Development of a reduced speciated VOC degradation mechanism for use in ozone models

A reduced mechanism to describe the formation of ozone from VOC oxidation has been developed, using the master chemical mechanism (MCM v2) as a reference benchmark. The ‘common representative intermediates’ (CRI) mechanism treats the degradation of methane and 120 VOC using ca. 570 reactions of ca. 250 species (i.e. the emitted VOC plus an average of about one additional species per VOC). It thus contains only ca. 5% of the number of reactions and ca. 7% of the number of chemical species in MCM v2, providing a computationally economical alternative. The CRI mechanism contains a series of generic intermediate radicals and products, which mediate the breakdown of larger VOC into smaller fragments (e.g., formaldehyde), the chemistry of which is treated explicitly. A key assumption in the mechanism construction methodology is that the potential for ozone formation from a given VOC is related to the number of reactive (i.e., C–C and C–H) bonds it contains, and it is this quantity which forms the basis of the generic intermediate groupings. Following a small degree of optimisation, the CRI mechanism is shown to generate levels of ozone, OH, peroxy radicals, NO and NO₂ which are in excellent agreement with those calculated using MCM v2, in simulations using a photochemical trajectory model applied previously to simulation of episodic ozone formation. The same model is used to calculate photochemical ozone creation potentials for 63 alkanes, alkenes, carbonyls and alcohols using both mechanisms. Those determined with the CRI mechanism show a variation from compound to compound which is remarkably consistent with that calculated with the detailed chemistry in MCM v2. This suggests that the CRI mechanism construction methodology is able to capture both the salient features of the ozone formation process in general, and how this varies from one VOC to another.     

Simulation of global warming potential (GWP) from rice fields in the Tai-Lake region,China by coupling 1:50,000 soil database with DNDC model

Quantifying greenhouse gas (GHG) emissions from wetland ecosystems is a relatively new issue in global climate change studies. China has approximately 22% of the world's rice paddies and 38% of the world's rice production, which are crucial to accurately estimate the global warming potential (GWP) at regional scale. This paper reports an application of a biogeochemical model (DeNitrification and DeComposition or DNDC) for quantifying GWP from rice fields in the Tai-Lake region of China. For this application, DNDC is linked to a 1:50,000 soil database, which was derived from 1107 paddy soil profiles compiled during the Second National Soil Survey of China in the 1980–1990s. The simulated results show that the 2.34 Mha of paddy soil cultivated in rice–wheat rotation in the Tai-Lake region emitted about ?1.48 Tg C, 0.84 Tg N and 5.67 Tg C as CO₂, N₂O, and CH₄ respectively, with a cumulative GWP of 565 Tg CO₂ equivalent from 1982 to 2000. As for soil subgroups, the highest GWP (26,900 kg CO₂ equivalent ha^?1 yr^?1) was linked to gleyed paddy soils accounting for about 4.4% of the total area of paddy soils. The lowest GWP (5370 kg CO₂ equivalent ha^?1 yr^?1) was associated with submergenic paddy soils accounting for about 0.32% of the total area of paddy soils. The most common soil in the area was hydromorphic paddy soils, which accounted for about 53% of the total area of paddy soils with a GWP of 12,300 kg CO₂ equivalent ha^?1 yr^?1. On a regional basis, the annual averaged GWP in the polder, Tai-Lake plain, and alluvial plain soil regions was distinctly higher than that in the low mountainous and Hilly soil regions. As for administrative areas, the average annual GWP of counties in Shanghai city was high. Conversely, the average annual GWP of counties in Jiangsu province was low. The high variability in soil properties throughout the Tai-Lake region is important and affects the net greenhouse gas emissions. Therefore, the use of detailed soil data sets with high-resolution digital soil maps is essential to improve the accuracy of GWP estimates with process-based models at regional and national scales.     

Effects of Constant versus Diurnally-Varying Light Intensity on Ozone Formation

Abstract

1-Bromo-propane (1-BP) is a replacement for high-end chlorofluorocarbon (HCFC) solvents. Its reaction rate constant with the OH radical is, on a weight basis, significantly less than that of ethane. However, the overall smog formation chemistry of 1-BP appears to be very unusual compared with typical volatile organic compounds (VOCs) and relatively complex because of the presence of bromine. In smog chamber experiments, 1-BP initially shows a faster ozone build-up than what would be expected from ethane, but the secondary products containing bromine tend to destroy ozone such that 1-BP can have a net overall negative reactivity. Alternative sets of reactions are offered to explain this unusual behavior. Follow-up studies are suggested to resolve the chemistry. Using one set of bromine-related reactions in a photo-chemical grid model shows that 1-BP would be less reactive toward peak ozone formation than ethane with a trend toward even lower ozone impacts in the future.     

