariate statistics to disentangle changes in the sources of sedimentary OM over time. The depositional OM history of SLNG04B core can be divided in four zones: (i) major influence of non-emergent vascular plants, typically found in transitional environments (ca. 1835 to ca. 1875); (ii) increased influence of grasses/herbs (ca. 1880 to ca. 1910); (iii) transition from non-emergent vascular plants and grasses/herbs to submerged and floating macrophytes and phytoplankton (ca. 1915 to ca. 1945); (iv) maintenance of autochthonous OM from submerged and floating macrophytes and phytoplankton (ca. 1945 to ca. 2014). The depositional OM history of the Black Lake core can be divided in two main zones: (i) major influence of non-emergent vascular plants and submerged and floating macrophytes (ca. 1915 to ca. 1980); (ii) increased influence of grasses/herbs and phytoplankton (ca. 1980 to ca. 2010). Natural events (e.g., an earthquake in 1862 caused flooding and subsidence of much of the land surrounding SLNG04 lake and a further catastrophic flood event in 1897) and anthropogenic activities (e.g., nutrient pollution from expansion of agricultural and livestock population) changed the composition of sedimentary OM resulting in ecological shifts across trophic levels in the Selenga River basin.

Mercury Pollution History in Tropical and Subtropical American Lakes: Multiple Impacts and the Possible Relationship with Climate Change.

Sediment cores obtained from 11 tropical and subtropical American lakes revealed that local human activities significantly increased mercury (Hg) inputs and pollution levels. Remote lakes also have been contaminated by anthropogenic Hg through atmospheric depositions. Long-term sediment-core profiles revealed an approximately 3-fold increase in Hg fluxes to sediments from c. 1850 to 2000. Generalized additive models indicate that c. 3-fold increases in Hg fluxes also occurred since 2000 in the remote sites, while Hg emissions from anthropogenic sources have remained relatively stable. The tropical and subtropical Americas are vulnerable to extreme weather events. Air temperatures in this region have shown a marked increase since the 1990s, and extreme weather events arising from climate change have increased. When comparing Hg fluxes to recent (1950-2016) climatic changes, results show marked increases in Hg fluxes to sediments during dry periods. The Standardized Precipitation-Evapotranspiration Index (SPEI) time series indicate a tendency toward more extreme drier conditions across the study region since the mid-1990s, suggesting that instabilities in catchment surfaces caused by climate change are responsible for the elevated Hg flux rates. Drier conditions since c. 2000 appear to be promoting Hg fluxes from catchments to lakes, a process that will likely be exacerbated under future climate-change scenarios.

High temporal resolution records of outdoor and indoor airborne microplastics.

There is increasing concern regarding airborne microplastics, but to date, studies have typically used coarse interval sampling (a day or longer) to generate deposition and concentration estimates. In this proof-of-concept study, we used a Burkard volumetric spore trap (intake 10 L min-1; recording airborne particulates onto an adhesive-coated tape moving at 2 mm hr-1) to assess whether this approach has potential to record airborne microplastics at an hourly resolution, thereby providing detailed diurnal patterns. Simultaneous sampling at outdoor and indoor locations at rural and urban sites showed clear daily and weekly patterns in microplastic concentrations which may be related to people and vehicle movement. Indoor residential concentrations of suspected microplastics were the highest (reaching hourly concentrations of 40-50 m-3), whilst rural outdoor concentrations were very low (typically 1-2 m-3 h-1). Whilst the approach shows great potential for high resolution data generation, further development is required for spectroscopic analysis and hence chemical confirmation of visual microplastic identification.

Deposition records of persistent organic pollutants and black carbon in dated sediment cores from China marginal seas: Implications for terrestrial sources and transport processes.

Black carbon (BC) and persistent organic pollutants (POPs) were analyzed from three sediment cores collected offshore in the East China Marginal Seas. The results showed steadily increasing or stable BC concentrations and fluxes. By contrast, time trends of POPs fluxes were consistent with historical records of commercial production and use in China. Although the POP inventories decreased significantly with increase in offshore distance, the relatively consistent trends for individual POPs in different sea areas confirmed that the main sources are derived from mainland China and that atmospheric input was an important contribution. POPs inventories decreased by 59-91 % during transport from the Yellow Sea to the remote East China Sea and deposition to the sediment. This suggests that the source signal for POPs may be preserved under stable depositional environments, even though only a fraction of those pollutants are buried in open sea sediments.

Temporal-spatial variations, source apportionment, and ecological risk of trace elements in sediments of water-level-fluctuation zone in the Three Gorges Reservoir, China.

