ALBERT

Description: Passive air samplers (PASs) for gaseous mercury (Hg) were deployed for time periods between 1 month and 1 year at 20 sites across the globe with continuous atmospheric Hg monitoring using active Tekran instruments. The purpose was to evaluate the accuracy of the PAS vis-à-vis the industry standard active instruments and to determine a sampling rate (SR; the volume of air stripped of gaseous Hg per unit of time) that is applicable across a wide range of conditions. The sites spanned a wide range of latitudes, altitudes, meteorological conditions, and gaseous Hg concentrations. Precision, based on 378 replicated deployments performed by numerous personnel at multiple sites, is 3.6 ± 3.0 %1, confirming the PAS's excellent reproducibility and ease of use. Using a SR previously determined at a single site, gaseous Hg concentrations derived from the globally distributed PASs deviate from Tekran-based concentrations by 14.2 ± 10 %. A recalibration using the entire new data set yields a slightly higher SR of 0.1354 ± 0.016 m3 day−1. When concentrations are derived from the PAS using this revised SR the difference between concentrations from active and passive sampling is reduced to 8.8 ± 7.5 %. At the mean gaseous Hg concentration across the study sites of 1.54 ng m−3, this represents an ability to resolve concentrations to within 0.13 ng m−3. Adjusting the sampling rate to deployment specific temperatures and wind speeds does not decrease the difference in active–passive concentration further (8.7 ± 5.7 %), but reduces its variability by leading to better agreement in Hg concentrations measured at sites with very high and very low temperatures and very high wind speeds. This value (8.7 ± 5.7 %) represents a conservative assessment of the overall uncertainty of the PAS due to inherent uncertainties of the Tekran instruments. Going forward, the recalibrated SR adjusted for temperature and wind speed should be used, especially if conditions are highly variable or deviate considerably from the average of the deployments in this study (9.89 ∘C, 3.41 m s−1). Overall, the study demonstrates that the sampler is capable of recording background gaseous Hg concentrations across a wide range of environmental conditions with accuracy similar to that of industry standard active sampling instruments. Results at sites with active speciation units were inconclusive on whether the PASs take up total gaseous Hg or solely gaseous elemental Hg primarily because gaseous oxidized Hg concentrations were in a similar range as the uncertainty of the PAS.

Description: Reports of abruptly declining flows of Canada's Athabasca River have prompted concern because this large, free-flowing river could be representative for northern North America, provides water for the massive Athabasca oil-sands projects and flows to the extensive and biodiverse Peace-Athabasca, Slave and Mackenzie River deltas. To investigate historic hydrology along the river and its major tributaries, we expanded the time series with interpolations for short data gaps; calculations of annual discharges from early, summer-only records; and by splicing records across sequential hydrometric gauges. These produced composite, century-long records (1913-2011) and trend detection with linear Pearson correlation provided similar outcomes to nonparametric Kendall τ-b tests. These revealed that the mountain and foothills reaches displayed slight increases in winter discharges versus larger declines in summer discharges and consequently declining annual flows (~0.16% per year at Hinton; p〈0.01). Conversely, with contrasting boreal contributions, the Athabasca River at Athabasca displayed no overall trend in monthly or annual flows, but there was correspondence with the Pacific Decadal Oscillation that contributed to a temporary flow decline from 1970 to 2000. These findings from century-long records contrast with interpretations from numerous shorter-term studies and emphasize the need for sufficient time series for hydrologic trend analyses. For Northern Hemisphere rivers, the study interval should be at least 80years to span two Pacific Decadal Oscillation cycles and dampen the influence from phase transitions. Most prior trend analyses considered only a few decades, and this weakens interpretations of the hydrologic consequences of climate change. © 2014 John Wiley & Sons, Ltd.

