Search

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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

The Mpumalanga Lake District (MLD) of South Africa hosts a regionally unique cluster of water bodies of great importance for wetland biodiversity. It is also located close to a global hotspot for coal-fired power station emissions but the local impacts from these sources of pollution are poorly understood. Sediment cores from three contrasting wetlands were 210 Pb dated and analysed for a range of contaminants linked to fossil fuel combustion, including trace elements, Hg, sulphur and spheroidal carbonaceous fly-ash particles (SCPs). At the two sites with pre-industrial (1900) baseline sediments, Pb, Zn and especially Cr concentrations and fluxes showed significant increases in the impact period (post-1975). Mercury showed the greatest proportional increase in flux (>4-fold) of all trace metals. Mercury and sulphur concentrations and fluxes showed highly significant correlations with emissions over the corresponding periods, while SCPs in sediments also closely tracked emissions. In a global context, levels of sediment contamination are relatively minor compared with other heavily industrialised regions, with only Cr exceeding the sediment Probable Effects Concentration for biological impact post-1975. Despite the relatively large increases in Hg, concentrations do not reach the Threshold Effects Concentration. The unexpectedly low levels of contamination may be due to i) low levels of many trace contaminants in South African coals compared to global averages, ii) prevailing recirculation patterns which transport pollution away from the study area during the wet season, minimising wet deposition, and iii) pollutant remobilisation through desiccation of wetlands or volatilization. The effects of hydrology and sediment accumulation rates lead to differential transport and preservation of organic-associated and more volatile contaminants (e.g. Hg, S) relative to non-volatile trace elements in wetlands of the MLD. The greatest fluxes of Hg and S are recorded in the site with the highest catchment: lake area ratio, lowest salinity and greatest sediment organic matter content., Competing Interests: Declaration of competing interest The authors declare no competing financial interests., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

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/m 2 /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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Crown Copyright © 2024. Published by Elsevier Ltd. All rights reserved.)

Fifty-two consecutive PM 2.5 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.

Fly-ash particles formed during industrial fossil-fuel combustion show a globally observed rapid increase in concentration within natural archives post-1950 and have been proposed as a marker for the Anthropocene Epoch. Here, we present the first record of fly-ash particles incorporated into coral skeletons. Particles are present in Mediterranean corals between CE 1957 and 1992 at concentrations of 8-30 g -1 coral, mirroring the period of increased industrial activity in the area, and corroborating with spheroidal carbonaceous particle (SCP) records globally. The findings have important implications for the use of SCPs as markers in natural archives. With the exception of microplastics, this is the first evidence of particulate contamination in corals collected from natural environments. Further research is needed to understand incorporation pathways into coral skeletons, any subsequent ecotoxicological impact of contaminants, and the influence on overall coral health globally., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

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., (© 2023 The Authors. Ecology and Evolution published by John Wiley & Sons Ltd.)

Spheroidal carbonaceous particles (SCPs) are a component of fly-ash, the particulate by-product of industrial high temperature combustion of fuel-oil and coal-series fuels. We provide the first evidence that these indelible markers of industrialisation have been deposited in Antarctic ice, thousands of kilometres from any potential source. The earliest observed particle was deposited in an ice layer from 1936 CE. While depositional fluxes are low, chemical analysis of individual SCPs indicates a coal combustion origin., (© 2023. The Author(s).)

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+240 Pu and 14 C: 12 C, 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., Competing Interests: The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article., (© The Author(s) 2023.)

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 239,240 Pu (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 239,240 Pu) and corresponding to October-December 1948 CE. This is consistent with a lag of 1-2 years between ejection of 239,240 Pu into the atmosphere and deposition. Auxiliary markers include: first appearance of 137 Cs in 1958; late 20th-century decreases in δ 15 N; 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., (© The Author(s) 2023.)

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.

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., (© 2023. The Author(s).)

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., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

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 (I geo ) 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., (© 2021. The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.)

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., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier B.V. All rights reserved.)

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 Letšeng-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., Competing Interests: Declaration of competing interest The authors declare no competing financial interest., (Copyright © 2020 Elsevier B.V. All rights reserved.)

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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier B.V. All rights reserved.)

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., Competing Interests: Declaration of competing interest No conflict of interest is declared for this study and final manuscript., (Copyright © 2020 Elsevier B.V. All rights reserved.)