The ozone formation potential of 1-bromo-propane

1-Bromo-propane (1-BP) is a replacement for high-end chlorofluorocarbon (HCFC) solvents. Its reaction rate constant with the OH radical is, on a weight basis, significantly less than that of ethane. However, the overall smog formation chemistry of 1-BP appears to be very unusual compared with typical volatile organic compounds (VOCs) and relatively complex because of the presence of bromine. In smog chamber experiments, 1-BP initially shows a faster ozone build-up than what would be expected from ethane, but the secondary products containing bromine tend to destroy ozone such that 1-BP can have a net overall negative reactivity. Alternative sets of reactions are offered to explain this unusual behavior. Follow-up studies are suggested to resolve the chemistry. Using one set of bromine-related reactions in a photochemical grid model shows that 1-BP would be less reactive toward peak ozone formation than ethane with a trend toward even lower ozone impacts in the future.     

Impact of biogenic VOC emissions on a tropical cyclone-related ozone episode in the Pearl River Delta region,China

For quantitative estimate of biogenic volatile organic compound emissions (BVOCs) in South China and their impact on the regional atmospheric chemistry, a 3-day tropical cyclone-related ozone episode was modeled using chemical transport model CMAQ, which was driven by the mesoscale meteorological model MM5. Hourly biogenic emission inventories were constructed using the Sparse Matrix Operator Kernel Emissions (SMOKE) model. The simulation results show good agreement with observation data in air temperature, ozone and NO_x levels. The estimated biogenic emissions of isoprene, terpene, and other reactive VOCs (ORVOCs) during this tropical cyclone-related episode are 8500, 3400, and 11 300 ton day⁻¹, respectively. The ratio of isoprene to the total BVOCs was 36.4%. Two test runs were carried out with one incorporated biogenic emissions and the other without. The simulations show that Guangdong province, particularly the Pearl River Delta (PRD) region, was the area most reactive to biogenic emissions in South China. More ozone was produced in all layers under 1500 m when biogenic emissions were included in comparison to that without BVOCs. The net formation of ozone from 9:00 to 15:00 h was the highest near the surface and could reach 38 ppb, which include 4 ppb attributed to biogenic impact. The enhanced ozone due to biogenic emissions first appeared in the PRD region and slowly spread to a greater area in South China. Process analysis indicated that the surface ozone budget was dominated by the vertical transport and dry deposition. The horizontal transport and gas-phase chemical production were relatively small in the surface layer. Presumably, ozone was produced in upper layers within the atmospheric boundary layer and convected down to surface where it is destroyed. When BVOCs was included, apart from the enhancement of gas-phase chemical production of ozone, both the surface deposition and vertical transport were also augmented.     

Impacts of boundary layer mixing on pollutant vertical profiles in the lower troposphere: Implications to satellite remote sensing

Mixing in the planetary boundary layer (PBL) affects vertical distributions of air tracers in the lower troposphere. An accurate representation of PBL mixing is critical for chemical-transport models (CTMs) for applications sensitive to simulations of the vertical profiles of tracers. The full mixing assumption in the widely used global CTM GEOS-Chem has recently been supplemented with a non-local PBL scheme. This study analyzes the impact of the non-local scheme on model representation of PBL mixing, consequences for simulations of vertical profiles of air tracers and surface air pollution, and implications for model applications to the interpretation of data retrieved from satellite remote sensing. The non-local scheme significantly improves simulations of the vertical distributions for NO₂ and O₃, as evaluated using aircraft measurements in summer 2004. It also reduces model biases over the U.S. by more than 10 ppb for surface ozone concentrations at night and by 2–5 ppb for peak ozone in the afternoon, as evaluated using ground observations. The application to inverse modeling of anthropogenic NO_x emissions for East China using satellite retrievals of NO₂ from OMI and GOME-2 suggests that the full mixing assumption results in 3–14% differences in top–down emission budgets as compared to the non-local scheme. The top–down estimate combining the non-local scheme and the Lin et al. inverse modeling approach suggests a magnitude of 6.6 TgN yr^?1 for emissions of NO_x over East China in July 2008 and 8.0 TgN yr^?1 for January 2009, with the magnitude and seasonality in good agreement with bottom–up estimates.     