The Three Gorges Reservoir (TGR) plays a crucial role in providing electricity for mega-cities across China. However, since the impoundment was completed in 2006, attention to environmental concerns has also been intensive. In order to determine the distribution, sources, and pollution status of trace elements in the water fluctuation zone of the TGR following ten years of repeated "submergence" and "exposure", we systematically collected 16 paired surface sediment samples (n = 32) covering the entire main body of the TGR in March 2018 (following 6 months of submergence) and September 2018 (after 6 months of exposure), and quantitatively analyzed 13 elements (e.g., Mn, Fe, V, Cr, Ni, Cu, Zn, As, Sr, Y, Zr, Ba, and Pb) using X-ray fluorescence spectrophotometry (XRF). The results showed that, except for Sr, concentrations of trace metals following submergence were generally higher than those after exposure due to the less settling of suspended solids at the faster flow velocity during the drawdown period. Assessment using enrichment factors (EFs) and a geo-accumulation index (Igeo) both characterized a relatively serious anthropogenic pollution status of metals in the upper reaches of the TGR with respect to the middle-lower reaches. Source apportionment by positive matrix factorization (PMF) analysis indicated that agricultural activities (24.8 and 24.3%, respectively) and industrial emissions (24.5 and 22.9%, respectively) were the two major sources in these two periods, followed by natural sources, domestic sewage, and ore mining. Ecological risk assessment showed that metalloid arsenic (As) could be the main potential issue of risk to aquatic organisms and human health. A new source-specific risk assessment method (pRI) combined with PMF revealed that agricultural activities could be the major source of potential ecological risk and should be prioritized as the focus of metal/metalloid risk management in the TGR.

Mercury atmospheric emission, deposition and isotopic fingerprinting from major coal-fired power plants in Australia: Insights from palaeo-environmental analysis from sediment cores.

Despite Australia's high reliance on coal for electricity generation, no study has addressed the extent to which mercury (Hg) deposition has increased since the commissioning of coal-fired power plants. We present stratigraphic data from lake sediments in the Hunter Valley (New South Wales) and Latrobe Valley (Victoria), where a significant proportion of Australia's electricity is generated via coal combustion. Mercury deposition in lake sediments increased in the 1970s with the commissioning of coal-fired power plants, by a factor of 2.9-times in sediments of Lake Glenbawn (Hunter Valley) and 14-times in Traralgon Reservoir (Latrobe Valley). Sediments deposited after the commissioning of power plants have distinct Hg isotope compositions, similar to those of combusted coals. Mercury emission, estimated using an atmospheric model (CALPUFF), was higher in the Latrobe Valley than in the Hunter Valley. This is a result of higher Hg concentrations in lignite coal, lax regulation and older pollution-control technologies adopted by coal-fired power plants in the Latrobe Valley. Near-source deposition of Hg in Australia is significantly higher than North America and Europe, where better emission controls (e.g. wet flue gas desulfurization) have been in effect for decades. The challenge for Australia in years to come will be to ratify the Minamata Convention and develop better regulation policies to reduce Hg emissions.

Temporal trends in radiometrically dated sediment cores from English lakes show polybrominated diphenyl ethers correlate with brominated but not mixed bromo/chloro dioxins and furans.

This paper reports concentrations between ~1950 and present, of polybrominated diphenyl ethers (PBDEs) and polybrominated dibenzo-p-dioxins and furans (PBDD/Fs), in radiometrically-dated sediment cores from three English lakes. Mixed bromo/chloro dibenzo-p-dioxins and furans (PXDD/Fs) were measured in two of the same lakes. Concentrations of PXDD/Fs decreased over time to the present. To our knowledge, this is the first report of temporal trends of PXDD/Fs in the environment. In contrast, concentrations of PBDEs increased towards the present and were significantly correlated (R = 0.88-0.98; p < 0.05) with concentrations of PBDFs in all three lakes. These observations suggest that the sources of PXDD/Fs are not related to PBDEs and differ from those of PBDFs. We also report for the first time the presence of octabromodibenzofuran (OBDF) in the two most recent core slices at one lake. The source of OBDF in these samples is unclear. While OBDF has been reported previously as a significant contaminant of some commercial formulations of Deca-BDE, it is also present in Octa-BDE products and in emissions from a variety of combustion activities. Overall, while the positive correlation between PBDEs and PBDFs suggests increased use of PBDEs has contributed substantially to environmental contamination with PBDFs; examination of PBDF homologue patterns implies emissions from combustion activities are likely also important.

