Impact of Absolute Myocardial Blood Flow Quantification on the Diagnostic Performance of PET-Based Perfusion Scans Using 82Rubidium.

BACKGROUND: Guidelines propose the inclusion of quantitative measurements from 82Rubidium positron emission tomography (RbPET) to discriminate obstructive coronary artery disease (CAD). However, the effect on diagnostic accuracy is unknown. The aim was to investigate the optimal RbPET reading algorithm for improved identification of obstructive CAD. METHODS: Prospectively enrolled patients (N=400) underwent RbPET and invasive coronary angiography with fractional flow reserve and quantitative coronary angiography. Quantitative measurements (myocardial blood flow (MBF), MBF reserve, transient ischemic dilatation) by RbPET were step-wisely added to a qualitative assessment by the summed stress score based on their diagnostic accuracy of obstructive CAD by invasive coronary angiography-fractional flow reserve. Prespecified cutoffs were summed stress score ≥4, hyperemic MBF 2.00 mL/g per min, and MBF reserve 1.80, respectively. Hemodynamically obstructive CAD was defined as >90% diameter stenosis or invasive coronary angiography-fractional flow reserve ≤0.80, and sensitivity analyses included a clinically relevant reference of anatomically severe CAD (>70% diameter stenosis by invasive coronary angiography-quantitative coronary angiography). RESULTS: Hemodynamically obstructive CAD was present in 170/400 (42.5%) patients. Stand-alone summed stress score showed a sensitivity and specificity of 57% and 93%, respectively, while hyperemic MBF showed similar sensitivity (61%, P=0.57) but lower specificity (85%, P=0.008). With increased discrimination by receiver-operating characteristic curves (0.78 versus 0.85; P<0.001), combining summed stress score, MBF and MBF reserve showed the highest sensitivity of 77% but lower specificity of 74% (P<0.001 for both comparisons). Against anatomically severe CAD, all measures independently yielded high discrimination ≥0.90 with increased sensitivity and lower specificity by additional quantification. CONCLUSIONS: The inclusion of quantitative measurements to a RbPET read increases in the identification of obstructive CAD. REGISTRATION: URL: https://www.clinicaltrials.gov; Unique identifier: NCT03481712.

Divergent Temporal Trends of Mercury in Arctic Char from Paired Lakes Influenced by Climate-Related Drivers.

Climate-driven changes including rising air temperatures, enhanced permafrost degradation, and altered precipitation patterns can have profound effects on contaminants, such as mercury (Hg), in High Arctic lakes. Two physically similar lakes, East Lake and West Lake at the Cape Bounty Arctic Watershed Observatory on Melville Island, Nunavut, Canada are being affected by climate change differently. Both lakes have experienced permafrost degradation in their catchments; however, West Lake has also undergone multiple underwater Mass Movement Events (MMEs; beginning in fall 2008), leading to a sustained 50-fold increase in turbidity. This provided the unique opportunity to understand the potential impacts of permafrost degradation and other climate-related effects on Hg concentrations and body condition of landlocked Arctic char (Salvelinus alpinus), an important sentinel species across the Circum-Arctic. Our objectives were to assess temporal trends in char Hg concentrations and to determine potential mechanisms driving the trends. There was a significant decrease in Hg concentrations in East Lake char, averaging 6.5%/year and 3.8%/year for length-adjusted and age-adjusted means, respectively, from 2008 to 2019. Conversely, in West Lake there was a significant increase, averaging 7.9%/year and 8.0%/year for length-adjusted and age-adjusted mean Hg concentrations, respectively, for 2009 to 2017 (the last year with sufficient sample size). The best predictors of length-adjusted Hg concentrations in West Lake were carbon and nitrogen stable isotope ratios, indicating a shift in diet including possible dietary starvation brought on by the profound increase in lake turbidity. Our study provides an example of how increasing lake turbidity, a likely consequence of climate warming in Arctic lakes, may influence fish condition and Hg concentrations. Environ Toxicol Chem 2023;42:2712-2725. © 2023 His Majesty the King in Right of Canada and The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC. Reproduced with the permission of the Minister of Environment and Climate Change Canada.

Mercury at the top of the world: A 31-year record of mercury in Arctic char in the largest High Arctic lake, linked to atmospheric mercury concentrations and climate oscillations.

