Estimation of source locations of total gaseous mercury measured in New York State using trajectory-based models

Ambient gaseous phase mercury concentrations (TGM) were measured at three locations in NY State including Potsdam, Stockton, and Sterling from May 2000 to March 2005. Using these data, three hybrid receptor models incorporating backward trajectories were used to identify source areas for TGM. The models used were potential source contribution function (PSCF), residence time weighted concentration (RTWC), and simplified quantitative transport bias analysis (SQTBA). Each model was applied using multi-site measurements to resolve the locations of important mercury sources for New York State.PSCF results showed that southeastern New York, Ohio, Indiana, Tennessee, Louisiana, and Virginia were important TGM source areas for these sites. RTWC identified Canadian sources including the metal production facilities in Ontario and Quebec, but US regional sources including the Ohio River Valley were also resolved. Sources in southeastern NY, Massachusetts, western Pennsylvania, Indiana, and northern Illinois were identified to be significant by SQTBA. The three modeling results were combined to locate the most important probable source locations, and those are Ohio, Indiana, Illinois, and Wisconsin. The Atlantic Ocean was suggested to be a possible source as well.     

Contributions of global and regional sources to mercury deposition in New York State

A modeling system that includes a global chemical transport model (CTM) and a nested continental CTM (TEAM) was used to simulate the atmospheric transport, transformations and deposition of mercury (Hg). Three scenarios were used: (1) a nominal scenario, (2) a scenario conducive to local deposition and (3) a scenario conducive to long-range transport. Deposition fluxes of Hg were analyzed at three receptor locations in New York State. For the nominal scenario, the anthropogenic emission sources (including re-emission of deposited Hg) in New York State, the rest of the contiguous United States, Asia, Europe, and Canada contributed 11-1, 25-9, 13-19, 5-7, and 2-5%, respectively to total Hg deposition at these three receptors. Natural sources contributed 16-4%. The results from the local deposition and long-range transport scenarios varied only slightly from these results. However, there are still uncertainties in our understanding of the atmospheric chemistry of Hg that are likely to affect these estimates of local, regional and global contributions. Comparison of model simulation results with data from the Mercury Deposition Network suggests that local and regional contributions may currently be overestimated.     

Rural and Urban Ozone Relationships In New York State

High ozone concentrations, often in excess of the national ambient air quality standard for photochemical oxidants, have been measured simultaneously in urban and rural areas of New York State. Average daily rural ozone concentrations were found to correlate well with daily maximum urban ozone concentrations suggesting a common source. Estimations of the quantity of ozone advectively transported into New York State are more than an order of magnitude greater than estimations of the potential photochemical generation of ozone from hydrocarbon emissions within New York State. It is suggested thai the high rural ozone levels are not primarily due to the transport of ozone and ozone precursors from olher urban areas, but are rather due to natural phenomena such as photochemical generation from naturally occurring precursors or transport of ozone from the stratosphere to the troposphere. The effectiveness of a hydrocarbon control strategy for New York State to meet the ambient air quality standard for photochemical oxidants when background levels themselves may be above the standard is questioned.     

Concentrations and trends of benzene in ambient air over New York State during 1990–2003

Since 1990s, a systematic program to measure air toxics has been active in New York State with monitors located both in urban and rural areas. In this study we examined the spatial and temporal characteristics of benzene, a known human carcinogen that is emitted by many source categories. The analysis indicates that ambient concentration levels of benzene have decreased by as much as 60% over this period not only in the ozone non-attainment area of New York City that had the reformulated gas (RFG) requirements, but also over the rest of the state as well. Although the rate of decrease appears to have flattened out in recent years, the annual average concentration levels are found to be above the health risk threshold even at the remote location, Whiteface Mountain, suggesting the need for further reductions in benzene emissions.     

NCAQ Report to Congress: Review and Response

Airborne measurements of gaseous and particulate sulfur and nitrogen pollutants were made in southwestern Kentucky on the afternoon of October 21, 1979. Back-trajectory analysis indicates that the sampled air parcel moved over northern Florida, Alabama, and western Tennessee during the two days prior to sampling. Before moving over Florida, the air parcel was over the Atlantic Ocean for at least five days. Analytical long-range transport (LRT) model predictions based on anthropogenic emissions account for only about 75% of the airborne measured concentrations of 14.7 μg m^?3 for SO₂ and 4.8 μg m^?3 for SO₄ ^2?. The remaining 25 % is thought to be due to biogenic sulfur emissions from the extensive wetland areas along the Gulf Coast.