Natural archives of long-range transported contamination at the remote lake Letseng-la Letsie, Maloti Mountains, Lesotho.

Naturally accumulating archives, such as lake sediments and wetland peats, in remote areas may be used to identify the scale and rates of atmospherically deposited pollutant inputs to natural ecosystems. Co-located lake sediment and wetland cores were collected from Letseng-la Letsie, a remote lake in the Maloti Mountains of southern Lesotho. The cores were radiometrically dated and analysed for a suite of contaminants including trace metals and metalloids (Hg, Pb, Cu, Ni, Zn, As), fly-ash particles, stable nitrogen isotopes, polycyclic aromatic hydrocarbons (PAHs) and persistent organic pollutants such as polychlorinated biphenyls (PCBs), polybrominated flame retardants (PBDEs) and hexachlorobenzene (HCB). While most trace metals showed no recent enrichment, mercury, fly-ash particles, high molecular weight PAHs and total PCBs showed low but increasing levels of contamination since c.1970, likely the result of long-range transport from coal combustion and other industrial sources in the Highveld region of South Africa. However, back-trajectory analysis revealed that atmospheric transport from this region to southern Lesotho is infrequent and the scale of contamination is low. To our knowledge, these data represent the first palaeolimnological records and the first trace contaminant data for Lesotho, and one of the first multi-pollutant historical records for southern Africa. They therefore provide a baseline for future regional assessments in the context of continued coal combustion in South Africa through to the mid-21st century.

A century of limnological evolution and interactive threats in the Panama Canal: Long-term assessments from a shallow basin.

Large tropical river dam projects are expected to accelerate over the forthcoming decades to satisfy growing demand for energy, irrigation and flood control. When tropical rivers are dammed the immediate impacts are relatively well studied, but the long-term (decades-centuries) consequences of impoundment remain poorly known. We combined historical records of water quality, river flow and climate with a multi-proxy (macrofossils, diatoms, biomarkers and trace elements) palaeoecological approach to reconstruct the limnological evolution of a shallow basin in Gatun Lake (Panama Canal, Panama) and assess the effects of multiple linked factors (river damming, forest flooding, deforestation, invasive species, pollution and hydro-climate) on the study area. Results show that a century after dam construction, species invasion, deforestation and salt intrusions have forced a gradual change in the study basin from a swamp-type environment towards a more saline lake-governed system of benthic-littoral production likely associated with the expansion of macrophyte stands. Hydrology still remains the most important long-term (decades) structural factor stimulating salinity intrusions, primary productivity, deposition of minerals, and reduction of water transparency during wet periods. During dry periods, physical-chemical conditions are in turn linked to clear water and aerobic conditions while nutrients shift to available forms for the aquatic biota in the detrital-rich reductive sediments. Our study suggests that to preserve the natural riverine system functioning of this area of the Panama Canal, management activities must address long-term ecosystem structural drivers such as river flow, runoff patterns and physical-chemical conditions.

Assessing environmental contamination from metal emission and relevant regulations in major areas of coal mining and electricity generation in Australia.

The Hunter and Latrobe Valleys have two of the richest coal deposits in Australia. They also host the largest coal-fired power stations in the country. We reconstructed metal deposition records in lake sediments in the Hunter and Latrobe Valleys to determine if metal deposition in freshwater lakes have increased in the region. The current regulatory arrangement applied to metal emissions from coal-fired power stations in Australia are presented, discussing their capacity to address future increases in metal deposition from these sources. Sediment records of spheroidal carbonaceous particles (SCPs), a component of fly-ash, were also used as an additional line of evidence to identify the contribution of industrial activities related to electricity generation to metal deposition in regions surrounding open-cut coal mines and coal-fired power stations. Sediment metal concentrations and SCP counts in the sedimentary records, from the Hunter and Latrobe Valleys, both indicated that open-cut coal mining and the subsequent combustion of coal in power stations has most likely resulted in an increase in atmospheric deposition of metals in the local region. In particular, the metalloids As and Se showed the greatest enrichment compared to before coal mining commenced. Although the introduction of bag filters at Liddell Power Station and the decommissioning of Hazelwood Power Station appear to have resulted in a decrease of metal deposition in nearby lakes, overall metal deposition in the environment is still increasing. The challenge for the years to come will be to develop better regulation policies and tools that will contribute to reduce metal emissions in these major electricity production centres in Australia.

Positive matrix factorization on source apportionment for typical pollutants in different environmental media: a review.