Global scale emission and distribution of sea-spray aerosol: Sea-salt and organic enrichment

The chemical composition of marine aerosols as a function of their size is an important parameter for the evaluation of their impact on the global climate system. In this work we model fine particle organic matter emitted by sea spray processes and its influence on the aerosol chemical properties at the global scale using the off-line global Chemistry-Transport Model TM5. TM5 is coupled to a microphysical aerosol dynamics model providing size resolved information on particle masses and numbers. The mass of the emitted sea spray particles is partitioned between water insoluble organic matter (WIOM) and sea salt components in the accumulation mode using a function that relates the emitted organic fraction to the surface ocean chlorophyll-a concentrations. The global emission in the sub-micron size range of organic matter by sea spray process is 8.2 Tg yr^?1, compared to 24 Tg fine yr^?1 sea-salt emissions. When the marine sources are included, the concentrations of modelled primary particulate organic matter (POM) increase mainly over the oceans. The model predictions of WIOM and sea salt are evaluated against measurements carried out at Mace Head (Northern Hemisphere) and Amsterdam Island (Southern Hemisphere), showing that in clean marine conditions WIOM marine emissions contribute significantly to POM values.     

Canopy leaching of nutrients and metals in a mountain spruce forest

Precipitation and throughfall fluxes of major ions, nutrients (C, N, P), and metals (Al, Fe, Mn), and the chemical composition of litter fall and living plant tissue in Norway spruce stands (the Bohemian Forest; Czech Republic), were used to evaluate how microbial processes and decay of plant tissue in canopies influence canopy leaching (CL) of elements. Proton exchange for Mg²⁺, Ca²⁺, and K⁺ in decaying biomass and co-transport of Ca²⁺ and K⁺ out of plant cells with organic acid anions were the most likely processes contributing to CL of base cations. The CL of total P and N (and also NO₃^?) was minor. Important proportions of the N and P mineral forms were transformed to organic forms by microbial processes (primary and bacterial production), with the respective CL of ?13.9 and 16.4 mmol m^?2 yr^?1 for NH₄⁺ and organic N, and ?0.33 and 0.22 mmol m^?2 yr^?1 for dissolved reactive P (DRP) and organic P. Most of particulate P and N in throughfall (～90%) originated from microbial DRP and NH₄⁺ transformations, but particulate C mostly came from the fragmentation of plant tissue (58%). Among metals, CL was not observed for Al, was small for Fe (0.3 mmol m^?2 yr^?1), and greatest for Mn (0.9 mmol m^?2 yr^?1) due to leaching from decaying tissue by acidic precipitation.     

Bottom-up uncertainty estimates of global ammonia emissions from global agricultural production systems

Here we present an uncertainty analysis of NH₃ emissions from agricultural production systems based on a global NH₃ emission inventory with a 5×5 min resolution. Of all results the mean is given with a range (10% and 90% percentile). The uncertainty range for the global NH₃ emission from agricultural systems is 27–38 (with a mean of 32) Tg NH₃-N yr⁻¹, N fertilizer use contributing 10–12 (11) Tg yr⁻¹ and livestock production 16–27 (21) Tg yr⁻¹. Most of the emissions from livestock production come from animal houses and storage systems (31–55%); smaller contributions come from the spreading of animal manure (23–38%) and grazing animals (17–37%). This uncertainty analysis allows for identifying and improving those input parameters with a major influence on the results. The most important determinants of the uncertainty related to the global agricultural NH₃ emission comprise four parameters (N excretion rates, NH₃ emission rates for manure in animal houses and storage, the fraction of the time that ruminants graze and the fraction of non-agricultural use of manure) specific to mixed and landless systems, and total animal stocks. Nitrogen excretion rates and NH₃ emission rates from animal houses and storage systems are shown consistently to be the most important parameters in most parts of the world. Input parameters for pastoral systems are less relevant. However, there are clear differences between world regions and individual countries, reflecting the differences in livestock production systems.     