Mercury (Hg) loading in Lake Baikal, a UNESCO world heritage site, is growing and poses a serious health concern to the lake's ecosystem due to the ability of Hg to transform into a toxic form, known as methylmercury (MeHg). Monitoring of Hg into Lake Baikal is spatially and temporally sparse, highlighting the need for insights into historic Hg loading. This study reports measurements of Hg concentrations from water collected in August 2013 and 2014 from across Lake Baikal and its main inflow, the Selenga River basin (Russia, Mongolia). We also report historic Hg contamination using sediment cores taken from the south and north basins of Lake Baikal, and a shallow lake in the Selenga Delta. Field measurements from August 2013 and 2014 show high Hg concentrations in the Selenga Delta and river waters, in comparison to pelagic lake waters. Sediment cores from Lake Baikal show that Hg enrichment commenced first in the south basin in the late-19th century, and then in the north basin in the mid-20th century. Hg flux was also 20-fold greater in the south basin compared to the north basin sediments. Hg enrichment was greatest in the Selenga Delta shallow lake (Enrichment Ratio (ER) = 2.3 in 1994 CE), with enrichment occurring in the mid-to late-20th century. Local sources of Hg are predominantly from gold mining along the Selenga River, which have been expanding over the last few decades. More recently, another source is atmospheric deposition from industrial activity in Asia, due to rapid economic growth across the region since the 1980s. As Hg can bioaccumulate and biomagnify through trophic levels to Baikal's top consumer, the world's only truly freshwater seal (Pusa sibirica), it is vital that Hg input at Lake Baikal and within its catchment is monitored and controlled., (Crown Copyright © 2020. Published by Elsevier Ltd. All rights reserved.)

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.

75 paired TSP and PM 2.5 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 PM 2.5 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 PM 2.5 . 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 PM 2.5 averaged from 3.29 to 17.22; while for TSP, they were from 1.20 to 7.07. Both of the ratios in PM 2.5 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., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

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 210 Pb 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 210 Pb/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 210 Pb/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.

Persistent organic pollutants (POPs) and polycyclic aromatic hydrocarbons (PAHs) have previously been detected in the surface sediments, water, and endemic organisms of Lake Baikal, a UNESCO World Heritage Site. The Selenga River is the primary source of freshwater to Lake Baikal, and transports pollutants accumulating in the Selenga River basin to the lake. Sources of POPs and PAHs in the Selenga River basin grew through the 20th century. In the present study, temporal changes in the concentrations of PAHs and POPs were reconstructed from two lakes in the Selenga River basin over the past 150 years using paleolimnological techniques. Increased concentrations in PAHs and PCBs were recorded initially in the 1930s. The 1940s-1980s was the period of greatest exposure to organic contamination, and concentrations of dichlorodiphenyltrichloroethane (DDT), polychlorinated biphenyls (PCBs), hexachlorocyclohexanes (HCHs) and many PAHs peaked between the 1960s and 1980s in the two lakes. Declines in concentrations and fluxes were recorded for most PAHs and POPs in the 1980s and 1990s. Temporal trends in concentrations of total and individual compounds/congeners of PAH, PCBs, and polybrominated diphenyl ethers (PBDEs) indicate the contribution of both local and regional sources of contamination in the 20th and 21st centuries. Temporal variations in contaminants can be linked to economic and industrial growth in the former USSR after World War II and the economic decline of Russia in the late-1980s and early-1990s, as well as global trends in industrialization and development during the mid-20th century., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

'Real-world' contaminant exposure of sediment-dwelling biota is typically long-term, low-level and to multiple pollutants. However, sediment quality guidelines, designed to protect these organisms, relate only to single contaminants. This study uses radiometrically dated sediment cores from 7 English lakes with varying contamination histories to reconstruct temporal changes in likely risk to biota (herein termed 'palaeotoxicity'). The Probable Effects Concentration Quotient (PEC-Q) approach was used to combine sediment concentrations from multiple contaminants (trace metals; PCBs; PBDEs) to determine risk allocated to metals and persistent organic pollutants (POPs) separately as well as combined (PEC-Q Mean-All). Urban-influenced lakes were considerably more contaminated, exceeding PEC-Q thresholds of 0.5 and 2.0 over long durations (some since the nineteenth century). This has been mainly due to metals (principally lead) and by factors of up to 10 for individual metals and by > 2 for PEC-Q Mean-Metals. In 6 out of 7 lakes, considerable reductions in risk associated with trace metals are observed since emissions reductions in the 1970s. However, at all lakes, PEC-Q Mean-POPs has increased sharply since the 1950s and at 5 out of 7 lakes now exceeds PEC-Q Mean-Metals. These organic pollutants are therefore now the dominant driver behind elevated contaminant risk to sediment-dwelling biota and recent temporal trends in PEC-Q Mean-All remain above threshold values as a result. Finally, PEC-Q Mean-All values were compared to standard biological toxicity tests for surface sediments at each site. While chironomid growth and daphniid reproduction were significantly reduced compared to controls at 5 out of 7, and all lakes, respectively, the scale of these reductions showed only limited quantitative agreement with predicted risk.

