Seasonal variation in dissolved gaseous mercury and total mercury concentrations in Juam Reservoir, Korea

Dissolved gaseous mercury (DGM) and total mercury (TM) concentrations were measured in Juam Reservoir, Korea. DGM concentrations were higher in spring (64+/-13pgL(-1)) and summer (109+/-15pgL(-1)), and lower in fall (20+/-2pgL(-1)) and winter (23+/-6pgL(-1)). In contrast, TM concentrations were higher in fall (3.2+/-0.1ngL(-1)) and winter (3.3+/-0.1ngL(-1)) than in spring (2.3+/-0.1ngL(-1)) and summer (2.2+/-0.4ngL(-1)). DGM concentrations were correlated with water temperature (p<0.0001), ORP (p<0.0001), UV intensity (UV-A: p=0.008; UV-B: p=0.003), and DOC concentration (p=0.0107). DGM concentrations varied diurnally with UV intensity. The average summer DGM (109+/-15pgL(-1)) and TM (2.2+/-0.4ngL(-1)) concentrations in Juam Reservoir were higher than the averages for North American lakes (DGM=38+/-16pgL(-1); TM=1.0+/-1.2ngL(-1)), but lower than levels reported for Baihua Reservoir in China.     

Measurement of Ultrafine Particle Size Distributions from Coal-, Oil-, and Gas-Fired Stationary Combustion Sources

Abstract

Currently, we have limited knowledge of the physical and chemical properties of emitted primary combustion aerosols and the changes in those properties caused by nucleation, condensation growth of volatile species, and particle coagulations under dilution and cooling in the ambient air. A dilution chamber was deployed to sample exhaust from a pilot-scale furnace burning various fuels at a nominal heat input rate of 160 kW/h^?1 and 3% excess oxygen. The formation mechanisms of particles smaller than 420 nm in electrical mobility diameter were experimentally investigated by measurement with a Scanning Mobility Particle Sizer (SMPS) as a function of aging times, dilution air ratios, combustion exhaust temperatures, and fuel types. Particle formation in the dilution process is a complex mixture of nucleation, coagulation, and condensational growth, depending on the concentrations of available condensable species and solid or liquid particles (such as soot, ash) in combustion exhausts. The measured particle size distributions in number concentrations measured show peaks of particle number concentrations for medium sulfur bituminous coal, No. 6 fuel oil, and natural gas at 40-50 nm, 70-100 nm, and 15-25 nm, respectively. For No. 6 fuel oil and coal, the particle number concentration is constant in the range of a dilution air ratio of 50, but the number decreases as the dilution air ratio decreases to 10. However, for natural gas, the particle number concentration is higher at a dilution air ratio of 10 and decreases at dilution air ratios of 20-50. At a dilution air ratio of 10, severe particle coagulation occurs in a relatively short time. Samples taken at different combustion exhaust temperatures for these fuel types show higher particle number concentrations at 645 K than at 450 K. As the aging time of particles increases, the particles increase in size and the number concentrations decrease. The largest gradient of particle number distribution occurs within the first 10 sec after dilution but shows only minor differences between 10 and 80 sec. The lifetimes of the ultrafine particles are relatively short, with a scale on the order of a few seconds. Results from this study suggest that an aging time of 10 sec and a dilution air ratio of 20 are sufficient to obtain representative primary particle emission samples from stationary combustion sources.     

Measurement of ultrafine particle size distributions from coal-, oil-, and gas-fired stationary combustion sources

Currently, we have limited knowledge of the physical and chemical properties of emitted primary combustion aerosols and the changes in those properties caused by nucleation, condensation growth of volatile species, and particle coagulations under dilution and cooling in the ambient air. A dilution chamber was deployed to sample exhaust from a pilot-scale furnace burning various fuels at a nominal heat input rate of 160 kW/h(-1) and 3% excess oxygen. The formation mechanisms of particles smaller than 420 nm in electrical mobility diameter were experimentally investigated by measurement with a Scanning Mobility Particle Sizer (SMPS) as a function of aging times, dilution air ratios, combustion exhaust temperatures, and fuel types. Particle formation in the dilution process is a complex mixture of nucleation, coagulation, and condensational growth, depending on the concentrations of available condensable species and solid or liquid particles (such as soot, ash) in combustion exhausts. The measured particle size distributions in number concentrations measured show peaks of particle number concentrations for medium sulfur bituminous coal, No. 6 fuel oil, and natural gas at 40-50 nm, 70-100 nm, and 15-25 nm, respectively. For No. 6 fuel oil and coal, the particle number concentration is constant in the range of a dilution air ratio of 50, but the number decreases as the dilution air ratio decreases to 10. However, for natural gas, the particle number concentration is higher at a dilution air ratio of 10 and decreases at dilution air ratios of 20-50. At a dilution air ratio of 10, severe particle coagulation occurs in a relatively short time. Samples taken at different combustion exhaust temperatures for these fuel types show higher particle number concentrations at 645 K than at 450 K. As the aging time of particles increases, the particles increase in size and the number concentrations decrease. The largest gradient of particle number distribution occurs within the first 10 sec after dilution but shows only minor differences between 10 and 80 sec. The lifetimes of the ultrafine particles are relatively short, with a scale on the order of a few seconds. Results from this study suggest that an aging time of 10 sec and a dilution air ratio of 20 are sufficient to obtain representative primary particle emission samples from stationary combustion sources.     