Lake Hazen, the largest lake north of the Arctic circle, is being impacted by mercury (Hg) pollution and climate change. The lake is inhabited by two morphotypes of land-locked Arctic char (Salvelinus alpinus), a sensitive indicator species for pollution and climatic impacts. The objectives of this study were to describe the trends in Hg concentration over time and to determine the relationship of climate to length-at-age and Hg concentrations in each char morphotype, as well as the relationship to atmospheric Hg measurements at a nearby monitoring station. Results for Hg in char muscle were available from 20 sampling years over the period 1990 to 2021. We found significant declines in Hg concentrations for both morphotypes during the 31-year study period. Increased rain and earlier freeze-up of lake ice during the summer growing season was linked to increased length-at-age in both char morphotypes. For the large morphotype, higher total gaseous Hg in the fall and winter seasons was related to higher concentrations of Hg in char, while increased glacial runoff was related to decreases in char Hg. For the small morphotype char, increased snow and snow accumulation in the fall season were linked to declines in char Hg concentration. The Atlantic Multidecadal Oscillation and Arctic Oscillation were positively related to the large char Hg trend and Arctic Oscillation was positively related to the small char Hg trend. Significant trend relationships between atmospheric Hg and Hg in biota in remote regions are rare and uniquely valuable for evaluation of the effectiveness of the Minamata Convention and related monitoring efforts.

Changing environmental conditions have altered the feeding ecology of two keystone Arctic marine predators.

Environmental change in the Arctic has impacted the composition and structure of marine food webs. Tracking feeding ecology changes of culturally-valued Arctic char (Salvelinus alpinus) and ringed seals (Pusa hispida) can provide an indication of the ecological significance of climate change in a vulnerable region. We characterized how changes in sea ice conditions, sea surface temperature (SST), and primary productivity affected the feeding ecology of these two keystone species over a 13- and 18-year period, respectively, in northern Labrador, Canada. Arctic char fed consistently on pelagic resources (δ13C) but shifted over time to feeding at a higher trophic level (δ15N) and on more marine/offshore resources (δ34S), which correlated with decreases in chlorophyll a concentration. A reduction in Arctic char condition factor and lipid content was associated with higher trophic position. Ringed seals also shifted to feeding at a higher trophic level, but on more pelagic resources, which was associated with lower SST and higher chlorophyll a concentrations. Years with abnormally high SSTs and reduced sea ice concentrations resulted in large isotopic niche sizes for both species, suggesting abrupt change can result in more variable feeding. Changes in abundance and distribution of species long valued by the Inuit of Labrador could diminish food security.

Diagnostic performance of clinical likelihood models of obstructive coronary artery disease to predict myocardial perfusion defects.

AIMS: Clinical likelihood (CL) models are designed based on a reference of coronary stenosis in patients with suspected obstructive coronary artery disease. However, a reference standard for myocardial perfusion defects (MPDs) could be more appropriate. We aimed to investigate the ability of the 2019 European Society of Cardiology pre-test probability (ESC-PTP), the risk-factor-weighted (RF-CL) model, and coronary artery calcium score-weighted (CACS-CL) model to diagnose MPDs. METHODS AND RESULTS: Symptomatic stable de novo chest pain patients (n = 3374) underwent coronary computed tomography angiography and subsequent myocardial perfusion imaging by single-photon emission computed tomography, positron emission tomography, or cardiac magnetic resonance. For all modalities, MPD was defined as coronary computed tomography angiography with suspected stenosis and stress-perfusion abnormality in ≥2 segments. The ESC-PTP was calculated based on age, sex, and symptom typicality, and the RF-CL and CACS-CL additionally included a number of risk factors and CACS. In total, 219/3374 (6.5%) patients had an MPD. Both the RF-CL and the CACS-CL classified substantially more patients to low CL (<5%) of obstructive coronary artery disease compared with the ESC-PTP (32.5 and 54.1 vs. 12.0%, P < 0.001) with preserved low prevalences of MPD (<2% for all models). Compared with the ESC-PTP [area under the receiver-operating characteristic curve (AUC) 0.74 (0.71-0.78)], the discrimination of having an MPD was higher for the CACS-CL model [AUC 0.88 (0.86-0.91), P < 0.001], while it was similar for the RF-CL model [AUC 0.73 (0.70-0.76), P = 0.32]. CONCLUSION: Compared with basic CL models, the RF-CL and CACS-CL models improve down classification of patients to a very low-risk group with a low prevalence of MPD.

