Modeling of mercury emission,transport and deposition in North America

Most studies on the atmospheric behaviour of mercury in North America have excluded a detailed treatment of natural mercury emissions. The objective of this work is to report a detailed simulation of the atmospheric mercury in a domain that covers a significant part of North America and includes not only anthropogenic mercury emissions but also those from natural sources including vegetation, soil and water.The simulations were done using a natural mercury emission model coupled with the US EPA's SMOKE/CMAQ modelling system. The domain contained 132×90 grid cells at a resolution of 36 km, covering the continental United States, and major parts of Canada and Mexico. The simulation was carried out for 2002, using boundary conditions from a global mercury model. Estimated total natural mercury emission in the domain was 230 tonnes (1 tonne=1000 kg) and the ratio of natural to anthropogenic emissions varied from 0.7 in January to 3.2 in July. Average total gaseous mercury (TGM) concentration ranged between 1 and 4 ng m⁻³. Good agreement was found between the modelled results and measurements at three Ontario sites for ambient mercury concentrations, and at 72 mercury deposition network sites in the domain for wet deposition. The correlation coefficient between the simulated and the measured values of the daily average TGM at three monitoring sites varied between 0.48 and 0.64. When natural emissions were omitted, the correlation coefficients dropped to between 0.15 and 0.40. About 335 tonnes of mercury were deposited in the domain during the simulation period but overall, it acted as a net source of mercury and contributed about 21 tonnes to the global pool. The net deposition of mercury to the Great Lakes was estimated to be about 2.4 tonnes. The estimated deposition values were similar to those reported by other researchers.     

Evaluation of mercury emissions to the atmosphere from coal combustion,China

Mercury emissions from the coal smoke is the main source of anthropogenic discharge and mercury pollution in atmosphere. The calculated total amount of mercury emissions of China in 1995 is approximately 213.8 tonnes, which accounts for c. 5% of estimated total global discharge of 4000 tonnes in the same period. From 1978 to 1995, total coal consumption increased fourfold. Based on these data it is estimated that the mercury emissions will increase at a rate of 5% a year, and the predicted emissions will be 273 tonnes in China in 2000. Controlling and solving mercury emissions from coal combustion are among the most important environmental tasks facing China.     

Relating summer ambient particulate sulfur, sulfur dioxide, and light scattering to gaseous tracer emissions from the MOHAVE Power Project

Project MOHAVE was initiated in 1992 to examine the role of emissions from the 1580 MW coal-fired MOHAVE Power Project (MPP) on haze at the Grand Canyon National Park (GCNP), located about 130 km north-north-east of the power plant. Statistical relationships were analyzed between summertime ambient concentrations of a gaseous perfluorocarbon tracer released from MPP and ambient SO2, particulate sulfur, and light scattering to evaluate whether MPP's emissions could be transported to the GCNP and then impact haze levels there. Spatial analyses indicated that particulate sulfur levels were strongly correlated across the monitoring network, regardless of whether the monitoring stations were upwind or downwind of MPP. This indicates that particulate sulfur levels in this region were influenced by distant regional emission sources. A significant particulate sulfur contribution from a point source such as MPP would result in a non-uniform pattern downwind. There was no suggestion of this in the data. Furthermore, correlations between the MPP tracer and ambient particulate sulfur and light scattering at locations in the park were virtually zero for averaging times ranging from 24 hr to 1 hr. Hour-by-hour MPP tracer levels and light scattering were individually examined, and still no positive correlations were detected. Finally, agreement between tracer and particulate sulfur did not improve as a function of meteorological regime, implying that, even during cloudy monsoon days when more rapid conversion of SO2 to particulate sulfur would be expected, there was no evidence for downwind particulate sulfur impacts. Despite the fact that MPP was a large source of SO2 and tracer, neither time series nor correlation analyses were able to detect any meaningful relationship between MPP's SO2 and tracer emission "signals" to particulate sulfur or light scattering.     