Fossil fuel combustion leads to increased levels of air pollution, which negatively affects human health as well as the environment. Documented data for Southeast Asia (SEA) show a strong increase in fossil fuel consumption since 1980, but information on coal and oil combustion before 1980 is not widely available. Spheroidal carbonaceous particles (SCPs) and heavy metals, such as mercury (Hg), are emitted as by-products of fossil fuel combustion and may accumulate in sediments following atmospheric fallout. Here we use sediment SCP and Hg records from several freshwater lentic ecosystems in SEA (Malaysia, Philippines, Singapore) to reconstruct long-term, region-wide variations in levels of these two key atmospheric pollution indicators. The age-depth models of Philippine sediment cores do not reach back far enough to date first SCP presence, but single SCP occurrences are first observed between 1925 and 1950 for a Malaysian site. Increasing SCP flux is observed at our sites from 1960 onward, although individual sites show minor differences in trends. SCP fluxes show a general decline after 2000 at each of our study sites. While the records show broadly similar temporal trends across SEA, absolute SCP fluxes differ between sites, with a record from Malaysia showing SCP fluxes that are two orders of magnitude lower than records from the Philippines. Similar trends in records from China and Japan represent the emergence of atmospheric pollution as a broadly-based inter-region environmental problem during the 20th century. Hg fluxes were relatively stable from the second half of the 20th century onward. As catchment soils are also contaminated with atmospheric Hg, future soil erosion can be expected to lead to enhanced Hg flux into surface waters., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

The Atlantic meridional overturning circulation (AMOC) is a system of ocean currents that has an essential role in Earth's climate, redistributing heat and influencing the carbon cycle 1, 2 . The AMOC has been shown to be weakening in recent years 1 ; this decline may reflect decadal-scale variability in convection in the Labrador Sea, but short observational datasets preclude a longer-term perspective on the modern state and variability of Labrador Sea convection and the AMOC 1, 3-5 . Here we provide several lines of palaeo-oceanographic evidence that Labrador Sea deep convection and the AMOC have been anomalously weak over the past 150 years or so (since the end of the Little Ice Age, LIA, approximately AD 1850) compared with the preceding 1,500 years. Our palaeoclimate reconstructions indicate that the transition occurred either as a predominantly abrupt shift towards the end of the LIA, or as a more gradual, continued decline over the past 150 years; this ambiguity probably arises from non-AMOC influences on the various proxies or from the different sensitivities of these proxies to individual components of the AMOC. We suggest that enhanced freshwater fluxes from the Arctic and Nordic seas towards the end of the LIA-sourced from melting glaciers and thickened sea ice that developed earlier in the LIA-weakened Labrador Sea convection and the AMOC. The lack of a subsequent recovery may have resulted from hysteresis or from twentieth-century melting of the Greenland Ice Sheet 6 . Our results suggest that recent decadal variability in Labrador Sea convection and the AMOC has occurred during an atypical, weak background state. Future work should aim to constrain the roles of internal climate variability and early anthropogenic forcing in the AMOC weakening described here.

We report a historical record of atmospheric deposition in dated sediment cores from Hasse Lake, ideally located near both currently and previously operational coal-fired power plants in Central Alberta, Canada. Accumulation rates of spheroidal carbonaceous particles (SCPs), an unambiguous marker of high-temperature fossil-fuel combustion, in the early part of the sediment record (pre-1955) compared well with historical emissions from one of North America's earliest coal-fired power plants (Rossdale) located ∼43 km to the east in the city of Edmonton. Accumulation rates in the latter part of the record (post-1955) suggested inputs from the Wabamun region's plants situated ∼17-25 km to the west. Increasing accumulation rates of SCPs, polycyclic aromatic hydrocarbons (PAHs) and Hg coincided with the previously documented period of peak pollution in the Wabamun region during the late 1960s to early 1970s, although Hg deposition trends were also similar to those found in western North American lakes not directly affected by point sources. A noticeable reduction in contaminant inputs during the 1970s is attributed in part to technological improvements and stricter emission controls. The over one hundred-year historical record of coal-fired power plant emissions documented in Hasse Lake sediments has provided insight into the impact that both environmental regulations and changes in electricity output have had over time. This information is crucial to assessing the current and future role of coal in the world's energy supply., (Crown Copyright © 2017. Published by Elsevier Ltd. All rights reserved.)

