Studies of potential sources that contributed to atmospheric mercury in Toronto,Canada

This study identified sources of mercury (Hg) in downtown Toronto, Canada by analyzing gaseous elemental mercury (GEM), mercury associated with particles with sizes less than 2.5 microns (PHg < 2.5), and gaseous oxidized inorganic mercury (GOIM), commonly referred to as reactive gaseous mercury (RGM), and air pollutants (CO, NO_x, O₃, PM_2.5, SO₂) concentrations between Dec 2003 and Nov 2004. The data were analyzed using Positive Matrix Factorization (PMF) model, Principal Components Analysis (PCA), ratio analysis, back trajectories, and correlation analyses. The analyses suggest industrial sources (chemical production, metal production, sewage treatment), rather than coal combustion, were the major contributors to measured Hg levels. Overlap in source profiles for the Hg sources listed in the Canadian National Pollutant Release Inventory (NPRI) and lack of source profiles for urban sources were the major limitations to positively identifying sources from the PMF and PCA factors. Correlation analyses revealed direct emissions were the sources of GOIM in spring, summer, and fall, and the occurrence of GEM oxidation by ozone in the summer. Elevated Hg events are attributed to emissions from urban sources near the sampling site, regional point sources, and photochemical processes involving ozone.     

Temporal distribution and potential sources of atmospheric mercury measured at a high-elevation background station in Taiwan

Measurements of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM), and particulate mercury (PHg) have been conducted at Lulin Atmospheric Background Station (LABS) in Taiwan since April 2006. This was the first long-term free tropospheric atmospheric Hg monitoring program in the downwind region of East Asia, which is a major Hg emission source region. Between April 13, 2006 and December 31, 2007, the mean concentrations of GEM, RGM, and PHg were 1.73 ng m^?3, 12.1 pg m^?3, and 2.3 pg m^?3, respectively. A diurnal pattern was observed for GEM with afternoon peaks and nighttime lows, whereas the diurnal pattern of RGM was opposite to that of GEM. Spikes of RGM were frequently observed between midnight and early morning with concurrent decreases in GEM and relative humidity and increases in O₃, suggesting the oxidation of GEM and formation of RGM in free troposphere (FT). Upslope movement of boundary layer (BL) air in daytime and subsidence of FT air at night resulted in these diurnal patterns. Considering only the nighttime data, which were more representative of FT air, the composite monthly mean GEM concentrations ranged between 1.06 and 2.06 ng m^?3. Seasonal variation in nighttime GEM was evident, with lower concentrations usually occurring in summer when clean marine air masses prevailed. Between fall and spring, air masses passed the East Asian continent prior to reaching LABS, contributing to the elevated GEM concentrations. Analysis of GEM/CO correlation tends to support the argument. Good GEM/CO correlations were observed in fall, winter, and spring, suggesting influence of anthropogenic emission sources. Our results demonstrate the significance of East Asian Hg emissions, including both anthropogenic and biomass burning emissions, and their long-range transport in the FT. Because of the pronounced seasonal monsoon activity and the seasonal variation in regional wind field, export of the Asian Hg emissions to Taiwan occurs mainly during fall, winter, and spring.     

Mercury Mass Balances: A Case Study of Two North Dakota Power Plants

ABSTRACT

The Energy & Environmental Research Center (EERC) conducted a mercury-sampling program to provide data on the quantity and forms of Hg emitted and on the Hg removal efficiency of the existing air pollution control devices at two North Dakota power plants—Milton R. Young Station and Coal Creek Station. Minnkota Power Cooperative, Great River Energy, the North Dakota Industrial Commission, and EPRI funded the project. The primary objective was to obtain accurate measurements of Hg released from each plant, as verified by a material balance. A secondary objective was to evaluate the ability of a mercury continuous emission monitor (CEM) to measure total Hg at the stack.

At both plants, speciated Hg measurements were made at the inlets and outlets of both the electrostatic precipi-tators (ESPs) and the flue gas desulfurization (FGD) systems. A Semtech Hg 2000 (Semtech Metallurgy AB) mercury CEM was used to measure the total Hg emissions at the stack in real time. Using these measurements and plant data, the measured Hg concentrations in the coal, FGD slurries, and ESP ash, a Hg mass flow rate was calculated at each sampling location. Excellent Hg mass balances were obtained (±15%). It was also found that the Hg was mostly in the elemental phase (~90%), and the small amount of oxidized Hg that was generated was removed by the FGD systems.