A Multi-Matrix Metabolomic Approach in Ringed Seals and Beluga Whales to Evaluate Contaminant and Climate-Related Stressors.

As a high trophic-level species, ringed seals (Pusa hispida) and beluga whales (Delphinapterus leucas) are particularly vulnerable to elevated concentrations of biomagnifying contaminants, such as polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and mercury (Hg). These species also face climate-change-related impacts which are leading to alterations in their diet and associated contaminant exposure. The metabolomic profile of marine mammal tissues and how it changes to environmental stressors is poorly understood. This study characterizes the profiles of 235 metabolites across plasma, liver, and inner and outer blubber in adult ringed seals and beluga whales and assesses how these profiles change as a consequence of contaminants and dietary changes. In both species, inner and outer blubber were characterized by a greater proportion of lipid classes, whereas the dominant metabolites in liver and plasma were amino acids, carbohydrates, biogenic amines and lysophosphatidylcholines. Several metabolite profiles in ringed seal plasma correlated with δ13C, while metabolite profiles in blubber were affected by hexabromobenzene in ringed seals and PBDEs and Hg in belugas. This study provides insight into inter-matrix similarities and differences across tissues and suggests that plasma and liver are more suitable for studying changes in diet, whereas liver and blubber are more suitable for studying the impacts of contaminants.

Contributions and perspectives of Indigenous Peoples to the study of mercury in the Arctic.

Arctic Indigenous Peoples are among the most exposed humans when it comes to foodborne mercury (Hg). In response, Hg monitoring and research have been on-going in the circumpolar Arctic since about 1991; this work has been mainly possible through the involvement of Arctic Indigenous Peoples. The present overview was initially conducted in the context of a broader assessment of Hg research organized by the Arctic Monitoring and Assessment Programme. This article provides examples of Indigenous Peoples' contributions to Hg monitoring and research in the Arctic, and discusses approaches that could be used, and improved upon, when carrying out future activities. Over 40 mercury projects conducted with/by Indigenous Peoples are identified for different circumpolar regions including the U.S., Canada, Greenland, Sweden, Finland, and Russia as well as instances where Indigenous Knowledge contributed to the understanding of Hg contamination in the Arctic. Perspectives and visions of future Hg research as well as recommendations are presented. The establishment of collaborative processes and partnership/co-production approaches with scientists and Indigenous Peoples, using good communication practices and transparency in research activities, are key to the success of research and monitoring activities in the Arctic. Sustainable funding for community-driven monitoring and research programs in Arctic countries would be beneficial and assist in developing more research/monitoring capacity and would promote a more holistic approach to understanding Hg in the Arctic. These activities should be well connected to circumpolar/international initiatives to ensure broader availability of the information and uptake in policy development.

Mercury Isotope Variations in Lake Sediment Cores in Response to Direct Mercury Emissions from Non-Ferrous Metal Smelters and Legacy Mercury Remobilization.

Nature archives record atmospheric mercury (Hg) depositions from directly emitted Hg and re-emitted legacy Hg. Tracing the legacy versus newly deposited Hg is still, however, challenging. Here, we measured Hg isotope compositions in three dated sediment cores at different distances from the Flin Flon smelter, the largest Canadian Hg sources to the atmosphere during the 1930s-2000s. During the smelter's operative period, Hg isotope compositions showed limited variations in the near-field lake (<10 km) sediments but were rather variable in middle- (20-75 km) and far-field lake (∼800 km) sediments. Only the post-2000 sediments in middle/far-field lakes showed significantly negative Hg isotope shifts, while sediments from the 1970s-1990s had Hg isotope values resembling those of near-field lake post-1930 sediments. We suggest that the smelter's peak Hg emissions during the 1970s-1990s, which coincided with the deployment of a super stack in the mid-1970s, largely increased the long-range dispersion of smelter plumes. For the top post-2000 sediments, the fugitive dust from ore tailings and terrestrial legacy Hg re-emissions dominated Hg deposition in near-field lakes and middle/far-field lakes, respectively. Our study demonstrates that legacy Hg remobilization now exports substantial amounts of Hg to ecosystems, highlighting the need for aggressive remediation measures of Hg-contaminated sites.