Monitoring of PM10 and PM2.5 around primary particulate anthropogenic emission sources

Investigations on the monitoring of ambient air levels of atmospheric particulates were developed around a large source of primary anthropogenic particulate emissions: the industrial ceramic area in the province of Castelló (Eastern Spain). Although these primary particulate emissions have a coarse grain-size distribution, the atmospheric transport dominated by the breeze circulation accounts for a grain-size segregation, which results in ambient air particles occurring mainly in the 2.5–10 μm range. The chemical composition of the ceramic particulate emissions is very similar to the crustal end-member but the use of high Al, Ti and Fe as tracer elements as well as a peculiar grain-size distribution in the insoluble major phases allow us to identify the ceramic input in the bulk particulate matter. PM2.5 instead of PM10 monitoring may avoid the interference of crustal particles without a major reduction in the secondary anthropogenic load, with the exception of nitrate. However, a methodology based in PM2.5 measurement alone is not adequate for monitoring the impact of primary particulate emissions (such as ceramic emissions) on air quality, since the major ambient air particles derived from these emissions are mainly in the range of 2.5–10 μm. Consequently, in areas characterised by major secondary particulate emissions, PM2.5 monitoring should detect anthropogenic particulate pollutants without crustal particulate interference, whereas PM10 measurements should be used in areas with major primary anthropogenic particulate emissions.     

Relating Summer Ambient Particulate Sulfur,Sulfur Dioxide,and Light Scattering to Gaseous Tracer Emissions from the MOHAVE Power Project

ABSTRACT

Project MOHAVE was initiated in 1992 to examine the role of emissions from the 1580 MW coal-fired MOHAVE Power Project (MPP) on haze at the Grand Canyon National Park (GCNP), located about 130 km north-northeast of the power plant. Statistical relationships were analyzed between summertime ambient concentrations of a gaseous perfluorocarbon tracer released from MPP and ambient SO₂, particulate sulfur, and light scattering to evaluate whether MPP's emissions could be transported to the GCNP and then impact haze levels there. Spatial analyses indicated that particulate sulfur levels were strongly correlated across the monitoring network, regardless of whether the monitoring stations were upwind or downwind of MPP. This indicates that particulate sulfur levels in this region were influenced by distant regional emission sources. A significant particulate sulfur contribution from a point source such as MPP would result in a non-uniform pattern downwind. There was no suggestion of this in the data.

Furthermore, correlations between the MPP tracer and ambient particulate sulfur and light scattering at locations in the park were virtually zero for averaging times ranging from 24 hr to 1 hr. Hour-by-hour MPP tracer levels and light scattering were individually examined, and still no positive correlations were detected. Finally, agreement between tracer and particulate sulfur did not improve as a function of meteorological regime, implying that, even during cloudy monsoon days when more rapid conversion of SO₂ to par-ticulate sulfur would be expected, there was no evidence for downwind particulate sulfur impacts. Despite the fact that MPP was a large source of SO₂ and tracer, neither time series nor correlation analyses were able to detect any meaningful relationship between MPP's SO₂ and tracer emission “signals” to particulate sulfur or light scattering.     

Modeling Atmospheric Mercury Deposition in the Vicinity of Power Plants

Abstract

Two mathematical models of the atmospheric fate and transport of mercury (Hg), an Eulerian grid–based model and a Gaussian plume model, are used to calculate the atmospheric deposition of Hg in the vicinity (i.e., within 50 km) of five coal–fired power plants. The former is applied using two different horizontal resolutions: coarse (84 km) and fine (16.7 km). More than 96% of the power plant Hg emissions are calculated with the plume model to be transported beyond 50 km from the plants. The grid–based model predicts a lower fraction to be transported beyond 50 km: >91% with a coarse resolution and >95% with a fine resolution. The contribution of the power plant emissions to total Hg deposition within a radius of 50 km from the plants is calculated to be <8% with the plume model, <14% with the Eulerian model with a coarse resolution, and <10% with the Eulerian model with a fine resolution. The Eulerian grid–based model predicts greater local impacts than the plume model because of artificially enhanced vertical dispersion; the former predicts about twice as much Hg deposition as the latter when the area considered is commensurate with the resolution of the grid–based model. If one compares the local impacts for an area that is significantly less than the grid–based model resolution, then the grid–based model may predict lower local deposition than the plume model, because two compensating errors affect the results obtained with the grid–based model: initial dilution of the power plant emissions within one or more grid cells and enhanced vertical mixing to the ground.     