While studies on microplastics in the marine environment show their wide-distribution, persistence and contamination of biota, the freshwater environment remains comparatively neglected. Where studies on freshwaters have been undertaken these have been on riverine systems or very large lakes. We present data on the distribution of microplastic particles in the sediments of Edgbaston Pool, a shallow eutrophic lake in central Birmingham, UK. These data provide, to our knowledge, the first assessment of microplastic concentrations in the sediments of either a small or an urban lake and the first for any lake in the UK. Maximum concentrations reached 25-30 particles per 100 g dried sediment (equivalent to low hundreds kg -1 ) and hence are comparable with reported river sediment studies. Fibres and films were the most common types of microplastic observed. Spatial distributions appear to be due to similar factors to other lake studies (i.e. location of inflow; prevailing wind directions; propensity for biofouling; distribution of macroplastic debris) and add to the growing burden of evidence for microplastic ubiquity in all environments., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

The use of geoforensic analysis in criminal investigations is continuing to develop, with the diversification of analytical techniques, many of which are semi-automated, facilitating prompt analysis of large sample sets at a relatively low cost. Whilst micro-scale geoforensic analysis has been shown to assist criminal investigations including homicide (Concheri et al., 2011 [1]), wildlife crime (Morgan et al., 2006 [2]), illicit drug distribution (Stanley, 1992 [3]), and burglary (Mildenhall, 2006 [4]), its application to the pressing international security threat posed by Improvised Explosive Devices (IEDs) is yet to be considered. This experimental study simulated an IED supply chain from the sourcing of raw materials through to device emplacement. Mineralogy, quartz grain surface texture analysis (QGSTA) and particle size analysis (PSA) were used to assess whether environmental materials were transferred and subsequently persisted on the different components of three pressure plate IEDs. The research also addressed whether these samples were comprised of material from single or multiple geographical provenances that represented supply chain activity nodes. The simulation demonstrated that material derived from multiple activity nodes, was transferred and persisted on device components. The results from the mineralogy and QGSTA illustrated the value these techniques offer for the analysis of mixed provenance samples. The results from the PSA, which produces a bulk signature of the sample, failed to distinguish multiple provenances. The study also considered how the environmental material recovered could be used to generate information regarding the geographical locations the device had been in contact with, in an intelligence style investigation, and demonstrated that geoforensic analysis has the potential to be of value to international counter-IED efforts. It is a tool that may be used to prevent the distribution of large quantities of devices, by aiding the identification of the geographical location of key activity nodes., (Copyright © 2017 The Authors. Published by Elsevier B.V. All rights reserved.)

Nine paired samples of atmospheric particulate matter with an aerodynamic diameter less than or equal to 2.5 μm (PM 2.5 ) were collected concurrently from an urban site in Shanghai, China and a background site in Huaniao Island (HNI) in the coastal East China Sea (ECS) between July 21 and 29, 2011. The samples were analyzed for 16 United States Environmental Protection Agency (USEPA) priority polycyclic aromatic hydrocarbons (PAHs), n-alkanes (20 species, C 14 -C 33 ), hopanes (10 species, C 29 -C 32 ), and steranes (12 species, C 27 -C 29 ). These two sites, approximately 66 km apart, are both on the pathway of land-based pollutants as they are transported to the ECS by seasonal winds. As expected, concentrations in Shanghai were higher (average: 8.4 and 67.8 ng m -3 for the 16 PAHs and n-alkanes, respectively) than those in HNI (average: 1.8 and 8.5 ng m -3 , respectively). The dominant contributor to the 16 PAHs in Shanghai was 5-6-ring PAHs (60.0%), whereas 2-3-ring PAHs contributed the most (72.5%) in HNI. Plant waxes contributed 45.7% and 25.9% of the n-alkanes in Shanghai and HNI, respectively, implying a relatively greater contribution from petroleum residues to the n-alkanes in HNI. Principal component analysis (PCA) and the compositions of hopanes and steranes highlighted a prominent contribution from traffic emissions to carbonaceous PM 2.5 aerosols. This study provides comprehensive details about the sources, formation, and transport of pollutants from eastern China to the coastal ECS.