Climate change and mercury in the Arctic: Abiotic interactions.

Dramatic environmental shifts are occuring throughout the Arctic from climate change, with consequences for the cycling of mercury (Hg). This review summarizes the latest science on how climate change is influencing Hg transport and biogeochemical cycling in Arctic terrestrial, freshwater and marine ecosystems. As environmental changes in the Arctic continue to accelerate, a clearer picture is emerging of the profound shifts in the climate and cryosphere, and their connections to Hg cycling. Modeling results suggest climate influences seasonal and interannual variability of atmospheric Hg deposition. The clearest evidence of current climate change effects is for Hg transport from terrestrial catchments, where widespread permafrost thaw, glacier melt and coastal erosion are increasing the export of Hg to downstream environments. Recent estimates suggest Arctic permafrost is a large global reservoir of Hg, which is vulnerable to degradation with climate warming, although the fate of permafrost soil Hg is unclear. The increasing development of thermokarst features, the formation and expansion of thaw lakes, and increased soil erosion in terrestrial landscapes are increasing river transport of particulate-bound Hg and altering conditions for aquatic Hg transformations. Greater organic matter transport may also be influencing the downstream transport and fate of Hg. More severe and frequent wildfires within the Arctic and across boreal regions may be contributing to the atmospheric pool of Hg. Climate change influences on Hg biogeochemical cycling remain poorly understood. Seasonal evasion and retention of inorganic Hg may be altered by reduced sea-ice cover and higher chloride content in snow. Experimental evidence indicates warmer temperatures enhance methylmercury production in ocean and lake sediments as well as in tundra soils. Improved geographic coverage of measurements and modeling approaches are needed to better evaluate net effects of climate change and long-term implications for Hg contamination in the Arctic.

Metal contamination in alkaline Phantom Lake (Flin Flon, Manitoba, Canada) generates strong responses in multiple paleolimnological proxies.

The copper-zinc smelter at Flin Flon (Manitoba) operated between 1930 and 2010 and emitted large amounts of metal(loid)s and sulphur dioxide into the atmosphere, damaging the surrounding terrestrial landscapes and depositing airborne industrial pollutants into aquatic ecosystems. However, the extent of biological impairment in regional lakes is largely unknown. Here, we analysed biological and geochemical proxies preserved in a dated sediment core from Phantom Lake, collected seven years after the smelter closed in 2010. Our objectives were to determine how smelting history affected long-term trends in (1) sedimentary elements, (2) biota across multiple trophic levels, and (3) spectrally-inferred chlorophyll a and lake-water total organic carbon. The effects of smelting activities were clearest in the diatom record, in concordance with modest responses in chironomid and cladoceran assemblages. Several metal(loid)s were naturally high and exceeded sediment quality guidelines during the pre-smelting era. With the opening of the smelter, metal(loid) concentrations in sediments increased through the 1930s, peaked in the 1960s, and declined thereafter with technological improvements but remained above background to this day. Although modest declines in inferred lake-water total organic carbon indicate reduced terrestrial carbon supply following sulphate deposition in the catchment, the diatom record showed no evidence of acidification as the lake was and remained well-buffered. Pre-smelting diatom and invertebrate assemblages were diverse and indicated oligo-mesotrophic conditions. Smelting was associated with the loss of metal-sensitive biological indicators and the emergence of assemblages dominated by metal-tolerant, generalist taxa. Diatoms tracked substantial reductions in aerial emissions since the 1990s, particularly after the smelter closed, but also indicated that the biological effects of metal pollution persist in Phantom Lake. Examining the effects of a base metal smelter on a well-buffered lake offered insights into multi-trophic level responses to severe metal contamination and potential recovery without the confounding effects of concurrent changes in lake acidity.

Quantification of Spatial and Temporal Trends in Atmospheric Mercury Deposition across Canada over the Past 30 Years.