The effect of variability in industrial emissions on ozone formation in Houston, Texas

Ambient observations have indicated that high concentrations of ozone observed in the Houston/Galveston area are associated with plumes of highly reactive hydrocarbons, mixed with NO_x, from industrial facilities. Ambient observations and industrial process data, such as mass flow rates for industrial flares, indicate that the VOCs associated with these industrial emissions can have significant temporal variability. To characterize the effect of this variability in emissions on ozone formation in Houston, data were collected on the temporal variability of industrial emissions or emission surrogates (e.g., mass flow rates to flares). The observed emissions variability was then used to construct regionwide emission inventories with variable industrial emissions, and the impacts of the variability on ozone formation were examined for two types of meteorological conditions, both of which lead to high ozone concentrations in Houston. The air quality simulations indicate that variability in industrial emissions has the potential to cause increases and decreases of 10–52 ppb (13–316%), or more, in ozone concentration. The largest of these differences are restricted to regions of 10–20 km², but the variability also has the potential to increase regionwide maxima in ozone concentrations by up to 12 ppb.     

Historical deposition of mercury and selected trace elements to high-elevation National Parks in the Western U.S. inferred from lake-sediment cores

Atmospheric deposition of Hg and selected trace elements was reconstructed over the past 150 years using sediment cores collected from nine remote, high-elevation lakes in Rocky Mountain National Park in Colorado and Glacier National Park in Montana. Cores were age dated by ²¹⁰Pb, and sedimentation rates were determined using the constant rate of supply model. Hg concentrations in most of the cores began to increase around 1900, reaching a peak sometime after 1980. Other trace elements, particularly Pb and Cd, showed similar post-industrial increases in lake sediments, confirming that anthropogenic contaminants are reaching remote areas of the Rocky Mountains via atmospheric transport and deposition. Preindustrial (pre-1875) Hg fluxes in the sediment ranged from 5.7 to 42 μg m^?2 yr^?1 and modern (post-1985) fluxes ranged from 17.7 to 141 μg m^?2 yr^?1. The average ratio of modern to preindustrial fluxes was 3.2, which is similar to remote lakes elsewhere in North America. Estimates of net atmospheric deposition based on the cores were 3.1 μg m^?2 yr^?1 for preindustrial and 11.7 μg m^?2 yr^?1 for modern times. Current-day measurements of wet deposition range from 5.0 to 8.6 μg m^?2 yr^?1, which are lower than the modern sediment-based estimate of 11.7 μg m^?2 yr^?1, perhaps owing to inputs of dry-deposited Hg to the lakes.     

Increase in springtime tropospheric ozone at a mountainous site in Japan for the period 1998–2006

The trend of tropospheric ozone from 1998 to 2006 was examined based on continuous measurements made at a site on Mt. Happo, Japan. We focused our study on springtime ozone, to coincide with the East Asian continental outflow that dominates the lower tropospheric ozone over Japan during this season. The observed increase of ～1 ppbv yr^?1 in the mean ozone level was statistically significant. We also found that the probability distribution of the springtime ozone mixing ratios was substantially modified, with the ozone mixing ratios greatly increasing at the upper end of the probability distribution. This increase has been particularly large since 2003, with larger increases occurring at the higher percentiles. The number of high-ozone days doubled during 2003–2006 compared to 1999–2002. One of the very likely explanations is the enhancement of regional ozone pollution due to rapidly increasing anthropogenic emissions from East Asia.     

Temperature and air velocity effects on ethanol emission from corn silage with the characteristics of an exposed silo face

Volatile organic compounds (VOCs) from agricultural sources are believed to be an important contributor to tropospheric ozone in some locations. Recent research suggests that silage is a major source of VOCs emitted from agriculture, but only limited data exist on silage emissions. Ethanol is the most abundant VOC emitted from corn silage; therefore, ethanol was used as a representative compound to characterize the pattern of emission over time and to quantify the effect of air velocity and temperature on emission rate. Ethanol emission was measured from corn silage samples removed intact from a bunker silo. Emission rate was monitored over 12 h for a range in air velocity (0.05, 0.5, and 5 m s^?1) and temperature (5, 20, and 35 °C) using a wind tunnel system. Ethanol flux ranged from 0.47 to 210 g m^?2 h^?1 and 12 h cumulative emission ranged from 8.5 to 260 g m^?2. Ethanol flux was highly dependent on exposure time, declining rapidly over the first hour and then continuing to decline more slowly over the duration of the 12 h trials. The 12 h cumulative emission increased by a factor of three with a 30 °C increase in temperature and by a factor of nine with a 100-fold increase in air velocity. Effects of air velocity, temperature, and air-filled porosity were generally consistent with a conceptual model of VOC emission from silage. Exposure duration, temperature, and air velocity should be taken into consideration when measuring emission rates of VOCs from silage, so emission rate data obtained from studies that utilize low air flow methods are not likely representative of field conditions.     