Impact of three interactive Texas state regulatory programs to decrease ambient air toxic levels

The Federal Clean Air Act (FCAA) framework envisions a federal-state partnership whereby the development of regulations may be at the federal level or state level with federal oversight. The U.S. Environmental Protection Agency (EPA) establishes National Ambient Air Quality Standards to describe “safe” ambient levels of criteria pollutants. For air toxics, the EPA establishes control technology standards for the 187 listed hazardous air pollutants (HAPs) but does not establish ambient standards for HAPs or other air toxics. Thus, states must ensure that ambient concentrations are not at harmful levels. The Texas Clean Air Act authorizes the Texas Commission on Environmental Quality (TCEQ), the Texas state environmental agency, to control air pollution and protect public health and welfare. The TCEQ employs three interactive programs to ensure that concentrations of air toxics do not exceed levels of potential health concern (LOCs): air permitting, ambient air monitoring, and the Air Pollutant Watch List (APWL). Comprehensive air permit reviews involve the application of best available control technology for new and modified equipment and ensure that permits protect public health and welfare. Protectiveness may be demonstrated by a number of means, including a demonstration that the predicted ground-level concentrations for the permitted emissions, evaluated on a case-by-case and chemical-by-chemical basis, do not cause or contribute to a LOC. The TCEQ's ambient air monitoring program is extensive and provides data to help assess the potential for adverse effects from all operational equipment in an area. If air toxics are persistently monitored at a LOC, an APWL area is established. The purpose of the APWL is to reduce ambient air toxic concentrations below LOCs by focusing TCEQ resources and heightening awareness. This paper will discuss examples of decreases in air toxic levels in Houston and Corpus Christi, Texas, resulting from the interactive nature of these programs.

Implications: Texas recognized through the collection of ambient monitoring data that additional measures beyond federal regulations must be taken to ensure that public health is protected. Texas integrates comprehensive air permitting, extensive ambient air monitoring, and the Air Pollutant Watch List (APWL) to protect the public from hazardous air toxics. Texas issues air permits that are protective of public health and also assesses ambient air to verify that concentrations remain below levels of concern in heavily industrialized areas. Texas developed the APWL to improve air quality in those areas where monitoring indicates a potential concern. This paper illustrates how Texas engaged its three interactive programs to successfully address elevated air toxic levels in Houston and Corpus Christi.     

Water striders (family Gerridae): mercury sentinels in small freshwater ecosystems

To circumvent some of the previous limitations associated with contaminant-monitoring programs, we tested the suitability of the water strider (Hemiptera: Gerridae) as a mercury sentinel by comparing total mercury concentrations in water striders and brook trout (Salvelinus fontinalis) from a variety of stream sites in New Brunswick, Canada. There was a strong association between the two variables across sites (r(2)=0.81, P<0.001) in systems where both atmospheric deposition and a point source (an abandoned gold mine) were likely contributing to ambient mercury levels. In a small stream draining the gold mine tailings pile, water striders had mercury concentrations an order of magnitude higher than those from reference locations. Temporal variation at three southern New Brunswick stream sites was non-significant. These results suggest that water strider mercury levels accurately quantify food chain entry of the element. The use of sentinel species holds great potential for expanding contaminant-monitoring programs.     