Mercury (Hg) is a pollutant of concern across Canada and transboundary anthropogenic Hg sources presently account for over 95% of national anthropogenic Hg deposition. This study applies novel statistical analyses of 82 high-resolution dated lake sediment cores collected from 19 regions across Canada, including nearby point sources and in remote regions and spanning a full west-east geographical range of ∼4900 km (south of 60°N and between 132 and 64°W) to quantify the recent (1990-2018) spatial and temporal trends in anthropogenic atmospheric Hg deposition. Temporal trend analysis shows significant synchronous decreasing trends in post-1990 anthropogenic Hg fluxes in western Canada in contrast to increasing trends in the east, with spatial patterns largely driven by longitude and proximity to known point source(s). Recent sediment-derived Hg fluxes agreed well with the available wet deposition monitoring. Sediment-derived atmospheric Hg deposition rates also compared well to the modeled values derived from the Hg model, when lake sites located nearby (<100 km) point sources were omitted due to difficulties in comparison between the sediment-derived and modeled values at deposition "hot spots". This highlights the applicability of multi-core approaches to quantify spatio-temporal changes in Hg deposition over broad geographic ranges and assess the effectiveness of regional and global Hg emission reductions to address global Hg pollution concerns.

Methylmercury Transport and Fate Shows Strong Seasonal and Spatial Variability along a High Arctic Freshwater Hydrologic Continuum.

The presence of toxic methylmercury (MeHg) in Arctic freshwater ecosystems and foodwebs is a potential health concern for northern Indigenous people. Addressing this issue requires a better understanding of MeHg production, fate during transport, and uptake into foodwebs. We used methylation assays and spatiotemporal surveys of MeHg concentrations, during the ice-covered and open water seasons, across a hydrologic continuum (composed of thaw seeps, lake/ponds, and a wetland) to identify Hg methylation hotspots and seasonal differences in MeHg cycling unique to Arctic ecosystems. Ponds and saturated wetland soils support methylation hotspots during the open water season, but subsequent export of MeHg to downstream ecosystems is limited by particle settling, binding of MeHg on soil organic matter, and/or demethylation in drier wetland soils. During the ice-covered season, MeHg concentrations in lake waters were approximately ten-fold greater than in summer; however, zooplankton MeHg concentrations were paradoxically five times lower at this time. Despite limited evidence of snow-phase methylation, the snowpack is an important MeHg reservoir. Changes in ice-cover duration will alter MeHg production and bioaccumulation in lakes, while increased thaw and surface water flow will likely result in higher methylation rates at the aquatic-terrestrial interface and more efficient downstream transport of MeHg.

Long-term spatial and temporal trends, and source apportionment of polycyclic aromatic compounds in the Athabasca Oil Sands Region.

We investigated the spatio-temporal trends of polycyclic aromatic compounds (PACs) deposition in the Athabasca Oil Sands Region (AOSR) between 2008 and 2017, and applied source apportionment tools to assess sources using snowpacks. Estimated PAC mass deposition was significantly correlated with crude oil production (R2 = 0.48, p = 0.03), and increased between 2008 and 2017. Loadings of alkylated PACs c1-, c2-fluorenes/pyrenes and c1-, c3-benzo[a]anthracenes/chrysenes/triphenylenes significantly increased at mid-field sites (25-50 km from central industrial reference site, AR6) (Mann-Kendall, p < 0.05) reflecting physical expansion of the AOSR. The distance from emission sources was important in the deposition of PACs, including the distance from AR6 (R2 = 0.69-0.91), nearest petcoke storage (R2 = 0.77-0.88), 0.89) and upgrader stack (R2 = 0.56-0.61). Source apportionment PAC distribution profiles of the source materials (petcokes, oil sand ores, road dust) did not show unique matching profiles with the snowpacks. However, the minimal presence of retene in petcokes and an abundance of benzo[ghi]fluoranthene in road dust was observed, and suggests potential for these compounds as chemical markers in distinguishing sources. Furthermore, correlations between PACs and selected metal(loid)s in the AOSR snowpacks were assessed to infer potential common sources. Significant positive (p < 0.05) correlations between metal(loid)s enriched in bitumen (vanadium, molybdenum, nickel) and PACs, at near to mid-field (0-50 km from AR6) sites suggests common sources or similar transfer and fate processes. The results of our study convey data necessary for monitoring studies in the constantly developing AOSR, advance our knowledge of PACs profiles in source materials (including the much less studied alkylated PACs and dibenzothiophenes), which will be valuable for other studies related to oil pollution, urban run-off and forest fires. PACs mass deposition increasing between 2008 and 2017 coincident with crude oil production, and retene and benzo[ghi]fluoranthene show potential in distinguishing AOSR sources.