Forward-trajectory analysis indicates that the air parcel moved to the Adirondack Mountains of New York State 24 hours after sampling. Model predictions indicate that SO₂ and SO₄ ^2? mean layer concentrations at the Adirondacks were 24 and 16 μg^?3, respectively. Almost half of this sulfur was estimated to come from emissions in the heavily industrialized region along the Ohio River Valley.

Further comparisons used a measurement data base obtained in southeastern Canada and the state of Arkansas during August 1976. An air parcel was tracked for seven days as it entered the north central United States, stagnated over the lower midwest, and then moved to eastern Canada. Model predictions were in substantial agreement with regional SO₄ ^2? concentrations measured at a number of ground-level sites. Average SO₄ ^2? concentrations measured in central Arkansas on August 10, 1976 were 20 μ m^?3 vs. a modeled value of 19 μ m^?3. Average SO₄ ^2? concentrations measured in Nova Scotia four days later were 22 μg^?3 vs. a modeled estimate of 24 μg^?3.     

Statistical Analysis of Trends in Urban Ozone Air Quality

The purpose of this paper is to demonstrate the use of some statistical methods for examining trends in ambient ozone air quality downwind of major urban areas. To this end, daily maximum 1 -hr ozone concentrations measured over New Jersey, metropolitan New York City and Connecticut for the period 1980 to 1989 were assembled and analyzed. This paper discusses the application of the bootstrap method, extreme value statistics and a nonparametric test for evaluating trends in urban ozone air quality. The results indicate that although there is an improvement in ozone air quality downwind of New York City, there has been little change in ozone levels upwind of New York City during this ten-year period.     

An Air Pollution Incident Due to a Stationary Front

In January 1971, the New York City area experienced a period of high pollution in which concentrations exceeded the present criteria for Stage I of the New York City Alert-Warning System. The incident was unusual because the high concentrations were associated with a weak frontal system which moved back and forth over the area and not with a stagnating anticyclone. Concentrations of pollutants were found to be closely related to the movement of the frontal system as well as to changes in wind speed and stability. Climatological criteria for identifying-periods of potential high air pollution and the criteria for mixing heights, transport wind speed and ventilation factors necessary for the issuance of an official advisory from the National Meteorological Center were not met during this incident. Therefore, some re-evaluation and redefinition of these criteria are recommended.     

Seasonal variation of levoglucosan in aerosols over the western North Pacific and its assessment as a biomass-burning tracer

Levoglucosan is considered as a useful molecular tracer of biomass-burning aerosols in the atmosphere. To characterize the seasonal variation of its concentrations over the Pacific Ocean and to assess its usefulness as a tracer after long-range transport, we investigated long-term variations of levoglucosan over Chichi-jima in the western North Pacific, from 2001 to 2004. Organic carbon (OC), elemental carbon (EC) and d-glucose were analyzed for comparison. The seasonal variation of levoglucosan concentrations showed a maximum in the winter, which is consistent with the enhanced Asian outflow to the Pacific indicated by backward air-mass trajectories. The concentration levels of levoglucosan estimated from global aerosol model outputs in the winter are, on average, comparable to the observed levels, suggesting that a considerable fraction of levoglucosan did not decompose during long-range transport from the Asian continent by westerly/northwesterly winds. This result is supported by comparable ratios of levoglucosan to EC in Chichi-jima and the East Asian coastal region. Conversely, the measured concentrations of levoglucosan in the summer were significantly lower than the modeled one. This implies a degradation of levoglucosan in the air masses that stagnated over the Pacific, although uncertainties in the model estimate may also be partly responsible for this discrepancy. One possible degradation pathway is oxidation by OH radicals; the contribution of acid-catalyzed reactions needs further investigation.     

Long-range transport of yellow sand to Taiwan in Spring 2000: observed evidence and simulation

More than 10 Asian dust storms occurring in Spring 2000 were found to transport dust long distances, with some fallout reaching as far as Taiwan. An air quality data set from Taiwan clearly shows that long-range transport of yellow-sand results in air quality in Taiwan, which is categorized as “Unhealthy” or “Very Unhealthy”. Backward trajectory analysis indicates that, for air parcels that arrived over Taiwan on 28 April, two or three days are required for transport from source regions, such as Inner Mongolia, a territory that is becoming a desert as a result of over-use and destruction of vegetation cover by human occupants. Furthermore, a 3-D long-range transport model for yellow sand, with an advanced size-dependent deflation module and driven by the NCAR/Penn State Fifth-Generation Mesoscale Model (MM5), is used to identify the long-range transport of yellow sand to Taiwan in April. Comparisons between observations and model calculations indicate that the model is able to reproduce some key features of the long-range transport. Transport of yellow sand to Taiwan is found to occur most easily when dust storms occurring in north China are accompanied by a high-pressure system located over the west of Japan. The high concentrations of yellow sand transported over Taiwan are usually between 500 and 1500 m high, not at the surface.     