Insignificant amounts of particulate-bound Hg were measured at both plants. However, 10-20% of the elemental Hg measured prior to the ESP was converted to oxidized Hg across the ESP. The data show that, at these facilities, almost all of the Hg generated is being emitted into the atmosphere as elemental Hg. Local or regional deposition of the Hg emitted from these plants is not a concern. However, the Hg does become part of the global Hg burden in the atmosphere. Also, the evidence appears to indicate that elemental Hg is more difficult to remove from flue gas than oxidized Hg is.     

Scientific uncertainties in atmospheric mercury models II: Sensitivity analysis in the CONUS domain

In this study, we present the response of model results to different scientific treatments in an effort to quantify the uncertainties caused by the incomplete understanding of mercury science and by model assumptions in atmospheric mercury models. Two sets of sensitivity simulations were performed to assess the uncertainties using modified versions of CMAQ-Hg in a 36-km Continental United States domain. From Set 1 Experiments, it is found that the simulated mercury dry deposition is most sensitive to the gaseous elemental mercury (GEM) oxidation product assignment, and to the implemented dry deposition scheme for GEM and reactive gaseous mercury (RGM). The simulated wet deposition is sensitive to the aqueous Hg(II) sorption scheme, and to the GEM oxidation product assignment. The inclusion of natural mercury emission causes a small increase in GEM concentration but has little impact on deposition. From Set 2 Experiments, it is found that both dry and wet depositions are sensitive to mercury chemistry. Change in model mercury chemistry has a greater impact on simulated wet deposition than on dry deposition. The kinetic uncertainty of GEM oxidation by O₃ and mechanistic uncertainty of Hg(II) reduction by aqueous HO₂ pose the greatest impact. Using the upper-limit kinetics of GEM–O₃ reaction or eliminating aqueous Hg(II)–HO₂ reaction results in unreasonably high deposition and depletion of gaseous mercury in the domain. Removing GEM–OH reaction is not sufficient to balance the excessive mercury removal caused by eliminating the HO₂ mechanism. Field measurements of mercury dry deposition, better quantification of mercury air-surface exchange and further investigation of mercury redox chemistry are needed for reducing model uncertainties and for improving the performance of atmospheric mercury models.     

The Fate and Behavior of Mercury in Coal-Fired Power Plants

Abstract

For the past 22 years in the Netherlands, the behavior of Hg in coal-fired power plants has been studied extensively. Coal from all over the world is fired in Dutch power stations. First, the Hg concentrations in these coals were measured. Second, the fate of the Hg during combustion was established by performing mass balance studies. On average, 43 ± 30% of the Hg was present in the flue gases downstream of the electrostatic precipitator (ESP; dust collector). In individual cases, this figure can vary between 1 and 100%. Important parameters are the Cl content of the fuel and the flue gas temperature in the ESP. On average, 54 ± 24% of the gaseous Hg was removed in the wet flue-gas desulfurization (FGD) systems, which are present at all Dutch coal-power stations. In individual cases, this removal can vary between 8% (outlier) and 72%.

On average, the fate of Hg entering the power station in the coal was as follows: <1% in the bottom ash, 49% in the pulverized fuel ash (ash collected in the ESP), 16.6% in the FGD gypsum, 9% in the sludge of the wastewater treatment plant, 0.04% in the effluent of the wastewater treatment plant, 0.07% in fly dust (leaving the stack), and 25% as gaseous Hg in the flue gases and emitted into the air. The distribution of Hg over the streams leaving the FGD depends strongly on the installation. On average, 75% of the Hg was removed, and the final concentration of Hg in the emitted flue gases of the Dutch power stations was only ~3 μg/m_STP ³ at 6% O₂. During co-combustion with biomass, the removal of Hg was similar to that during 100% coal firing.

Speciation of Hg is a very important factor. An oxidized form (HgCl₂) favors a high degree of removal. The conversion from Hg⁰ to HgCl₂ is positively correlated with the Cl content of the fuel. A catalytic DENOX (SCR) favors the formation of oxidized Hg, and, in combination with a wet FGD, the total removal can be as high as 90%.     