Members of the public in England were invited in 2010 to take part in a national metals survey, by collecting samples of littoral sediment from a standing water body for geochemical analysis. To our knowledge, this is the first national sediment metals survey using public participation and reveals a snapshot of the extent of metals contamination in ponds and lakes across England. Hg, Ni, Cu, Zn and Pb concentrations exceeding sediment quality guidelines for the health of aquatic biota are ubiquitous in ponds and lakes, not just in areas with a legacy of industrial activity. To validate the public sampling approach, a calibration exercise was conducted at ten water bodies selected to represent a range of lakes found across England. Sediment concentrations of Hg, Ni, Cu, Zn and Pb were measured in samples of soil, stream and littoral and deep water sediment to assess inputs. Significant differences between littoral sediment metal concentrations occur due to local variability, but also organic content, especially in upland, peat soil catchments. Variability of metal concentrations between littoral samples is shown to be low in small (<20 ha) lowland lakes. Larger and upland lakes with more complex inputs and variation in organic content of littoral samples have a greater variability. Collection of littoral sediments in small lakes and ponds, with or without voluntary participation, can provide a reliable sampling technique for the preliminary assessment of metal contamination in standing waters. However, the heterogeneity of geology, soils and history/extent of metal contamination in the English landscape, combined with the random nature of sample collection, shows that systematic sampling for evaluating the full extent of metal contamination in lakes is still required.

The homologous glycosyltransferases α-1,3-N-acetylgalactosaminyltransferase (GTA) and α-1,3-galactosyltransferase (GTB) carry out the final synthetic step of the closely related human ABO(H) blood group A and B antigens. The catalytic mechanism of these model retaining enzymes remains under debate, where Glu303 has been suggested to act as a putative nucleophile in a double displacement mechanism, a local dipole stabilizing the intermediate in an orthogonal associative mechanism or a general base to stabilize the reactive oxocarbenium ion-like intermediate in an SNi-like mechanism. Kinetic analysis of GTA and GTB point mutants E303C, E303D, E303Q and E303A shows that despite the enzymes having nearly identical sequences, the corresponding mutants of GTA/GTB have up to a 13-fold difference in their residual activities relative to wild type. High-resolution single crystal X-ray diffraction studies reveal, surprisingly, that the mutated Cys, Asp and Gln functional groups are no more than 0.8 Å further from the anomeric carbon of donor substrate compared to wild type. However, complicating the analysis is the observation that Glu303 itself plays a critical role in maintaining the stability of a strained "double-turn" in the active site through several hydrogen bonds, and any mutation other than E303Q leads to significantly higher thermal motion or even disorder in the substrate recognition pockets. Thus, there is a remarkable juxtaposition of the mutants E303C and E303D, which retain significant activity despite disrupted active site architecture, with GTB/E303Q, which maintains active site architecture but exhibits zero activity. These findings indicate that nucleophilicity at position 303 is more catalytically valuable than active site stability and highlight the mechanistic elasticity of these enzymes., (© The Author 2016. Published by Oxford University Press. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.)

Sediment cores and soil samples were taken from nine lakes and their catchments across England with varying degrees of direct human disturbance. Mercury (Hg) analysis demonstrated a range of impacts, many from local sources, resulting from differing historical and contemporary site usage and management. Lakes located in industrially important areas showed clear evidence for early Hg pollution with concentrations in sediments reaching 400-1600 ng g -1 prior to the mid-19th century. Control of inputs resulting from local management practices and a greater than 90% reduction in UK Hg emissions since 1970 were reflected by reduced Hg pollution in some lakes. However, having been a sink for Hg deposition for centuries, polluted catchment soils are now the major Hg source for most lakes and consequently recovery from reduced Hg deposition is being delayed., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Background: Public participation in scientific data collection is a rapidly expanding field. In water quality surveys, the involvement of the public, usually as trained volunteers, generally includes the identification of aquatic invertebrates to a broad taxonomic level. However, quality assurance is often not addressed and remains a key concern for the acceptance of publicly-generated water quality data. The Open Air Laboratories (OPAL) Water Survey, launched in May 2010, aimed to encourage interest and participation in water science by developing a 'low-barrier-to-entry' water quality survey. During 2010, over 3000 participant-selected lakes and ponds were surveyed making this the largest public participation lake and pond survey undertaken to date in the UK. But the OPAL approach of using untrained volunteers and largely anonymous data submission exacerbates quality control concerns. A number of approaches were used in order to address data quality issues including: sensitivity analysis to determine differences due to operator, sampling effort and duration; direct comparisons of identification between participants and experienced scientists; the use of a self-assessment identification quiz; the use of multiple participant surveys to assess data variability at single sites over short periods of time; comparison of survey techniques with other measurement variables and with other metrics generally considered more accurate. These quality control approaches were then used to screen the OPAL Water Survey data to generate a more robust dataset., Results: The OPAL Water Survey results provide a regional and national assessment of water quality as well as a first national picture of water clarity (as suspended solids concentrations). Less than 10 % of lakes and ponds surveyed were 'poor' quality while 26.8 % were in the highest water quality band., Conclusions: It is likely that there will always be a question mark over untrained volunteer generated data simply because quality assurance is uncertain, regardless of any post hoc data analyses. Quality control at all stages, from survey design, identification tests, data submission and interpretation can all increase confidence such that useful data can be generated by public participants.