Atmospheric trace metal deposition to remote Northwest Ontario, Canada: Anthropogenic fluxes and inventories from 1860 to 2010.

National and global inventories of anthropogenic trace element emissions to air is a comparatively recent phenomenon (post-1993 in Canada) as is the monitoring of atmospheric metal deposition, the latter being also very spatially limited. Paleo-reconstructive methods offer a contiguous record of environmental contamination providing a needed framework to establish locally relevant "pre-industrial" (~natural) conditions which can be compare with relative and quantitative deviations away from reference conditions. In this study, we reconstruct the history of the long-range, anthropogenic sourced atmospheric trace element deposition to the remote region of Northwestern Ontario Canada (Experimental Lakes Area (ELA)) using dated sediment records from five lakes. Several elements are shown to be highly enriched in lake sediments relative to pre-1860 sediments (Antimony, Lead, Tellurium, Tin, Arsenic, Bismuth, Cadmium and Mercury) and moderately (Zinc, Tungsten, Thallium, Copper, Silver, Selenium, Nickel and Vanadium). Mean decadal anthropogenic atmospheric fluxes (mg m-2 yr-1) are reconstructed for 1860-2010 and compare well with available local (ELA), regional (NW Ontario Canada, N Michigan USA) monitoring data, as well as global assessments of anthropogenic contribution to atmospheric trace metal burdens. Quantitative paleo reconstructions of atmospheric contamination history using the collective signal from multiple lakes provide a rigorous methodology to assess trends, uncertainties, evaluation with monitoring data and, provide an opportunity to explore landscape processes of contaminant transport and storage. Further study of the latter is recommended to understand the latency of legacy anthropogenic contamination of the environment.

The distribution and transport of lead over two centuries as recorded by lake sediments from northeastern North America.

We evaluated anthropogenic Pb deposition along a west-east transect from the Adirondack Mountains, New York, USA (ADIR) region, the Vermont-New Hampshire-Maine, USA (VT-NH-ME) region, and Nova Scotia, Canada (NS) region using 47 210Pb-dated lake sediment records. We used focus-corrected Pb inventories to evaluate cumulative deposition and breakpoint analysis to evaluate possible differences in timings among regions. Peak Pb concentrations decreased from west to east (ADIR region: 52-378 mg kg-1, VT-NH-ME region: 54-253 mg kg-1, NS: 38-140 mg kg-1). Cumulative deposition of anthropogenic Pb also decreased from west to east (ADIR region: 791-1344 mg m-2, VT-NH-ME region: 209-1206 mg m-2, NS: 52-421 mg m-2). The initiation of anthropogenic Pb deposition occurred progressively later along the same transect (ADIR region: 1869-1900, VT-NH-ME region: 1874-1905, NS region: 1901-1930). Previous lead isotope studies suggest that eastern Canadian Pb deposition over the past ~150 years has originated from a mix of both Canadian and U.S. sources. The results of this study indicate that anthropogenic Pb from sources west of the ADIR region were deposited in lesser amounts from west to east and/or Pb sources reflect less population density from west to east. The timing of the initiation of anthropogenic Pb deposition in the NS region suggests that Pb from gasoline may be an important source in this region.

A one-century sedimentary record of N- and S-polycyclic aromatic compounds in the Athabasca oil sands region in Canada.

The atmospheric deposition of polycyclic aromatic compounds (PACs) is considered a major pathway to isolated lakes and bogs in the Athabasca oil sands region (AOSR), Canada. However, the suite of PACs measured has been limited. We report the detailed depositional history of nitrogen and sulphur heterocyclic PACs using a 210Pb dated sediment core (1914-2015) near major developments in the AOSR. We observed (1) an exponential growth in the deposition of heterocyclic PACs to recent times with an average doubling time of 12 years, (2) significant breakpoints in PAC fluxes in the mid to late 1980s, and (3) a synchronous increase of PACs with crude oil production (r2 = 0.82, p = 0.001). NPACs were not detected prior to the 1960s in the sediment core studied, suggesting they may hold promise in serving as indicators for atmospheric PAC deposition of industrial origin. Furthermore, a change in heterocyclic PAC distribution profiles beginning in the 1970-1980s, after the onset of mining, resembling a petcoke signature, was also observed. Significant positive correlations (p < 0.05) were observed between heterocyclic PACs, and several metal(loid)s, including priority pollutant elements, chromium and beryllium, and rare earth elements, cerium, lanthanum and yttrium (r2 > 0.75), suggesting the potential of a common source or similar transport and fate mechanisms. Significant negative or no correlations were observed between heterocyclic PACs and other metal(loid)s, including vanadium, total mercury and lead, possibly reflecting the impact of broader regulatory controls introduced in the mid-1970s on some metal(loids) but not on PACs, including the installation of electrostatic precipitators in major upgrader stacks.

