Gaseous elemental mercury (Hg0) is a globally distributed air toxin with a long atmospheric residence time. Any process that reduces its atmospheric lifetime increases its potential accumulation in the biosphere. Our data from Barrow, AK, at 71 degrees N show that rapid, photochemically driven oxidation of boundary-layer Hg0 after polar sunrise, probably by reactive halogens, creates a rapidly depositing species of oxidized gaseous mercury in the remote Arctic troposphere at concentrations in excess of 900 pg m(-3). This mercury accumulates in the snowpack during polar spring at an accelerated rate in a form that is bioavailable to bacteria and is released with snowmelt during the summer emergence of the Arctic ecosystem. Evidence suggests that this is a recent phenomenon that may be occurring throughout the earth's polar regions.
Atmospheric mercury is predominantly present in the gaseous elemental form (Hg0). However, anthropogenic emissions (e.g., incineration, fossil fuel combustion) emit and natural processes create particulate-phase mercury(Hg(p)) and divalent reactive gas-phase mercury (RGM). RGM species (e.g., HgCl2, HgBr2) are water-soluble and have much shorter residence times in the atmosphere than Hg0 due to their higher removal rates through wet and dry deposition mechanisms. Manual and automated annular denuder methodologies, to provide high-resolution (1-2 h) ambient RGM measurements, were developed and evaluated. Following collection of RGM onto KCl-coated quartz annular denuders, RGM was thermally decomposed and quantified as Hg0. Laboratory and field evaluations of the denuders found the RGM collection efficiency to be >94% and mean collocated precision to be <15%. Method detection limits for sampling durations ranging from 1 to 12 h were 6.2-0.5 pg m(-3), respectively. As part of this research, the authors observed that methods to measure Hg(p) had a significant positive artifact when RGM coexists with Hg(p). This artifact was eliminated if a KCl-coated annular denuder preceded the filter. This new atmospheric mercury speciation methodology has dramatically enhanced our ability to investigate the mechanisms of transformation and deposition of mercury in the atmosphere.
Background:The increasing size and frequency of wildland fires are leading to greater potential for cardiopulmonary disease and cancer in exposed populations; however, little is known about how the types of fuel and combustion phases affect these adverse outcomes.Objectives:We evaluated the mutagenicity and lung toxicity of particulate matter (PM) from flaming vs. smoldering phases of five biomass fuels, and compared results by equal mass or emission factors (EFs) derived from amount of fuel consumed.Methods:A quartz-tube furnace coupled to a multistage cryotrap was employed to collect smoke condensate from flaming and smoldering combustion of red oak, peat, pine needles, pine, and eucalyptus. Samples were analyzed chemically and assessed for acute lung toxicity in mice and mutagenicity in Salmonella.Results:The average combustion efficiency was 73 and 98% for the smoldering and flaming phases, respectively. On an equal mass basis, PM from eucalyptus and peat burned under flaming conditions induced significant lung toxicity potencies (neutrophil/mass of PM) compared to smoldering PM, whereas high levels of mutagenicity potencies were observed for flaming pine and peat PM compared to smoldering PM. When effects were adjusted for EF, the smoldering eucalyptus PM had the highest lung toxicity EF (neutrophil/mass of fuel burned), whereas smoldering pine and pine needles had the highest mutagenicity EF. These latter values were approximately 5, 10, and 30 times greater than those reported for open burning of agricultural plastic, woodburning cookstoves, and some municipal waste combustors, respectively.Conclusions:PM from different fuels and combustion phases have appreciable differences in lung toxic and mutagenic potency, and on a mass basis, flaming samples are more active, whereas smoldering samples have greater effect when EFs are taken into account. Knowledge of the differential toxicity of biomass emissions will contribute to more accurate hazard assessment of biomass smoke exposures. https://doi.org/10.1289/EHP2200