Mercury mass balances: a case study of two North Dakota power plants

The Energy & Environmental Research Center (EERC) conducted a mercury-sampling program to provide data on the quantity and forms of Hg emitted and on the Hg removal efficiency of the existing air pollution control devices at two North Dakota power plants--Milton R. Young Station and Coal Creek Station. Minnkota Power Cooperative, Great River Energy, the North Dakota Industrial Commission, and EPRI funded the project. The primary objective was to obtain accurate measurements of Hg released from each plant, as verified by a material balance. A secondary objective was to evaluate the ability of a mercury continuous emission monitor (CEM) to measure total Hg at the stack. At both plants, speciated Hg measurements were made at the inlets and outlets of both the electrostatic precipitators (ESPs) and the flue gas desulfurization (FGD) systems. A Semtech Hg 2000 (Semtech Metallurgy AB) mercury CEM was used to measure the total Hg emissions at the stack in real time. Using these measurements and plant data, the measured Hg concentrations in the coal, FGD slurries, and ESP ash, a Hg mass flow rate was calculated at each sampling location. Excellent Hg mass balances were obtained (+/- 15%). It was also found that the Hg was mostly in the elemental phase (approximately 90%), and the small amount of oxidized Hg that was generated was removed by the FGD systems. Insignificant amounts of particulate-bound Hg were measured at both plants. However, 10-20% of the elemental Hg measured prior to the ESP was converted to oxidized Hg across the ESP. The data show that, at these facilities, almost all of the Hg generated is being emitted into the atmosphere as elemental Hg. Local or regional deposition of the Hg emitted from these plants is not a concern. However, the Hg does become part of the global Hg burden in the atmosphere. Also, the evidence appears to indicate that elemental Hg is more difficult to remove from flue gas than oxidized Hg is.     

Estimation of Organic Compound Emissions from Waste Lagoons

Abstract

With the recent focus on fine particle matter (PM_2.5),new, self-consistent data are needed to characterize emissions from combustion sources. Such data are necessary for health assessment and air quality modeling. To address this need, emissions data for gas-fired combustors are presented here, using dilution sampling as the reference.The dilution method allows for collection of emitted particles under conditions simulating cooling and dilution during entry from the stack into the air. The sampling and analysis of the collected particles in the presence of precursor gases, SO₂, nitrogen oxide, volatile organic compound, and NH₃ is discussed; the results include data from eight gas fired units, including a dual-fuel institutional boiler and a diesel engine powered electricity generator. These data are compared with results in the literature for heavy-duty diesel vehicles and stationary sources using coal or wood as fuels. The results show that the gas-fired combustors have very low PM_2.5 mass emission rates in the range of ～10_-4 lb/million Btu (MMBTU) compared with the diesel backup generator with particle filter, with ～5 × 10_-3 lb/MMBTU. Even higher mass emission rates are found in coal-fired systems, with rates of ～0.07 lb/MMBTU for a bag-filter-controlled pilot unit burning eastern bituminous coal. The characterization of PM_2.5 chemical composition from the gas-fired units indicates that much of the measured primary particle mass in PM_2.5 samples is organic or elemental carbon and, to a much less extent, sulfate. Metal emissions are quite low compared with the diesel engines and the coal- or woodfueled combustors. The metals found in the gas-fired combustor particles are low in concentration, similar in concentration to ambient particles. The interpretation of the particulate carbon emissions is complicated by the fact that an approximately equal amount of particulate carbon (mainly organic carbon) is found on the particle collector and a backup filter. It is likely that measurement artifacts, mostly adsorption of volatile organic compounds on quartz filters, are positively biasing “true” particulate carbon emission results.     

Temporal variability of mercury speciation in urban air

Semi-continuous measurements of ambient mercury (Hg) species were performed in Detroit, MI, USA for the calendar year 2003. The mean (±standard deviation) concentrations for gaseous elemental mercury (GEM), particulate mercury (HgP), and reactive gaseous mercury (RGM) were 2.2±1.3 ng m⁻³, 20.8±30.0, and 17.7±28.9 pg m⁻³, respectively. A clear seasonality in Hg speciation was observed with GEM and RGM concentrations significantly (p<0.001) greater in warm seasons, while HgP concentrations were greater in cold seasons. The three measured Hg species also exhibited clear diurnal trends which were particularly evident during the summer months. Higher RGM concentrations were observed during the day than at night. Hourly HgP and GEM concentrations exhibited a similar diurnal pattern with both being inversely correlated with RGM. Multivariate analysis coupled with conditional probability function analysis revealed the conditions associated with high Hg concentration episodes, and identified the inter-correlations between speciated Hg concentrations, three common urban air pollutants (sulfur dioxide, ozone, and nitric oxides), and meteorological parameters. This analysis suggests that both local and regional sources were major factors contributing to the observed temporal variations in Hg speciation. Boundary layer dynamics and the seasonal meteorological conditions, including temperature and moisture content, were also important factors affecting Hg variability.     