A bibliometric analysis of published papers with the key words "positive matrix factorization" and "source apportionment" in 'Web of Science', reveals that more than 1000 papers are associated with this research and that approximately 50% of these were produced in Asia. As a receptor-based model, positive matrix factorization (PMF) has been widely used for source apportionment of various environmental pollutants, such as persistent organic pollutants (POPs), heavy metals, volatile organic compounds (VOCs) as well as inorganic cations and anions in the last decade. In this review, based on the papers mainly from 2008 to 2018 that focused on source apportionment of pollutants in different environmental media, we provide a comparison and summary of the source categories of typical environmental pollutants, with a special focus on polycyclic aromatic hydrocarbons (PAHs), apportioned using PMF. Based on the statistical average, coal combustion and vehicular emission, are shown to be the two most common sources of PAHs, and contribute much more to emissions than other sources, such as biomass burning, biogenic sources and waste incineration. Heavy metals were mainly from agricultural activities, industrial and vehicular emissions and mining activities. Quantitative source apportionment on pollutants such as VOCs and particulate matter were also apportioned, showing a prominent contribution from fossil-fuel combustion. We conclude that, aside from natural sources, abatement strategies should be focused on changes in energy structure and industrial activities, especially in China. Source apportionment of typical POPs including polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), halogenated flame retardants (HFRs) and perfluorinated compounds (PFCs) is less comprehensive and further study is required.

Sources and dry deposition of carbonaceous aerosols over the coastal East China Sea: Implications for anthropogenic pollutant pathways and deposition.

75 paired TSP and PM2.5 samples were collected over four seasons on Huaniao Island (HNI), an island that lies downwind of continental pollutants emitted from mainland China to the East China Sea (ECS). These samples were analyzed for organic carbon (OC) and elemental carbon (EC), with a special focus on char-EC (char) and soot-EC (soot), to understand their sources, and the scale and extent of pollution and dry deposition over the coastal ECS. The results showed that char concentrations in PM2.5 and TSP averaged from 0.13 to 1.01 and 0.31-1.44 µg m-3; while for soot, they were from 0.03 to 0.21 and 0.16-0.56 µg m-3, respectively. 69.0% of the char and 36.4% of the soot were present in PM2.5. The char showed apparent seasonal variations, with highest concentrations in winter and lowest in summer; while soot displayed maximum concentrations in fall and minimum in summer. The char/soot ratios in PM2.5 averaged from 3.29 to 17.22; while for TSP, they were from 1.20 to 7.07. Both of the ratios in PM2.5 and TSP were highest in winter and lowest in fall. Comparisons of seasonal variations in OC/EC and char/soot ratios confirmed that char/soot may be a more effective indicator of carbonaceous aerosol source identification than OC/EC. Annual average atmospheric dry deposition fluxes of OC and EC into ECS were estimated to be 229 and 107 µg m-2 d-1, respectively, and their deposition fluxes significantly increased during episodes. It was estimated that the loadings of OC + EC and EC accounted for 1.3% and 4.1% of the total organic carbon and EC in ECS surface sediments, respectively, implying a relatively small contribution of OC and EC dry deposition to organic carbon burial. This finding also indicates a possibly more important contribution of wet deposition to organic carbon burial in sediments of ECS, and this factor should be considered for future study.

Legacy Lead Stored in Catchments Is the Dominant Source for Lakes in the U.K.: Evidence from Atmospherically Derived 210Pb.

There has been a considerable reduction in anthropogenic lead (Pb) emission in the atmosphere in recent decades. However, the reduction in Pb inputs in many lakes does not match this as the Pb stored in catchment upper soil layers, derived from previous deposition, has become an important source although it is difficult to assess quantitatively. This work uses atmospherically deposited 210Pb as a tracer to track Pb movement, and so for the first time, we were able to calculate the relative Pb inputs from direct atmospheric deposition and catchment sources to lakes in the U.K. directly. Within individual lake sites, ratios of 210Pb/Pb in the catchment terrestrial mosses were normally an order of magnitude higher than those in the catchment surface soils, trapped lake sediments, and the surface sediments in the lake bottom. Results suggest that the Pb isotope signatures in the mosses are close to or dominated by atmospheric depositions, and it is reasonable to use the ratios of 210Pb/Pb in terrestrial mosses collected from the lake sites with a high annual rainfall over 2000 mm to represent those in atmospheric depositions. It reveals that after the reduction in Pb emissions, catchment Pb inputs now typically account for more than 95% of the total Pb entering the lakes.