Characteristics of atmospheric speciated mercury concentrations (TGM,Hg(II) and Hg(p)) in Seoul,Korea

Ambient speciated mercury concentrations including total gaseous mercury (TGM), gaseous divalent mercury (Hg(II)), and particulate mercury (Hg(p)) were measured on the roof of the Graduate School of Public Health building in Seoul, Korea from February 2005 to February 2006. The average concentrations were 3.22 ± 2.10 ng m^?3, 27.2 ± 19.3 pg m^?3, and 23.9 ± 19.6 pg m^?3 for TGM, Hg(II), and Hg(p), respectively. Hg(II) and Hg(p) concentrations were higher during the daytime than during the nighttime, probably because of high photochemical activity. Hg⁰ concentrations were not significantly correlated with ozone however a positive correlation between ozone and Hg(II) was found during periods of high humidity. Eighteen days were characterized as pollution events with 24 h average PM_2.5 concentrations >65 μg m^?3. The average concentrations of TGM and Hg(p) during these events were 1.4–2 times higher than those during non-pollution events. In order to identify the contribution of long-range transported mercury to the enhanced mercury concentrations in Korea, an episode was defined as a period with hourly average TGM and CO concentrations higher than the monthly average TGM and CO concentrations and with significant enhancement of both TGM and CO concentrations for at least 10 h. A total of 70 episodes were identified during the sampling period: 36 local episodes and 34 long-range transport episodes. The mean ΔTGM/ΔCO slope for all episodes was 0.0063 ng m^?3 ppbv^?1 which agreed well with the slope (0.0036–0.0074 ng m^?3 ppbv^?1) found in previous studies that identified long-range transport of TGM from China. The mean slope during non-events was 0.0011 ng m^?3 ppbv^?1. Back-trajectory analysis showed that during episodes, air parcels arrived mostly from the major industrial areas in China (n = 25, 73%), followed by Japan (n = 4, 12%), Yellow Sea (n = 3, 9%), and Russia (n = 2, 6%).     

Emissions of polychlorinated biphenyls (PCBs) from sludge drying beds to the atmosphere in Chicago

Ambient air PCB concentrations in the Lake Calumet region in Southeast Chicago have been found to be significantly higher than in nearby non-urban areas. This area is highly industrialized and also contains municipal sludge drying facilities and landfills. In an effort to quantify the importance of the sludge drying facilities to the elevated concentrations, upwind/downwind air samples from the Calumet East sludge drying bed were obtained between April and October 2002. For these samples, the downwind minus upwind (downwind-upwind) concentration varied from 0.33 to 1.27ngm(-3) for non-northeast (NE) direction winds suggesting sludge drying is a source of PCBs to the atmosphere. However, the upwind concentrations were higher than the downwind for winds from the NE of the sampling site suggesting more significant source(s), possibly Lake Calumet or the so called "Cluster site" NE of the sludge drying beds. Flux chamber experiments carried out during the sampling period measured average PCB fluxes of 210ngm(-2)h(-1) (range 43-910ngm(-2)h(-1)) which resulted in an overall flux of 0.005kgday (d)(-1) ( approximately 2kgyr(-1)). A developed regression equation between moisture content and sludge concentration estimated higher PCB losses of 0.26kgd(-1) ( approximately 95kgyr(-1)). Although these two approaches yielded different values, they both indicate that the emission from the Calumet East sludge drying beds were of minimal importance when compared to the total estimated amount of 2-70kgd(-1) (700-2100kgyr(-1)) of PCBs entering the Chicago atmosphere.     

The application and development of country-specific parameters for accurate estimations of methane emissions from solid-waste disposal sites

To identify the application and development of country-specific parameters for methane emission estimations from solid-waste disposal sites, National Inventory Reports of 41 Annex I countries and National Communications of ten non-Annex I countries of the United Nations Framework Convention on Climate Change were analyzed. A first-order decay method was applied to 38 out of 41 Annex I countries and to five out of ten non-Annex I countries in national GHG inventory submissions up to 2012. Country-specific parameters were approximately 26 % of the total number of parameters used in the 38 Annex I countries and were mostly developed for degradable organic carbon and reaction constants that cover certain waste compositions. The UNFCCC encourages countries to develop more country-specific parameters reflecting the distinct characteristics of each country in which solid-waste disposal site is a key source. Depending on a country’s condition, a stepwise approach regarding the development of country-specific parameters needs to be done so as to improve the accuracy of methane emission estimates in the solid-waste disposal site category.     