Seasonal variation and source estimation of organic compounds in urban aerosol of Augsburg, Germany

This study reports a general assessment of the organic composition of the PM_2.5 samples collected in the city of Augsburg, Germany in a summer (August-September 2007) and a winter (February-March 2008) campaign of 36 and 30 days, respectively. The samples were directly submitted to in-situ derivatisation thermal desorption gas chromatography coupled with time of flight mass spectrometry (IDTD-GC-TOFMS) to simultaneously determine the concentrations of many classes of molecular markers, such as n-alkanes, iso- and anteiso-alkanes, polycyclic aromatic hydrocarbons (PAHs), oxidized PAHs, n-alkanoic acids, alcohols, saccharides and others.The PCA analysis of the data identified the contributions of three emission sources, i.e., combustion sources, including fossil fuel emissions and biomass burning, vegetative detritus, and oxidized PAHs. The PM chemical composition shows seasonal trend: winter is characterized by high contribution of petroleum/wood combustion while the vegetative component and atmospheric photochemical reactions are predominant in the hot season.     

Quantification of Monosaccharide Anhydrides by Liquid Chromatography Combined with Mass Spectrometry: Application to Aerosol Samples from an Urban and a Suburban Site Influenced by Small-Scale Wood Burning

Abstract

Levels of the monosaccharide anhydride (MA) levoglucosan and its isomeric compounds galactosan and mannosan were quantified in the PM₁₀ fraction (particulate matter ≤10 µm in aerodynamic diameter) of ambient aerosols from an urban (Oslo) and a suburban (Elverum) site in Norway, both influenced by small-scale wood burning. MAs are degradation products of cellulose and hemicellulose, and levoglucosan is especially emitted in high concentrations during pyrolysis and combustion of wood, making it a potential tracer of primary particles emitted from biomass burning. MAs were quantified using a novel high-performance liquid chromatography/ high-resolution mass spectrometry-time of flight method. This approach distinguishes between the isomeric compounds of MAs and benefits from the limited sample preparation required before analysis, and no extensive derivatization step is needed. The highest concentrations of levogucosan, galactosan, and mannosan (∑MA) were recorded in winter because of wood burning for residential heating (∑MA_MAX = 1,240 ng m^-3). This finding was substantiated by a relatively high correlation (R² = 0.64) between the levoglucosan concentration and decreasing ambient temperature. At the suburban site, ∑MA accounted for 3.1% of PM₁₀, whereas the corresponding level at the urban site was 0.6%. The mass size distribution of MAs associated with atmospheric aerosols was measured using a Berner cascade impactor. The size distribution was characterized with a single mode at 561 nm. Ninety-five percent of the mass concentration of the MAs was found to be associated with particles <2 µm. A preliminary attempt to estimate the contribution of wood burning to the mass concentration of PM₁₀ in Oslo using levoglucosan as a tracer indicates that 24% comes from wood burning. This is approximately a factor of 2 lower than estimated by the AirQUIS dispersion model.     

Gaseous mercury capture by coir fibre coated with a metal-halide

ABSTRACT

Toxic gaseous elemental mercury (GEM) is emitted to the atmosphere through a variety of routes at rates estimated at over 5000 tonnes per annum, a large fraction of which is Anthropogenic. It is then widely disbursed atmospherically and eventually deposited, where it is subject to further biogeochemical cycling, including re-emission. Research into capture of point source mercury emissions revolves almost exclusively around the use of activated carbons, various catalytic oxidation substrates, or as a by-product of acidic treatments of flue gas during SOx and NOx reduction methods. GEM is very non-reactive in its native state, but capture rates are greatly enhanced if GEM is first oxidized, or at least where oxidation states play a role at the substrate GEM interface. Little research has been devoted to capture of GEM directly. However, presented here is a novel adaption of coir fibers for use as a substrate in capturing GEM emissions directly. Various coir modifications were investigated, with the most effective being fibers coated with CuI crystals dispersed in a non-crosslinked poly-siloxane matrix. Scanning electron microscopy was used to view surface morphologies, and sorption characteristics were measured using atomic absorption spectroscopy (AAS). These results indicate that coir fibers modified by CuI-[SiO₂] _n show great promise in their ability to efficiently sorb GEM, and could potentially be utilized in a variety of configurations and settings where GEM emissions need to be captured.     