Description: Passive air samplers (PASs) for gaseous mercury (Hg) were deployed for time periods between 1 month and 1 year at 20 sites across the globe with continuous atmospheric Hg monitoring using active Tekran instruments. The purpose was to evaluate the accuracy of the PAS vis-à-vis the industry standard active instruments and to determine a sampling rate (SR; the volume of air stripped of gaseous Hg per unit of time) that is applicable across a broad variety of conditions. The sites spanned a wide range of latitudes, altitudes, meteorological conditions, and gaseous Hg concentrations. Precision, based on 378 replicated deployments performed by numerous personnel at multiple sites, is 3.6 ± 3.0 %*, confirming the PAS's excellent reproducibility and ease-of-use. Using a SR previously determined at a single site, gaseous Hg concentrations derived from the globally distributed PASs deviate from Tekran-based concentrations by 14.2 ± 10 %. A recalibration using the entire new data set yields a slightly higher SR of 0.1354 ± 0.016 m3 day−1. When concentrations are derived from the PAS using this revised SR the difference is reduced to 8.8 ± 7.5 %. At the mean gaseous Hg concentration across the study sites of 1.54 ng m−3, this represents an ability to resolve concentrations to within 0.13 ng m−3. Adjusting the sampling rate to deployment specific temperatures and wind speeds does not decrease the difference in active–passive concentration further (8.7 ± 5.7 %), but reduces its variability by leading to better agreement in Hg concentrations measured at sites with very high and very low temperatures and very high wind speeds. This value (8.7 ± 5.7 %) represents a conservative assessment of the overall uncertainty of the PAS due to inherent uncertainties of the Tekran instruments. Going forward, the recalibrated SR adjusted for temperature and wind speed should be used, especially if conditions are highly variable or deviate considerably from the average of the deployments in this study (9.89 °C, 3.41 m s−1). Overall, the study demonstrates that the sampler is capable of recording background gaseous Hg concentrations across a wide range of environmental conditions with accuracy similar to that of industry standard active sampling instruments. Results at sites with active speciation units were inconclusive on whether the PASs take up total gaseous Hg or solely gaseous elemental Hg primarily because gaseous oxidized Hg concentrations were in a similar range as the uncertainty of the PAS.

Description: Emissions from biomass burning are an important source of mercury (Hg) to the atmosphere and an integral component of the global Hg biogeochemical cycle. In 2018, measurements of gaseous elemental Hg (GEM) were taken on board a research aircraft along with a series of co-emitted contaminants in the emissions plume of an 88 km2 boreal forest wildfire on the Garson Lake Plain (GLP) in NW Saskatchewan, Canada. A series of four flight tracks were made perpendicular to the plume at increasing distances from the fire, each with three to five passes at different altitudes at each downwind location. The maximum GEM concentration measured on the flight was 2.88 ng m−3, which is ≈ 2.4× background concentration. GEM concentrations were significantly correlated with the co-emitted carbon species (CO, CO2, and CH4). Emissions ratios (ERs) were calculated from measured GEM and carbon co-contaminant data. Using the most correlated (least uncertain) of these ratios (GEM:CO), GEM concentrations were estimated at the higher 0.5 Hz time resolution of the CO measurements, resulting in maximum GEM concentrations and enhancements of 6.76 ng m−3 and ≈ 5.6×, respectively. Extrapolating the estimated maximum 0.5 Hz GEM concentration data from each downwind location back to source, 1 km and 1 m (from fire) concentrations were predicted to be 12.9 and 30.0 ng m−3, or enhancements of ≈ 11× and ≈ 25×, respectively. ERs and emissions factors (EFs) derived from the measured data and literature values were also used to calculate Hg emissions estimates on three spatial scales: (i) the GLP fires themselves, (ii) all boreal forest biomass burning, and (iii) global biomass burning. The most robust estimate was of the GLP fires (21 ± 10 kg of Hg) using calculated EFs that used minimal literature-derived data. Using the Top-down Emission Rate Retrieval Algorithm (TERRA), we were able to determine a similar emission estimate of 22 ± 7 kg of Hg. The elevated uncertainties of the other estimates and high variability between the different methods used in the calculations highlight concerns with some of the assumptions that have been used in calculating Hg biomass burning in the literature. Among these problematic assumptions are variable ERs of contaminants based on vegetation type and fire intensity, differing atmospheric lifetimes of emitted contaminants, the use of only one co-contaminant in emissions estimate calculations, and the paucity of atmospheric Hg species concentration measurements in biomass burning plumes.