Anomalously weak Labrador Sea convection and Atlantic overturning during the past 150 years.

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 cycle1, 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 AMOC1, 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.

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.

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.

Palaeotoxicity: reconstructing the risk of multiple sedimentary pollutants to freshwater organisms.

'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.

A gradient of mercury concentrations in Scottish single malt whiskies.

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.

Spheroidal carbonaceous fly ash particles provide a globally synchronous stratigraphic marker for the Anthropocene.

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.

Spatial and Temporal Patterns in Black Carbon Deposition to Dated Fennoscandian Arctic Lake Sediments from 1830 to 2010.

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.

20th century atmospheric deposition and acidification trends in lakes of the Sierra Nevada, California, USA.

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.

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.

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.

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.

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 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.

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.

Long-range transport of pollutants to the Falkland Islands and Antarctica: evidence from lake sediment fly ash particle records.

(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.

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.

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 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.