High-resolution inventory of NO emissions from agricultural soils over the Ile-de-France region

Arable soils are a significant source of nitric oxide (NO), a precursor of tropospheric ozone, and thereby contribute to ozone pollution. However, their actual impact on ozone formation is strongly related to their spatial and temporal emission patterns, which warrant high-resolution estimates.Here, we combined an agro-ecosystem model and geo-referenced databases to map these sources over the 12 000 km² administrative region surrounding Paris, France, with a kilometric level resolution. The six most frequent arable crop species were simulated, with emission rates ranging from 1.4 kg N-NO ha⁻¹ yr⁻¹ to 11.1 kg N-NO ha⁻¹ yr⁻¹. The overall emission factor for fertilizer-derived NO emissions was 1.7%, while background emissions contributed half of the total NO efflux. Emissions were strongly seasonal, being highest in spring due to fertilizer inputs. They were mostly sensitive to soil type, crops' growing season and fertilizer N rates.     

A kinetic mechanism for predicting secondary organic aerosol formation from toluene oxidation in the presence of NOx and natural sunlight

A kinetic mechanism to predict secondary organic aerosol (SOA) formation from the photo-oxidation of toluene was developed. Aerosol phase chemistry that includes nucleation, gas–particle partitioning and particle-phase reactions as well as the gas-phase chemistry of toluene and its degradation products were represented. The mechanism was evaluated against experimental data obtained from the University of North Carolina (UNC) 270 m³ dual outdoor aerosol smog chamber facility. The model adequately simulates the decay of toluene, the nitric oxide (NO) to nitrogen dioxide (NO₂) conversion and ozone formation. It also provides a reasonable prediction of SOA production under different conditions that range from 15 to 300 μg m⁻³. Speciation of simulated aerosol material shows that up to 70% of the aerosol mass comes from oligomers and polymers depending on initial reactant concentrations. The dominant particle-phase species predicted by the mechanism are glyoxal oligomers, ketene oligomers from the photolysis of the toluene OH reaction product 2-methyl-2,4-hexadienedial, organic nitrates, methyl nitro-phenol analogues, C7 organic peroxides, acylperoxy nitrates and for the low-concentration experiments, unsaturated hydroxy nitro acids.     

Kinetic aspects and identification of by-products during the ozonation of bitertanol in agricultural wastewaters

The degradation of bitertanol by ozone treatment is investigated. Solutions of bitertanol (8.4 μg mL^?1) were prepared either by dissolution of the standard or by dilution of Gaucho Blé seed loading solution and then ozonated under different conditions. Evolution of the concentrations of bitertanol and its ozonation by-products in both solutions was monitored by HPLC–UV as a function of the treatment time for a concentration of 100 g m^?3 of ozone in the inlet gas. Bitertanol degradation was found to follow a pseudo-first order reaction in both cases. However, the rate of the reaction in diluted seed loading solution was much lower (0.19 vs. 0.27 min^?1 in standard solution) and was close to the reaction rate observed in the presence of a radical scavenger, tert-butanol (0.11 min^?1). Thus, it may be suggested that additives present in the seed loading solution may play the role of radical scavengers. Study of ozone concentration in the inlet gas (from 25 to 100 g m^?3) showed that ozone degradation is also a first-order reaction with respect to ozone. Four ozonation by-products were highlighted, collected and identified by HPLC coupled with an ion trap mass spectrometer using positive electrospray ionization mode. A degradation pathway of bitertanol was finally proposed.     