Mercury species measured atop the Moody Tower TRAMP site,Houston, Texas

Atmospheric mercury speciation was monitored within Houston, Texas, USA, August 6–October 14, 2006 as part of the TexAQS Radical and Aerosol Measurement Program (TRAMP). On average, all mercury levels were significantly elevated compared to a rural Gulf of Mexico coastal site. Concentrations varied from very clean to very dirty. Multi-day periods of stagnant or low-wind conditions brought elevated concentrations of all mercury species, whereas multi-day periods of strong winds, particularly southerly winds off the Gulf of Mexico, brought very low values of mercury species. Over the entire mercury measurement period, the daily averages of mercury species showed distinct and consistent relationships with the average planetary boundary layer dynamics, with gaseous elemental and particulate-bound mercury near-surface concentrations enhanced by a shallow nocturnal boundary layer, and reactive gaseous mercury concentration enhanced by midday convective boundary layer air entrainment transporting air aloft to the surface. Mercury concentrations were not significantly correlated with known products of combustion, likely indicating non-combustion mercury sources from the Houston area petrochemical complexes. On the morning of August 31, 2006 an observed emission event at a refinery complex on the Houston Ship Channel resulted in extremely high concentrations of aerosol mass and particulate-bound mercury at the TRAMP measurement site 20 km downwind.     

Chemical trends in Finnish wildlife: A study on time trends in starlings during 1967–1983

The OECD monitoring programmes 1966–1971 and 1972–1975 have been extended at national level in Finland to 1983 by analysing chlorinated hydrocarbons, mercury and chlorophenols in starlings (terrestrial environment). At the end of the study period levels in fresh muscles were for DDE 10, PCB 30, HCB 1, Lindan 8 and mercury 50 ppb. Of chlordane residues only traces of oxychlordane were found. Ten different chlorophenol compounds were detected at ppb levels, but most of them in only few samples. Pentachlorophenol was most frequently found. Statistical treatment of the analysis results gave some decreasing trends which were very significant for DDE, DDT and PCB 1967–1983, significant for mercury 1967–1983 and somewhat significant for lindane 1978–1983.     

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.     

Environmental toxins in Finnish Wildlife. A study on time trends of residue contents in fish during 1973–1978

The O.E.C.D. monitoring Wildlife Sampling and Analysis Programme 1973–1975 has been extended at national level in Finland to 1978 by analysing chlorinated hydrocarbon residues in fish at two marine and two freshwater environments and mercury at the latter two freshwater environments. Statistical treatment of the analysis results gave significant decreasing trends in most cases of PCB and DDT residues but in mercury levels no significant change was detected.     

Revealing source signatures in ambient BTEX concentrations

Management of ambient concentrations of Volatile Organic Compounds (VOCs) is essential for maintaining low ozone levels in urban areas where its formation is under a VOC-limited regime. The significant decrease in traffic-induced VOC emissions in many developed countries resulted in relatively comparable shares of traffic and non-traffic VOC emissions in urban airsheds. A key step for urban air quality management is allocating ambient VOC concentrations to their pertinent sources. This study presents an approach that can aid in identifying sources that contribute to observed BTEX concentrations in areas characterized by low BTEX concentrations, where traditional source apportionment techniques are not useful. Analysis of seasonal and diurnal variations of ambient BTEX concentrations from two monitoring stations located in distinct areas reveal the possibility to identify source categories. Specifically, the varying oxidation rates of airborne BTEX compounds are used to allocate contributions of traffic emissions and evaporative sources to observed BTEX concentrations.     

Mercury in sediment and fish communities of Lake Vänern, Sweden: recovery from contamination

The past effluents of mercury (Hg) into Lake V?nern were considerable. The consequences of, and recovery from these have been monitored through continuous measurements of mercury in sediment and fish. Mercury levels in lake sediments in the vicinity of the main source of mercury, a chloralkali plant on the northern shore, have only decreased by slightly more than a half since the mid-1970s, despite a radical decrease in effluents from the source, already during the 1960s. The mercury levels in pike (Esox lucius) have decreased to a similar extent during this time period. They are now about 30% higher in the worst affected parts of the lake compared to the least affected parts. Lower levels have been measured in perch (Perca fluviatilis) and salmonoid fish in the lake. Despite the increased presence of mercury in the sediment of Lake V?nern, the mercury levels in the fish of the lake are relatively low compared to fish in lakes situated in the same region, but not affected by any local mercury effluents. As calculated, the total fish biomass of L. V?nern holds less than 1000th of the amount of mercury contained in the upper, biologically active layers of the bottom sediment of the lake. This demonstrates the potential influence of various environmental factors and motivates continued monitoring of mercury levels in the lake in the future.     