Multiple PM2.5 samples collected through different seasons from October 2011 to August 2012 at an urban site in Shanghai, China were analyzed for carbonaceous pollutants. Data from this site, a 'super' air quality monitoring station at Fudan University, has been used by researchers to investigate the formation mechanism of haze episodes. The characteristics and concentrations of organic carbon (OC), elemental carbon (EC), n-alkanes, as well as relative abundances of hopanes, in these samples were determined. The concentrations showed a pronounced annual cycle with higher values in cold seasons (spring and winter, mean: 8.6 μg/m(3), 3.3 μg/m(3) and 136.4 ng/m(3) for OC, EC and n-alkanes, respectively) and lower values in warm seasons (fall and summer, mean: 6.6 μg/m(3), 2.6 μg/m(3) and 73.8 ng/m(3) for OC, EC and n-alkanes, respectively). EC generally displayed a common source with that of OC in all seasons. Petroleum residue was the major source of n-alkanes, contributing 71.4% to the targeted C14-C33n-alkanes over four seasons. Principal components analysis and the composition of hopanes showed that emissions from vehicle exhaust contributed more carbonaceous aerosols than coal combustion. These data could provide important information for measures to reduce carbonaceous pollutant emissions and improve air quality in Shanghai, and other urban centers across China., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Mercury (Hg) concentrations were measured in 26 Scottish single malt whiskies, and all found to be very low (<10 ng L(-1)), posing no threat to human health through reasonable levels of consumption. However, a significant south-to-north declining gradient in Hg concentrations was observed reflecting that reported for atmospheric deposition. We speculate that this gradient could be due to a combination of contemporary deposition and the legacy of industrial mercury emissions and deposition over the last 200 years affecting concentrations in local waters used in whisky production. As UK atmospheric emissions of mercury have declined by 90 % since the 1970s, we suggest that whisky being produced today should have even lower Hg concentrations when consumed in 10- to 15-years time. This reduction may be compromised by the remobilisation of contaminants stored in catchment soils being transferred to source waters, but is very unlikely to raise the negligible health risk due to Hg from Scottish single malt whisky consumption.

Information on historical deposition of persistent organic pollutants (POPs) for African lakes is very limited. We investigated historical deposition trends and sources of POPs in sediment cores from Lakes Victoria (SC1), Bujuku (Buju2) and Mahoma (Maho2). The latter two lakes are situated in the Rwenzori mountain range in western Uganda. SC1 was taken from a central depositional area within the Ugandan part of the lake. Profiles in Buju2 and Maho2 were used as a reference for historical atmospheric deposition. For the post-1940 sediment deposits in SC1, average focusing factor-adjusted fluxes (FFFs) of ΣDDTs, polychlorinated biphenyls (ΣPCBs), hexachlorocyclohexanes (ΣHCHs) and chlordanes (ΣCHLs) were 390, 230, 210 and 120 ng m(-2) yr(-1). Higher fluxes of ΣDDTs, ΣPCBs, and ΣCHLs were observed in Buju2 and Maho2. The average FFF of HCB in Buju2 was the highest while the values for Maho2 and SC1 were similar. The endosulfan FFFs in SC1 were lower than in the alpine lake cores. Generally, Buju2 was a better reference for historical atmospheric deposition of POPs than Maho2 probably due to distortion of the latter's profile by Lake Mahoma's forested catchment. Profiles of p,p'-DDE, ΣCHLs and HCB in SC1 were consistent with atmospheric deposition while profiles of PCBs and HCHs were indicative of particle-bound loadings from additional sources. Profiles of endosulfans, DDTs, and chlordanes were consistent with influence of other factors such as anoxia, and dilution. Further studies of spatial resolution of historical deposition, especially in near-shore deposition areas of the lake are recommended., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