The impact of recirculation,ventilation and filters on secondary organic aerosols generated by indoor chemistry

This study examined the impact of recirculation rates (7 and 14 h^?1), ventilation rates (1 and 2 h^?1), and filtration on secondary organic aerosols (SOAs) generated by ozone of outdoor origin reacting with limonene of indoor origin. Experiments were conducted within a recirculating air handling system that serviced an unoccupied, 236 m³ environmental chamber configured to simulate an office; either no filter, a new filter or a used filter was located downstream of where outdoor air mixed with return air. For otherwise comparable conditions, the SOA number and mass concentrations at a recirculation rate of 14 h^?1 were significantly smaller than at a recirculation rate of 7 h^?1. This was due primarily to lower ozone concentrations, resulting from increased surface removal, at the higher recirculation rate. Increased ventilation increased outdoor-to-indoor transport of ozone, but this was more than offset by the increased dilution of SOA derived from ozone-initiated chemistry. The presence of a particle filter (new or used) strikingly lowered SOA number and mass concentrations compared with conditions when no filter was present. Even though the particle filter in this study had only 35% single-pass removal efficiency for 100 nm particles, filtration efficiency was greatly amplified by recirculation. SOA particle levels were reduced to an even greater extent when an activated carbon filter was in the system, due to ozone removal by the carbon filter. These findings improve our understanding of the influence of commonly employed energy saving procedures on occupant exposures to ozone and ozone-derived SOA.     

Gas-phase chemistry of benzyl alcohol: Reaction rate constants and products with OH radical and ozone

A bimolecular rate constant, k_{OH+Benzyl alcohol}, of (28 ± 7) × 10^?12 cm³ molecule^?1 s^?1 was measured using the relative rate technique for the reaction of the hydroxyl radical (OH) with benzyl alcohol, at (297 ± 3) K and 1 atm total pressure. Additionally, an upper limit of the bimolecular rate constant, k_{O3+Benzyl alcohol}, of approximately 6 × 10^?19 cm³ molecule^?1 s^?1 was determined by monitoring the decrease in benzyl alcohol concentration over time in an excess of ozone (O₃). To more clearly define part of benzyl alcohol's indoor environment degradation mechanism, the products of the benzyl alcohol + OH were also investigated. The derivatizing agents O-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine (PFBHA) and N,O-bis(trimethylsilyl) trifluoroacetamide (BSTFA) were used to positively identify benzaldehyde, glyoxal and 4-oxopentanal as benzyl alcohol/OH reaction products. The elucidation of other reaction products was facilitated by mass spectrometry of the derivatized reaction products coupled with plausible benzyl alcohol/OH reaction mechanisms based on previously published volatile organic compound/OH gas-phase reaction mechanisms.     

Evidence for short-range transport of atmospheric mercury to a rural,inland site

Atmospheric mercury (Hg) species, including gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particulate-bound mercury (Hg_p), were monitored near three sites, including a cement plant (monitored in 2007 and 2008), an urban site and a rural site (both monitored in 2005 and 2008). Although the cement plant was a significant source of Hg emissions (for 2008, GEM: 2.20 ± 1.39 ng m^?3, RGM: 25.2 ± 52.8 pg m^?3, Hg_p 80.8 ± 283 pg m^?3), average GEM levels and daytime average dry depositional RGM flux were highest at the rural site, when all three sites were monitored sequentially in 2008 (rural site, GEM: 2.37 ± 1.26 ng m^?3, daytime RGM flux: 29 ± 40 ng m^?2 day^?1). Photochemical conversion of GEM was not the primary RGM source, as highest net RGM gains (75.9 pg m^?3, 99.0 pg m^?3, 149 m^?3) occurred within 3.0–5.3 h, while the theoretical time required was 14–23 h. Instead, simultaneous peaks in RGM, Hg_p, ozone (O₃), nitrogen oxides, and sulfur dioxide in the late afternoon suggested short-range transport of RGM from the urban center to the rural site. The rural site was located more inland, where the average water vapor mixing ratio was lower compared to the other two sites (in 2008, rural: 5.6 ± 1.4 g kg^?1, urban: 9.0 ± 1.1 g kg^?1, cement plant: 8.3 ± 2.2 g kg^?1). Together, these findings suggested short-range transport of O₃ from an urban area contributed to higher RGM deposition at the rural site, while drier conditions helped sustain elevated RGM levels. Results suggested less urbanized environments may be equally or perhaps more impacted by industrial atmospheric Hg emissions, compared to the urban areas from where Hg emissions originated.