Sources of atmospheric metal(loid) pollution recorded in Thompson Manitoba lake sediment cores within the Canadian boreal biome.

Global atmospheric emissions and subsequent deposition of numerous metal(loid)s has increased markedly since the industrial revolution. Due to a paucity of long-term metal(loid) flux measurements, the magnitude and timing of change are largely unknown, resulting in limited ability to predict time-scales of ecosystem recovery in response to emission decreases. In the absence of long-term data, palaeo-reconstructions provide continuous records of atmospheric metal(loid) deposition on an ecosystem, and landscape, scale. Here, we use high-resolution dated lake sediment cores to reconstruct the last c. 100 years of atmospheric anthropogenic deposition of a full suite (40) of metal(loid)s near a large nickel (Ni) and copper (Cu) smelter in an other-wise largely "pristine" region of northern Canada (Thompson, Manitoba). Anthropogenic depositional fluxes were compared to other regions of Canada including Kejimkujik National Park in Nova Scotia, Experimental Lakes Area in Ontario, as well as the Flin Flon, Manitoba Cu and zinc (Zn) smelter, located ~200 km southwest of Thompson. Deposition of 12 metal(loid)s were enriched above baseline (pre-1915) levels: antimony (Sb) > palladium (Pd) > bismuth (Bi) > mercury (Hg) > cadmium (Cd) > Ni > lead (Pb) > arsenic (As) > strontium (Sr) > Cu > platinum (Pt) > Zn. Spatio-temporal patterns in depositional fluxes and inventories demonstrate that 6 of these metal(loid)s were sourced primarily from the smelter, while As, Hg, Pb, Pt, Sb and Zn were sourced primarily from global and/or regional sources. Comparison of anthropogenic fluxes and inventories to available emissions data showed that Cu and Ni deposition has plateaued since the late 1970s despite dramatic smelter emission decreases between 2005 and 2014. We hypothesize that this discrepancy is due to releases of terrestrial metal(loid)s by climate-driven permafrost degradation, which is widespread across the region and will likely continue to drive increased metal(loid) fluxes to northern Canadian lakes for unknown time-scales.

Accumulating Mercury and Methylmercury Burdens in Watersheds Impacted by Oil Sands Pollution.

Bitumen mining and upgrading in northeastern Alberta, Canada, releases toxic pollutants into the atmosphere, including mercury (Hg) and methylmercury (MeHg). This Hg and MeHg is then deposited to the surrounding landscape; however, the fate of these contaminants remains unknown. Here, we compare snowpack chemistry to high-frequency measurements of river water quality across six watersheds (five impacted by oil sands development and one unimpacted). Catchment scale snowpack Hg and MeHg loads normalized to watershed area were highest near oil sands operations. River water Hg concentrations and loads tracked discharge and tended to be higher downstream of mining operations, while MeHg concentrations and loads increased through the summer, reflecting peak summer MeHg production rates. Except in the reference watershed, snowpack Hg and MeHg loads equaled or exceeded the amount of Hg and MeHg exported during freshet and, in some cases, the entire hydrologic year. This suggests landscapes across the oil sands region, which are dominated by low-relief wetlands and other shallow-water systems, are accumulating Hg and MeHg. Importantly, during years of high discharge, these low-relief systems appear to become better connected and flush MeHg (and Hg) from the watershed. Thus, these watersheds may act as temporary, rather than as permanent, natural repositories of oil sands contaminants.

Danish study of Non-Invasive testing in Coronary Artery Disease 2 (Dan-NICAD 2): Study design for a controlled study of diagnostic accuracy.