This paper reports input fluxes between ~1950 and present, of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), and hexabromocyclododecanes (HBCDs) in radiometrically-dated sediment cores from 7 English lakes. Fluxes of PCBs at all but one location prone to significant sediment resuspension peaked in the late-1960s/early-1990s, before declining thereafter. Input fluxes of HBCDs at all sites increased from first emergence in the mid-1960s. Thereafter, fluxes peaked in the late-1980s/early-2000s, before declining through to the present, except at the most urban site where HBCD fluxes are still increasing. Trends of PBDEs predominant in the Penta-BDE and Octa-BDE formulations vary between sites. While at some locations, fluxes peaked in the late-1990s/early-2000s; at others, fluxes are still increasing. This suggests the full impact of EU restrictions on these formulations has yet to be felt. Fluxes of BDE-209 have yet to peak at all except one location, suggesting little discernible environmental response to recent EU restrictions on the Deca-BDE product. Strikingly, fluxes of BDE-209 in the most recent core slices either exceed or approach peak fluxes of ΣPCBs, implying substantial UK use of Deca-BDE. Excepting HBCDs, inventories of our target contaminants correlated significantly with local population density, implying substantial urban sources., (Copyright © 2015 Elsevier B.V. All rights reserved.)

Black carbon (BC) is fine particulate matter produced by the incomplete combustion of biomass and fossil fuels. It has a strong climate warming effect that is amplified in the Arctic. Long-term trends of BC play an important role in assessing the climatic effects of BC and in model validation. However, few historical BC records exist from high latitudes. We present five lake-sediment soot-BC (SBC) records from the Fennoscandian Arctic and compare them with records of spheroidal carbonaceous fly-ash particles (SCPs), another BC component, for ca. the last 120 years. The records show spatial and temporal variation in SBC fluxes. Two northernmost lakes indicate declining values from 1960 to the present, which is consistent with modeled BC deposition and atmospheric measurements in the area. However, two lakes located closer to the Kola Peninsula (Russia) have recorded increasing SBC fluxes from 1970 to the present, which is likely caused by regional industrial emissions. The increasing trend is in agreement with a Svalbard ice-core-BC record. The results suggest that BC deposition in parts of the European Arctic may have increased over the last few decades, and further studies are needed to clarify the spatial extent of the increasing BC values and to ascertain the climatic implications.

Human impacts on Earth are now so great that they have led to the concept of a new geological epoch defined by this global human influence: the Anthropocene. While not universally accepted, the term is increasingly popular and widely used. However, even among proponents, there is considerable debate regarding when the epoch may have started, from coeval with the Holocene, through the Industrial Revolution, to the mid-20th century when unprecedented human activities resulted in exponential increases in population, resource consumption, and pollutant emission. Recently, this latter period, known as the Great Acceleration, appears to be becoming the more widely accepted start date. To define any start point, a global stratigraphic marker or Global Boundary Stratotype Section and Point (GSSP) is typically required. Here, spheroidal carbonaceous fly ash particles (SCPs), byproducts of industrial fossil-fuel combustion, are proposed as a primary marker for a GSSP at the time of the Great Acceleration. Data from over 75 lake sediment records show a global, synchronous, and dramatic increase in particle accumulation starting in c. 1950 driven by the increased demand for electricity and the introduction of fuel-oil combustion, in addition to coal, as a means to produce it. SCPs are morphologically distinct and solely anthropogenic in origin, providing an unambiguous marker. This is a clear signal of great stratigraphic utility representing a primary driving force for global anthropogenic change.

We investigated multiple lines of evidence to determine if observed and paleo-reconstructed changes in acid neutralizing capacity (ANC) in Sierra Nevada lakes were the result of changes in 20th century atmospheric deposition. Spheroidal carbonaceous particles (SCPs) (indicator of anthropogenic atmospheric deposition) and biogenic silica and δ(13)C (productivity proxies) in lake sediments, nitrogen and sulfur emission inventories, climate variables, and long-term hydrochemistry records were compared to reconstructed ANC trends in Moat Lake. The initial decline in ANC at Moat Lake occurred between 1920 and 1930, when hydrogen ion deposition was approximately 74 eq ha(-1) yr(-1), and ANC recovered between 1970 and 2005. Reconstructed ANC in Moat Lake was negatively correlated with SCPs and sulfur dioxide emissions (p = 0.031 and p = 0.009). Reconstructed ANC patterns were not correlated with climate, productivity, or nitrogen oxide emissions. Late 20th century recovery of ANC at Moat Lake is supported by increasing ANC and decreasing sulfate in Emerald Lake between 1983 and 2011 (p < 0.0001). We conclude that ANC depletion at Moat and Emerald lakes was principally caused by acid deposition, and recovery in ANC after 1970 can be attributed to the United States Clean Air Act.