Abstract. Low-cost particulate matter (PM) sensors are promising tools for supplementing existing air quality monitoring networks. However, the performance of the new generation of low-cost PM sensors under field conditions is not well understood. In this study, we characterized the performance capabilities of a new low-cost PM sensor model (Plantower model PMS3003) for measuring PM 2.5 at 1 min, 1 h, 6 h, 12 h, and 24 h integration times. We tested the PMS3003 sensors in both low-concentration suburban regions (Durham and Research Triangle Park (RTP), NC, US) with 1 h PM 2.5 (mean ± SD) of 9 ± 9 and 10 ± 3 µg m −3 , respectively, and a high-concentration urban location (Kanpur, India) with 1 h PM 2.5 of 36 ± 17 and 116 ± 57 µg m −3 during monsoon and post-monsoon seasons, respectively. In Durham and Kanpur, the sensors were compared to a research-grade instrument (environmental β attenuation monitor, E-BAM) to determine how these sensors perform across a range of PM 2.5 concentrations and meteorological factors (e.g., temperature and relative humidity, RH). In RTP, the sensors were compared to three Federal Equivalent Methods (FEMs) including two Teledyne model T640s and a Thermo Scientific model 5030 SHARP to demonstrate the importance of the type of reference monitor selected for sensor calibration. The decrease in 1 h mean errors of the calibrated sensors using univariate linear models from Durham (201 %) to Kanpur monsoon (46 %) and post-monsoon (35 %) seasons showed that PMS3003 performance generally improved as ambient PM 2.5 increased. The precision of reference instruments (T640: ±0.5 µg m −3 for 1 h; SHARP: ±2 µg m −3 for 24 h, better than the E-BAM) is critical in evaluating sensor performance, and β-attenuation-based monitors may not be ideal for testing PM sensors at low concentrations, as underscored by (1) the less dramatic error reduction over averaging times in RTP against optically based T640 (from 27 % for 1 h to 9 % for 24 h) than in Durham (from 201 % to 15 %); (2) the lower errors in RTP than the Kanpur post-monsoon season (from 35 % to 11 %); and (3) the higher T640-PMS3003 correlations (R 2 ≥ 0.63) than SHARP-PMS3003 (R 2 ≥ 0.25). A major RH influence was found in RTP (1 h RH = 64 ± 22 %) due to the relatively high precision of the T640 measurements that can explain up to ∼ 30 % of the variance in 1 min to 6 h PMS3003 PM 2.5 measurements. When proper RH corrections are made by empirical nonlinear equations after using a more precise reference method to calibrate the sensors, our work suggests that the PMS3003 sensors can measure PM 2.5 concentrations within ∼ 10 % of ambient values. We observed that PMS3003 sensors appeared to exhibit a nonlinear response when ambient PM 2.5 exceeded ∼ 125 µg m −3 and found that the quadratic fit is more appropriate than the univariate linear model to capture this nonlinearity and can further reduce errors by up to 11 %. Our results have substantial implications for how variability in ambient PM 2.5 concentrations, reference monitor types, and meteorologi...
Long-term monitoring of data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (http://www.gmos.eu) and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere as well as in the lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010-2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both.
Wet and dry mercury (Hg) deposition were calculated to Lake Michigan using a hybrid receptor modeling framework. The model utilized mercury monitoring data collected during the Lake Michigan Mass Balance Study and the Atmospheric Exchange Over Lakes and Oceans Studytogether with high-resolution over-water meteorological date provided by the National Oceanic and Atmospheric Administration (July, 1994-October, 1995). Atmospheric deposition was determined to be the primary pathway for mercury inputto Lake Michigan, contributing approximately 84% of the estimated 1403 kg total annual input (atmospheric deposition + tributary input). Wet (10.6 microg m(-2)) and dry deposition (9.7 microg m(-2)) contributed almost equally to the annual atmospheric Hg deposition of 20.3 microg m(-2) (1173 kg). Re-emission of dissolved gaseous Hg from the lake was also significant (7.8 microg m(-2)), reducing the net atmospheric deposition to 12.5 microg m(-2) (720 kg). A strong urban influence was observed in the over-water mercury deposition estimates in the southern portion of the lake. The Chicago/Gary urban area was estimated to contribute approximately 20% (127 kg) of the annual atmospheric mercury deposition to Lake Michigan. The magnitude of local anthropogenic mercury sources in the Chicago/Gary urban area suggests that emission reductions could significantly reduce atmospheric mercury deposition into Lake Michigan.
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