Assessing the effects of transboundary ozone pollution between Ontario,Canada and New York,USA

We investigated the effects of transboundary pollution between Ontario and New York using both observations and modeling results. Analysis of the spatial scales associated with ozone pollution revealed the regional and international character of this pollutant. A back-trajectory-clustering methodology was used to evaluate the potential for transboundary pollution trading and to identify potential pollution source regions for two sites: CN tower in Toronto and the World Trade Center in New York City. Transboundary pollution transport was evident at both locations. The major pollution source areas for the period examined were the Ohio River Valley and Midwest. Finally, we examined the transboundary impact of emission reductions through photochemical models. We found that emissions from both New York and Ontario were transported across the border and that reductions in predicted O3 levels can be substantial when emissions on both sides of the border are reduced.     

The concurrent observation of methyl iodide and dimethyl sulphide in marine air; implications for sources of atmospheric methyl iodide

Continuous atmospheric measurements of methyl iodide and dimethyl sulphide were carried out at Mace Head, western Ireland, over a 4-week period in July 1996. The concurrent observations of methyl iodide and dimethyl sulphide reported here display a clear association, indeed statistical analysis indicated a very significant degree of covariance. A simple yet informative use of modelled 5-day back trajectories was employed in tandem with examination of local meteorology to illuminate the geographical source regions of methyl iodide and dimethyl sulphide. The interpretation of the atmospheric observations in terms of air-mass flow has elucidated part of the global methyl iodide cycle and provides evidence for two distinct source regions of methyl iodide:1. Under certain synoptic meteorological conditions, long-range transport of methyl iodide and dimethyl sulphide was observed from discrete areas of the sub-tropical Atlantic Ocean located in a region between 30–50°N and 20–50°W.2. Measurements taken under different conditions led us to believe that there was an additional source of methyl iodide that influenced the Mace Head atmosphere, most likely produced by coastal macroalgae which inhabit waters off the western coast of Ireland.     

New York State’s Action for Clean Air Program

In New York State there is a tradition of teamwork between industry and government toward air pollution control programs. This was demonstrated initially when Associated Industries assisted in writing New York State’s Air Pollution Control Law. Industry in New York State has accepted a two-way responsibility for educating industry and the public. New York State’s Department of Public Health has organized an “Action for Clean Air” program and Associated Industries of New York has joined with official agencies in promoting the public information program to lessen the possibility of hysteria.     

Analysis of long-range transport influences on urban PM10 using two-stage atmospheric trajectory clusters

There is evidence that long-range transport of natural and/or anthropogenic particles can have a negative impact on urban air quality. Certain European cities may fail to comply with the currently implemented 24-h PM₁₀ limit value due to the additional impact of remote sources of particles, which are not controllable at local level. For that reason, reliable methodologies identifying long-range transport patterns and quantifying their contribution to urban PM₁₀ levels are required. In this study, a two-stage clustering methodology was developed and applied to back trajectories arriving in three European cities: Athens, Madrid and Birmingham, which experience large, moderate and small numbers of daily PM₁₀ episodes, respectively. The atmospheric trajectories used in this analysis were computed with HYSPLIT model (NOAA) for a 3-year period. The two-stage cluster analysis has the advantage of providing highly disaggregated trajectory clusters, which proved to correspond to significantly different PM₁₀ levels. In the case of Madrid and Birmingham, clusters of trajectories originating from North Africa and continental Europe, respectively, were strongly associated with the highest PM₁₀ levels recorded in selected monitoring stations. In Athens, long-range transport patterns and trans-boundary influences were less evident, which highlighted the more substantial impact of local emission sources. Finally, two simple statistical indexes were proposed for assessing PM₁₀ episodes associated with different clusters of trajectories. This study has established a practical methodology for examining the impact of long-range atmospheric transport on local air quality, without resorting to high resource-demanding source apportionment techniques.     

New York State urban and rural measurements of continuous PM2.5 mass by FDMS, TEOM, and BAM

Field evaluations and comparisons of continuous fine particulate matter (PM2,5) mass measurement technologies at an urban and a rural site in New York state are performed. The continuous measurement technologies include the filter dynamics measurement system (FDMS) tapered element oscillating microbalance (TEOM) monitor, the stand-alone TEOM monitor (without the FDMS), and the beta attenuation monitor (BAM). These continuous measurement methods are also compared with 24-hr integrated filters collected and analyzed under the Federal Reference Method (FRM) protocol. The measurement sites are New York City (the borough of Queens) and Addison, a rural area of southwestern New York state. New York City data comparisons between the FDMS TEOM, BAM, and FRM are examined for bias and seasonality during a 2-yr period. Data comparisons for the FDMS TEOM and FRM from the Addison location are examined for the same 2-yr period. The BAM and FDMS measurements at Queens are highly correlated with each other and the FRM. The BAM and FDMS are very similar to each other in magnitude, and both are approximately 25% higher than the FRM filter measurements at this site. The FDMS at Addison measures approximately 9% more mass than the FRM. Mass reconstructions using the speciation trends network filter data are examined to provide insight as to the contribution of volatile species of PM2.5 in the FDMS mass measurement and the fraction that is likely lost in the FRM mass measurement. The reconstructed mass at Queens is systematically lower than the FDMS by approximately 10%.     