Capillary GC-MS analysis of PAH emissions from combustion of peat and wood in a hot water boiler

A preliminary investigation has been made on the emissions of Polynuclear Aromatic Hydrocarbons (PAH) when burning wood chips and peat in a modified commercial hot water boiler. The amount of the investigated eighteen PAH that were filter trapped from peat combustion averaged 2.7 times greater than that from wood combustion per cubic meter flue gas. The total emitted amount (particulate plus gas phase PAH) was 9.7 times greater than from wood combustion. The corresponding values for benzo(a)pyrene only were 1.7 and 3.5 times greater, respectively. The comparison of PAH emitted by the combustion of wood and peat showed a pronounced tendency towards the emission of high molecular weight PAH by the latter.Particulate phase-gas phase distribution ourves are presented for PAH in the boiling point range 336°C – 525°C. In addition, the emission of a polynuclear aromatic ketone is shown.     

Urban–rural differences in atmospheric mercury speciation

Measurements of gaseous elemental mercury (GEM), particulate mercury (Hg_p), and reactive gaseous mercury (RGM) were concurrently recorded at an urban site in Detroit and a rural site in Dexter, both in Michigan for the calendar year 2004. Their average concentrations (±standard deviation) for the urban area were 2.5 ± 1.4 ng m^?3, 18.1 ± 61.0 pg m^?3, and 15.5 ± 54.9 pg m^?3, respectively, while their rural counterparts were 1.6 ± 0.6 ng m^?3, 6.1 ± 5.5 pg m^?3, and 3.8 ± 6.6 pg m^?3, respectively. The medians of urban-to-rural ratios of Hg concentrations indicate approximately 1-fold, 2-fold, and 3-fold gradients between Detroit and Dexter for GEM, Hg_p, and RGM, respectively. The urban–rural differences in Hg also varied considerably on different temporal scales and with wind flow patterns, which was most evident in RGM. Our results show that while Hg at both sites was impacted by regional sources, meteorological conditions, and photochemical transformations, the extent of variations in the observed urban-to-rural gradients, particularly in RGM, cannot be fully accounted for by these processes. Both analyses of the annual data and case studies indicate that the more variable and episodic nature of Hg, particularly RGM, seen in Detroit compared with Dexter, was the result of direct impact from local anthropogenic sources.     

The fate and behavior of mercury in coal-fired power plants

For the past 22 years in the Netherlands, the behavior of Hg in coal-fired power plants has been studied extensively. Coal from all over the world is fired in Dutch power stations. First, the Hg concentrations in these coals were measured. Second, the fate of the Hg during combustion was established by performing mass balance studies. On average, 43 +/- 30% of the Hg was present in the flue gases downstream of the electrostatic precipitator (ESP; dust collector). In individual cases, this figure can vary between 1 and 100%. Important parameters are the Cl content of the fuel and the flue gas temperature in the ESP. On average, 54 +/- 24% of the gaseous Hg was removed in the wet flue-gas desulfurization (FGD) systems, which are present at all Dutch coal-power stations. In individual cases, this removal can vary between 8% (outlier) and 72%. On average, the fate of Hg entering the power station in the coal was as follows: <1% in the bottom ash, 49% in the pulverized fuel ash (ash collected in the ESP), 16.6% in the FGD gypsum, 9% in the sludge of the wastewater treatment plant, 0.04% in the effluent of the wastewater treatment plant, 0.07% in fly dust (leaving the stack), and 25% as gaseous Hg in the flue gases and emitted into the air. The distribution of Hg over the streams leaving the FGD depends strongly on the installation. On average, 75% of the Hg was removed, and the final concentration of Hg in the emitted flue gases of the Dutch power stations was only -3 microg/m3(STP) at 6% O2. During co-combustion with biomass, the removal of Hg was similar to that during 100% coal firing. Speciation of Hg is a very important factor. An oxidized form (HgCl2) favors a high degree of removal. The conversion from Hg0 to HgCl2 is positively correlated with the Cl content of the fuel. A catalytic DENOX (SCR) favors the formation of oxidized Hg, and, in combination with a wet FGD, the total removal can be as high as 90%.     