Variability of nitrous oxide and carbon dioxide emissions continuously measured in solid waste incinerators

Nitrous oxide and carbon dioxide were continuously measured and variability of emission factors (EFs) was evaluated in five municipal waste incinerators (MWIs) and four industrial waste incinerators (IWIs) from 24 to 86 days between 2008 and 2011. N₂O EFs were calculated by Monte Carlo simulation and mean N₂O EFs were 7.1, 107, 127, 219 g N₂O/ton waste combusted in MWIs with selective catalytic reduction (SCR) for NOx control, MWIs with selective non-catalytic reduction (SNCR), IWIs with SNCR, and a MWI using fluidized bed with SNCR, respectively. Climate-relevant CO₂ EFs ranged from 0.45 to 0.72 ton CO₂/ton waste combusted in MWIs. Maximum values of upper limit for 95% confidence intervals (CIs) of N₂O EFs estimated in each MWIs with SCR, MWIs with SNCR, IWIs with SNCR were 185, 94, 101% of mean N₂O EFs, respectively. Meanwhile, maximum values of upper limit for 95% CIs of CO₂ EFs were much lower as between 18 and 36% in those facilities. 84% CIs of mean N₂O EFs in MWIs with SNCR and IWIs with SNCR were overlapped indicating those values are not significantly different.     

Mercury wet deposition in rural Korea: concentrations and fluxes

The characteristics of Hg wet deposition were investigated in a rural area of Korea from August 2006 to July 2008. The volume weighted mean (VWM) Hg(T) concentration and cumulative Hg(T) flux were 8.8 ng L(-1) and 9.4 μg m(-2) per year, respectively. The VWM Hg(T) concentration varied seasonally, similar to the seasonal pattern in atmospheric Hg(p) concentration. The enhancement of both VWM Hg(T) and atmospheric Hg(p) concentrations in spring and winter was likely caused by the long-range transport of Hg from China. Monthly VWM Hg(T) and atmospheric Hg(p) concentrations were well correlated (R(2) = 0.36); however, there was no correlation between VWM Hg(T) and RGM (reactive gaseous mercury) concentrations, suggesting that Hg(p) was responsible for the majority of the Hg in wet deposition at this site. The VWM Hg(T) concentration in snow was statistically higher than in rain. In addition, the atmospheric Hg(p) concentration appeared to be elevated for snow events as well. This suggests that both elevated Hg(p) concentrations and the enhanced scavenging efficiency of snow for Hg(p) were responsible for the elevated VWM Hg(T) concentrations measured during snow events.     

Measured summertime concentrations of particulate components,Hg0, and speciated polycyclic aromatic hydrocarbons at rural sites in New York State

Daily PM2.5 samples, Hg0 and speciated polycyclic aromatic hydrocarbon (PAH) were simultaneously collected at Potsdam and Stockton site in NY during the summers of 2000 and 2001. Samples for determination of the mass concentration and chemical composition of the PM2.5 were obtained with a speciation network PM2.5 sampler. Chemical composition including trace elemental composition, water-soluble ions, and elemental carbon were analyzed. Elemental mercury and PAHs were sampled separately. Daily PM2.5 concentrations ranged from 0.47 to 53.7 microg m(-3) at the Potsdam site, and from 0.82 to 47.23 microg m(-3) at the Stockton site with large daily differences between the two sites. Potsdam consistently had lower mass values than Stockton. The greatest contributors to the PM2.5 mass (generally >0.1 microg/m(3)) were sulfate, nitrate, ammonium, and BC at both sites. Seventeen PAHs were identified at each site in 2000 and the average total concentrations were 3.2 ng/m(3) and 2.9 ng/m(3) at the Potsdam and Stockton sites, respectively. The mean vapor phase mercury concentration at the Potsdam site (2.4 +/-1.2 ng m(-3), n=93) was higher than that at the Stockton site (1.2 +/- 1.0 ng m(-3), n=60) in 2000, whereas in 2001, the average concentrations were 1.1 ng m(-3) and 1.6 ng m(-3) at the Potsdam and Stockton sites, respectively. In general, vapor phase mercury concentrations increased with increasing ambient temperature at the Stockton site in 2000. These differences in values between 2000 and 2001 can be largely explained by distinct differences in the meteorological regimes that dominated in the different years.     

Health risk assessment and source apportionment of PM2.5-bound toxic elements in the industrial city of Siheung,Korea

Environmental Science and Pollution Research - The emission sources and their health risks of fine particulate matter (PM2.5) in Siheung, Republic of Korea, were investigated as a middle-sized...