Luncheon Address

ABSTRACT

The U.S. Department of Energy (DOE), through the Federal Energy Technology Center (FETC), manages the largest funded program in the country for developing (1) an understanding of mercury emissions, (2) measurement of these emissions, and (3) control technology (-ies) for these emissions for the U.S. coal-fired electric generating industry. DOE has initiated, or has collaborated with other government and industrial organizations in, these and other efforts relating to mercury and other hazardous air pollutants (HAPs), also known as air toxics. One of DOE's first reports on trace elements in coal was conducted from 1976 through 1978 by researchers at DOE's Pittsburgh Energy Technology Center (PETC, now FETC) and the Pittsburgh Mining Operations of the Department of the Interior's Bureau of Mines. The report was completed less than two years after DOE was formed, and 13 years before Title III of the 1990 Clean Air Act Amendments was enacted (Cavallaro et al., March 1978).     

Impact of emissions from natural gas production facilities on ambient air quality in the Barnett Shale area: A pilot study

Rapid and extensive development of shale gas resources in the Barnett Shale region of Texas in recent years has created concerns about potential environmental impacts on water and air quality. The purpose of this study was to provide a better understanding of the potential contributions of emissions from gas production operations to population exposure to air toxics in the Barnett Shale region. This goal was approached using a combination of chemical characterization of the volatile organic compound (VOC) emissions from active wells, saturation monitoring for gaseous and particulate pollutants in a residential community located near active gas/oil extraction and processing facilities, source apportionment of VOCs measured in the community using the Chemical Mass Balance (CMB) receptor model, and direct measurements of the pollutant gradient downwind of a gas well with high VOC emissions. Overall, the study results indicate that air quality impacts due to individual gas wells and compressor stations are not likely to be discernible beyond a distance of approximately 100 m in the downwind direction. However, source apportionment results indicate a significant contribution to regional VOCs from gas production sources, particularly for lower-molecular-weight alkanes (<C6). Although measured ambient VOC concentrations were well below health-based safe exposure levels, the existence of urban-level mean concentrations of benzene and other mobile source air toxics combined with soot to total carbon ratios that were high for an area with little residential or commercial development may be indicative of the impact of increased heavy-duty vehicle traffic related to gas production

ImplicationsRapid and extensive development of shale gas resources in recent years has created concerns about potential environmental impacts on water and air quality. This study focused on directly measuring the ambient air pollutant levels occurring at residential properties located near natural gas extraction and processing facilities, and estimating the relative contributions from gas production and motor vehicle emissions to ambient VOC concentrations. Although only a small-scale case study, the results may be useful for guidance in planning future ambient air quality studies and human exposure estimates in areas of intensive shale gas production.     

Source attribution and quantification of benzene event emissions in a Houston ship channel community based on real-time mobile monitoring of ambient air

A mobile laboratory equipped with a proton transfer reaction mass spectrometer (PTR-MS) operated in Galena Park, Texas, near the Houston Ship Channel during the Benzene and other Toxics Exposure Study (BEE-TEX). The mobile laboratory measured transient peaks of benzene of up to 37 ppb_v in the afternoon and evening of February 19, 2015. Plume reconstruction and source attribution were performed using the four-dimensional (4D) variational data assimilation technique and a three-dimensional (3D) micro-scale forward and adjoint air quality model based on mobile PTR-MS data and nearby stationary wind measurements at the Galena Park Continuous Air Monitoring Station (CAMS). The results of inverse modeling indicate that significant pipeline emissions of benzene may at least partly explain the ambient concentration peaks observed in Galena Park during BEE-TEX. Total pipeline emissions of benzene inferred within the 16-km² model domain exceeded point source emissions by roughly a factor of 2 during the observational episode. Besides pipeline leaks, the model also inferred significant benzene emissions from marine, railcar, and tank truck loading/unloading facilities, consistent with the presence of a tanker and barges in the Kinder Morgan port terminal during the afternoon and evening of February 19. Total domain emissions of benzene exceeded corresponding 2011 National Emissions Inventory (NEI) estimates by a factor of 2–6.