Concentrations of tri-to-hexa-BDEs were determined in water samples taken from 9 English lakes on 13 occasions between April 2008 and February 2012. Across all sites, concentrations of ΣBDEs in individual samples ranged from 9.2 to 171.5pgL(-)(1), with an average of 61.9pgL(-)(1). Notwithstanding the far greater use of the Penta-BDE commercial formulation in the USA, concentrations in this study are comparable to the limited data available for the Great Lakes. PBDE concentrations showed no evidence of a decline at any monitored location over the study period. This may be because this study commenced 4years after the introduction of restrictions on the Penta- and Octa-BDE formulations. While concentrations normalised to water volume at the different locations were statistically indistinguishable; significant spatial variation was apparent when the data were normalised to total suspended solids (TSS) content. However, this spatial variation was not correlated with factors such as population density and lake catchment area, suggesting that concentrations of PBDEs in lake water in this study are a complex integral of numerous factors. BDE-47:99 ratios and concentrations of ΣBDEs respectively decreased and increased significantly with increasing TSS content. As TSS content was elevated in colder compared with warmer periods, such seasonal variation in TSS content appears a major contributor to the observed elevation of ΣBDE concentrations in colder periods, and higher BDE-47:99 ratios in warmer periods., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Depositional records of methylmercury (MeHg) are rare, especially for remote and mountainous areas. Our data from Lochnagar, a mountain lake in Scotland, covering a 7-year period from 2001-2008, show an unusual seasonal pattern in that elevated MeHg concentrations occur each winter while concentrations each summer fall below the limit of detection. To our knowledge this is the first time this seasonal pattern has been reported. Peak concentrations at the site in October 2006 (1.2 ng L(-1)) are amongst the highest reported depositional values in the literature. As the soils and lakes in the region are frozen or snow covered for much of each winter, we consider possible sources of this winter deposited MeHg to be either aqueous phase methylation in the atmosphere or marine evasion. However, the factor driving this seasonal pattern is likely to be scavenging by snow, as elevated concentrations in deposition coincide with periods of snowfall at the site. If this mechanism is correct, then predicted impacts of climate change, which will reduce annual snowfall at the site by between 50% and 100% by 2080, will effectively eliminate this input source. However, other climate-influenced inputs of mercury, such as remobilisation from catchment soils, are likely to increase and negate any benefit., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

(210)Pb-dated sediment cores taken from lakes on the Falkland Islands, the South Orkney Islands, and the Larsemann Hills in Antarctica were analyzed for fly ash particles to assess the temporal record of contamination from high temperature fossil-fuel combustion sources. Very low, but detectable, levels were observed in the Antarctic lakes. In the Falkland Island lakes, the record of fly ash extended back to the late-19th century and the scale of contamination was considerably higher. These data, in combination with meteorological, modeling, and fossil-fuel consumption data, indicate most likely sources are in South America, probably Chile and Brazil. Other southern hemisphere sources, notably from Australia, contribute to a background contamination and were more important historically. Comparing southern polar data with the equivalent from the northern hemisphere emphasizes the difference in contamination of the two circumpolar regions, with the Falkland Island sites only having a level of contamination similar to that of northern Svalbard.

We report a synchronous increase in accumulation of reduced inorganic sulfur since c. 1980 in sediment cores from eight of nine lakes studied in the Canadian Arctic and Svalbard (Norway). Sediment incubations and detailed analyses of sediment profiles from two of the lakes indicate that increases in sulfur accumulation may be due ultimately to a changing climate. Warming-induced lengthening of the ice-free season is resulting in well-documented increases in algal production and sedimentation of the resulting detrital matter. Algal detritus is a rich source of labile carbon, which in these sediments stimulates dissimilatory sulfate reduction. The sulfide produced is stored in sediment (as acid volatile sulfide), converted to other forms of sulfur, or reoxidized to sulfate and lost to the water column. An acceleration of the sulfur cycle in Arctic lakes could have profound effects on important biogeochemical processes, such as carbon burial and mercury methylation.