BACKGROUND: Coronary computed tomography angiography (CTA) is the preferred primary diagnostic modality when examining patients with low to intermediate pre-test probability of coronary artery disease (CAD). Only 20-30% of these have potentially obstructive CAD. Because of the relatively poor positive predictive value of coronary CTA, unnecessary invasive coronary angiographies (ICAs) are conducted with the costs and risks associated with the procedure. Hence, an optimized diagnostic CAD algorithm may reduce the numbers of ICAs not followed by revascularization. The Dan-NICAD 2 study has 3 equivalent main aims: (1) To examine the diagnostic precision of a sound-based diagnostic algorithm, The CADScor®System (Acarix A/S, Denmark), in patients with a low to intermediate pre-test risk of CAD referred to a primary examination by coronary CTA. We hypothesize that the CADScor®System provides better stratification prior to coronary CTA than clinical risk stratification scores alone. (2) To compare the diagnostic accuracy of 3T cardiac magnetic resonance imaging (3T CMRI), 82rubidium positron emission tomography (82Rb-PET), and CT-derived fractional flow reserve (FFRCT) in patients where obstructive CAD cannot be ruled out by coronary CTA using ICA fractional flow reserve (FFR) as reference standard. (3) To compare the diagnostic performance of quantitative flow ratio (QFR) and ICA-FFR in patients with low to intermediate pre-test probability of CAD using 82Rb-PET as reference standard. METHODS: Dan-NICAD 2 is a prospective, multicenter, cross-sectional study including approximately 2,000 patients with low to intermediate pre-test probability of CAD and without previous history of CAD. Patients are referred to coronary CTA because of symptoms suggestive of CAD, as evaluated by a cardiologist. Patient interviews, sound recordings, and blood samples are obtained in connection with the coronary CTA. If coronary CTA does not rule out obstructive CAD, patients will be examined by 3T CMRI 82Rb-PET, FFRCT, ICA, and FFR. Reference standard is ICA-FFR. Obstructive CAD is defined as an FFR ≤0.80 or as high-grade stenosis (>90% diameter stenosis) by visual assessment. Diagnostic performance will be evaluated as sensitivity, specificity, predictive values, likelihood ratios, calibration, and discrimination. Enrolment started January 2018 and is expected to be completed by June 2020. Patients are followed for 10 years after inclusion. DISCUSSION: The results of the Dan-NICAD 2 study are expected to contribute to the improvement of diagnostic strategies for patients suspected of CAD in 3 different steps: risk stratification prior to coronary CTA, diagnostic strategy after coronary CTA, and invasive wireless QFR analysis as an alternative to ICA-FFR.

Athabasca oil sands region snow contains efficient micron and nano-sized ice nucleating particles.

The Athabasca Oil Sands Region (AOSR) in Alberta, Canada, is an important source of atmospheric pollutants, such as aerosols, that have repercussions on both the climate and human health. We show that the mean freezing temperature of snow-borne particles from AOSR was elevated (-7.1 ±â€¯1.8 °C), higher than mineral dust which freezes at ∼ -15 °C and is recognized as one of the most relevant ice nuclei globally. Ice nucleation of nanosized snow samples indicated an elevated freezing ability (-11.6 ±â€¯2.0 °C), which was statistically much higher than snow-borne particles from downtown Montreal. AOSR snow had a higher concentration (∼2 orders of magnitude) of >100 nm particles than Montreal. Triple quadrupole ICP-(QQQ)-MS/MS analysis of AOSR and Montreal snow demonstrated that most concentrations of metals, including those identified as emerging nanoparticulate contaminants, were much more elevated in AOSR in contrast to Montreal: 34.1, 34.1, 16.6, 5.8, 0.3, 0.1, and 9.4 mg/m3 for Cr, Ni, Cu, As, Se, Cd, and Pb respectively, in AOSR and 1.3, 0.3, 2.0, <0.03, 0.1, 0.03, and 1.2 mg/m3 in Montreal snow. High-resolution Scanning Transmission Electron Microscopy/Energy-dispersive X-ray Spectroscopy (STEM-EDS) imaging provided evidence for various anthropogenic nano-materials, including carbon nanotubes resembling structures, in AOSR snow up to 7-25 km away from major oil sands upgrading facilities. In summary, particles characterized as coming from oil sands are more efficient at ice nucleation. We discuss the potential impacts of AOSR emissions on atmospheric and microphysical processes (ice nucleation and precipitation) both locally and regionally.