Implications:?Port operations involving petrochemicals may significantly increase emissions of air toxics from the transfer and storage of materials. Pipeline leaks, in particular, can lead to sporadic emissions greater than in emission inventories, resulting in higher ambient concentrations than are sampled by the existing monitoring network. The use of updated methods for ambient monitoring and source attribution in real time should be encouraged as an alternative to expanding the conventional monitoring network.     

Fine Particulate Matter Emissions Inventories: Comparisons of Emissions Estimates with Observations from Recent Field Programs

Abstract

Emissions inventories of fine particulate matter (PM_2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM_2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM_2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5–20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM_2.5 are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM_2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Recent trends of persistent organic pollutants in air in central Europe - Air monitoring in combination with air mass trajectory statistics as a tool to study the effectivity of regional chemical policy

We use air mass back trajectory analysis of persistent organic pollutant (POP) levels monitored at a regional background site, Ko?etice, Czech Republic, as a tool to study the effectiveness of emission reduction measures taken in the last decade in the region. The representativity of the chosen trajectory starting height for air sampling near ground was ensured by excluding trajectories starting at time of inversions lower than their starting height. As the relevant pollutant sources are exclusively located in the atmospheric boundary layer, trajectory segments above this layer were also excluded from the analysis. We used a linear time weight to account for the influence of dispersion and deposition on trace components abundances and to quantify the ground source loading, a continuous measure for the influence of surface emissions. Hexachlorocyclohexanes (HCHs), hexachlorobenzene (HCB), polychlorinated biphenyls (PCBs), DDT, and two time periods, the years 1997–1999 and 2004–2006, were studied. The pollutant levels transported to Ko?etice decreased for all substances except HCB. Except for lindane seasonal emissions were insignificant. Increasing emissions of HCB were at least partly linked to the 2002 floods in the Danube basin. Major emissions of 1997–1999 which decreased significantly were in France (lindane), western Poland, Hungary and northern ex-Yugoslavia (technical HCH), and the Czech Republic (DDT). Emissions remaining in 2004–2006 include HCB and DDT in the northern Czech Republic, HCB and PCBs in Germany. Besides changes in emission strength meteorological factors influence the level of transported pollutant concentrations. The prevailing air flow pattern limits the geographic coverage of this analysis to central Europe and parts of western Europe. However, no POP monitoring stations exist in areas suitable for a possible extension of the study area.     

Air quality at Santiago,Chile: a box modeling approach II. PM2.5, coarse and PM10 particulate matter fractions

Ambient monitored data at Santiago, Chile, are analyzed using box models with the goal of assessing contributions of different economic activities to air pollution levels. The box modeling approach was applied to PM₁₀, PM_2.5 and coarse (PM₁₀–PM_2.5) particulate matter (PM) fractions; the period analyzed is 1989–1999. A linear model for each PM fraction was obtained, having as independent variables CO and SO₂ concentrations, plus a term proportional to (wind speed)⁻¹ that lumps together non-combustion emissions and secondary generation terms; wet scavenging is included as another independent variable. Model identification results show good agreement for the different parameters across monitoring stations. The washout ratios and scavenging coefficients agree with data published in the literature, being higher for the coarse PM fraction. The CO and SO₂ coefficients fitted for 1989–1995 agree with a priori estimates for the same period. Background estimates for the PM fractions are in agreement with measurement campaigns in upwind sites. Results show that transportation sources have become the dominant contributors to ambient PM levels, while stationary sources have decreased their contributions in the last years. The relative importance of mobile sources to PM_2.5 ambient concentrations has doubled in the last 10 years, whereas stationary sources have reduced their relative contributions to half the value in the early 1990s. Model estimates of regional background of PM_2.5 and PM₁₀ have decreased 50% and 22% in the last decade, respectively; coarse background has shown no significant change. The final conclusion is that there is room and need for a more intensive emission reduction strategy for Santiago, focusing on mobile sources. The approach pursued in this work is feasible for cities or regions where comprehensive, transport and chemistry models are not available yet, but estimates of air quality contributions are needed for policy purposes. The methodology requires data on ambient air quality measurements and surface meteorology.