Dynamic exchange of gaseous elemental mercury during polar night and day

From February 29 until June 15 2008 gaseous elemental mercury (GEM) fluxes above a snow covered surface was measured in Ny-Ålesund, Svalbard using a GEM flux gradient method. A clear seasonal pattern in the meteorological variables associated with the GEM flux was observed. For the first time in Ny-Ålesund a net deposition of GEM was recorded during polar night, despite the lack of Atmospheric Mercury Depletion Events (AMDE). 7500 ng m⁻² GEM was emitted from the surface snow to the air during the entire study. The depositions of GEM and reactive gaseous mercury (RGM) were calculated to be 1500 and 1000 ng m⁻², respectively, during the same time period. The GEM fluxes reported in this study were found to be comparable to GEM fluxes measured at other Arctic locations (i.e. Alert and Barrow), suggesting that GEM acts in a similar way throughout the Arctic. An assessment of the GEM flux gradient method used discovered a non-linear GEM concentration profile. The nonlinearity was explained by a non-stationary turbulence regime. The GEM flux calculated was not found to be representative for the entire surface boundary layer.     

Effects of combustion and operating conditions on PCDD/PCDF emissions from power boilers burning salt-laden wood waste

This paper discusses the effects of combustion conditions on PCDD/PCDF emissions from pulp and paper power boilers burning salt-laden wood waste. We found no correlation between PCDD/PCDF emissions and carbon monoxide emissions. A good correlation was, however, observed between PCDD/PCDF emissions and the concentration of stack polynuclear aromatic hydrocarbons (PAHs) in the absence of TDF addition. Thus, poor combustion conditions responsible for the formation of products of incomplete combustion (PICs), such as PAHs and PCDD/PCDF precursors, increase PCDD/PCDF emissions. PAH concentrations increased with higher boiler load and/or low oxygen concentrations at the boiler exit, probably because of lower available residence times and insufficient excess air. Our findings are consistent with the current understanding that high ash carbon content generally favours heterogeneous reactions leading to either de novo synthesis of PCDD/PCDFs or their direct formation from precursors. We also found that, in grate-fired boilers, a linear increase in the grate/lower furnace temperature produces an exponential decrease in PCDD/PCDF emissions. Although the extent of this effect appears to be mill-specific, particularly at low temperatures, the results indicate that increasing the combustion temperature may decrease PCDD/PCDF emissions. It must be noted, however, that there are other variables, such as elevated ESP and stack temperatures, a high hog salt content, the presence of large amounts of PICs and a high Cl/S ratio, which contribute to higher PCDD/PCDFs emissions. Therefore, higher combustion temperatures, by themselves, will not necessarily result in low PCDD/PCDFs emissions.     

Dilution-based emissions sampling from stationary sources: Part 2--Gas-fired combustors compared with other fuel-fired systems

With the recent focus on fine particle matter (PM2.5), new, self-consistent data are needed to characterize emissions from combustion sources. Such data are necessary for health assessment and air quality modeling. To address this need, emissions data for gas-fired combustors are presented here, using dilution sampling as the reference. The dilution method allows for collection of emitted particles under conditions simulating cooling and dilution during entry from the stack into the air. The sampling and analysis of the collected particles in the presence of precursor gases, SO2 nitrogen oxide, volatile organic compound, and NH3 is discussed; the results include data from eight gas fired units, including a dual-fuel institutional boiler and a diesel engine powered electricity generator. These data are compared with results in the literature for heavy-duty diesel vehicles and stationary sources using coal or wood as fuels. The results show that the gas-fired combustors have very low PM2.5 mass emission rates in the range of approximately 10(-4) lb/million Btu (MMBTU) compared with the diesel backup generator with particle filter, with approximately 5 x 10(-3) lb/MMBTU. Even higher mass emission rates are found in coal-fired systems, with rates of approximately 0.07 lb/MMBTU for a bag-filter-controlled pilot unit burning eastern bituminous coal. The characterization of PM2.5 chemical composition from the gas-fired units indicates that much of the measured primary particle mass in PM2.5 samples is organic or elemental carbon and, to a much less extent, sulfate. Metal emissions are quite low compared with the diesel engines and the coal- or wood-fueled combustors. The metals found in the gas-fired combustor particles are low in concentration, similar in concentration to ambient particles. The interpretation of the particulate carbon emissions is complicated by the fact that an approximately equal amount of particulate carbon (mainly organic carbon) is found on the particle collector and a backup filter. It is likely that measurement artifacts, mostly adsorption of volatile organic compounds on quartz filters, are positively biasing "true" particulate carbon emission results.     

Factors influencing concentrations of dissolved gaseous mercury (DGM) and total mercury (TM) in an artificial reservoir

The effects of various factors including turbidity, pH, DOC, temperature, and solar radiation on the concentrations of total mercury (TM) and dissolved gaseous mercury (DGM) were investigated in an artificial reservoir in Korea. Episodic total mercury accumulation events occurred during the rainy season as turbidity increased, indicating that the TM concentration was not controlled by direct atmospheric deposition. The DGM concentration in surface water ranged from 3.6 to 160 pg/L, having a maximum in summer and minimum in winter. While in most previous studies DGM was controlled primarily by a photo-reduction process, DGM concentrations tracked the amount of solar radiation only in winter when the water temperature was fairly low in this study. During the other seasons microbial transformation seemed to play an important role in reducing Hg(II) to Hg(0). DGM increased as dissolved organic carbon (DOC) concentration increased (p-value < 0.01) while it increased with a decrease of pH (p-value < 0.01).     

Evidence for a significant contribution of wood burning aerosols to PM2.5 during the winter season in Paris,France

Although particulate emissions from residential wood burning have become a subject of great scientific concern for a few years, data related to their impact on the air quality of large European urban centres are still missing. In the present study, we investigated the chemical and optical properties of fine (PM_2.5) carbonaceous aerosols in Paris during the 2005 winter season in order to track the presence of wood burning emissions in such a large city. The use of a seven wavelength Aethalometer allowed us to document shortwave light absorption by brown-carbon-containing organic aerosols of biomass burning origin. In particular, a well-marked diurnal pattern of the spectral dependence of light absorption, with maxima during the night, could be observed every day of the campaign and attributed to wood burning emissions. Relatively high absorption Ångstrom exponents and WSOC/OC ratios (respectively 1.25 and 0.35 on average for the period of study) also indicated the importance of biomass burning aerosols in the Paris atmosphere in winter. Finally, a rough estimate of the contribution of wood burning carbonaceous aerosols to PM_2.5 could be achieved. This contribution was found to be as high as 20 ± 10% on average at the Paris background site investigated here.     

Characterization and seasonal variations of levoglucosan in fine particulate matter in Xi’an,China

PM_2.5 (particulate matter with an aerodynamic diameter <2.5 μm) samples (n = 58) collected every sixth day in Xi’an, China, from 5 July 2008 to 27 June 2009 are analyzed for levoglucosan (1,6-anhydro-β-d-glucopyranose) to evaluate the impacts of biomass combustion on ambient concentrations. Twenty-four-hour levoglucosan concentrations displayed clear summer minima and winter maxima that ranged from 46 to 1889 ng m^?3, with an average of 428 ± 399 ng m^?3. Besides agricultural burning, biomass/biofuel combustion for household heating with straws and branches appears to be of regional importance during the heating season in northwestern China. Good correlations (0.70 < R < 0.91) were found between levoglucosan relative to water-soluble K⁺, Cl^?, organic carbon (OC), elemental carbon (EC), and glyoxal. The highest levoglucosan/OC ratio of 2.3% was found in winter, followed by autumn (1.5%). Biomass burning contributed to 5.1–43.8% of OC (with an average of 17.6 ± 8.4%).

Implications:?PM_2.5 levoglucosan concentrations and the correlation between levoglucosan relative to other compounds during four seasons in Xi’an showed that the influence of biomass burning is maximum during the residential heating season (winter), although some important influences may be detected in spring (field preparation burnings) and autumn (corn stalks and wheat straw burning, fallen dead leaves burning) at Xi’an and surrounding areas. Household heating with biomass during winter was quite widespread in Guanzhong Plain. Therefore, the control of biomass/biofuel combustion could be an effective method to reduce pollutant emission on a regional scale.