Comparison of constant volume balloons, model trajectories and tracer transport during ETEX

In the field phases of the European Tracer EXperiment (ETEX), an inert tracer was released for 12 h into the atmosphere and samples taken at several locations downwind. During the same time, several Constant Volume Balloons (CVB) (10 and 6 for ETEX first and second release, respectively) were launched into different altitudes and followed as far as 21–188 km, to indicate the initial dispersion directions of the tracer puff. A model simulating the CVB behaviour in hydrostatic meso-scale model forecasts is applied to ETEX data to demonstrate its capability to predict the tracer puff mean axis over long distances (−2000 km). CVB model results are first compared to air parcels trajectories and 2D (i.e. isentropic, isobaric and isodensity) trajectories. Then they are compared to the measured CVB trajectories and finally to the tracer puff trajectories. As expected, the CVB model and isodensity model trajectories are found to be identical. The 16 CVBs calculated trajectories nearly overlap the real ones over 21–188 km with mean absolute horizontal transport deviations less than 20 km (average value of 8.2 km). The corresponding relative transport deviations are less than 45% with an average value of 20.6%. Better predictions are obtained for the ETEX second release. During the 60 h following ETEX’s first release start, the simulated CVBs are mainly found in the area of the maximum surface concentrations of the released tracer, up to 2000 km. Up to 36 h after ETEX second tracer release start, the simulated CVB trajectories predict well the mean axis of the tracer puff, but failed later.     

High ozone levels in the northeast of Portugal: Analysis and characterization

Each summer period extremely high ozone levels are registered at the rural background station of Lamas d'Olo, located in the Northeast of Portugal. In average, 30% of the total alert threshold registered in Portugal is detected at this site. The main purpose of this study is to characterize the atmospheric conditions that lead to the ozone-rich episodes at this site. Synoptic patterns anomalies and back trajectories cluster analysis were performed, for the period between 2004 and 2007, considering 76 days when ozone maximum hourly concentrations were above 200 μg m^?3. The obtained atmospheric anomaly fields suggested that a positive temperature anomaly is visible above the Iberian Peninsula. A strong wind flow pattern from NE is observable in the North of Portugal and Galicia, in Spain. These two features may lead to an enhancement of the photochemical production and to the transport of pollutants from Spain to Portugal. In addition, the 3D mean back trajectories associated to the ozone episode days were analysed. A clustering method has been applied to the obtained back trajectories. Four main clusters of ozone-rich episodes were identified, with different frequencies of occurrence: north-westerly flows (11%); north-easterly flows (45%), southern flow (4%) and westerly flows (40%). Both analyses highlight the NE flow as a dominant pattern over the North of Portugal during summer. The analysis of the ozone concentrations for each selected cluster indicates that this northeast circulation pattern, together with the southern flow, are responsible for the highest ozone peak episodes. This also suggests that long-range transport of atmospheric pollutants is the main contributor to the ozone levels registered at Lamas d'Olo. This is also highlighted by the correlation of the ozone time-series with the meteorological parameters analysed in the frequency domain.     

Ozone Transport

Elevated concentrations of ozone, often above the national ambient air quality standard for photochemical oxidants, have been measured in both urban and rural areas of Connecticut. One such episode took place on June 10, 1974. Ozone levels, after stabilizing at values slightly above the standard (i.e., 80 to 110 ppb; Connecticut generated ozone concentrations), rose sharply late in the afternoon reaching concentrations as high as 310 ppb (almost 4 times the standard) in Hartford. The trajectory of the air mass, which arrived in Hartford at the time of maximum O₃ occurence, had its origin in the metropolitan New York area during the early morning rush hour on the episode day. This illustrates that the advective transport of O₃ and O₃ precursors into Connecticut from New York are probably responsible for a significant portion (approximately two-thirds) of the elevated O₃ concentrations measured throughout Connecticut on days when winds are from the south-southwest direction. The fact that peak O₃ levels occur late in the afternoon, several hours after maximum sunlight intensity, reinforces the conclusion that excessive O₃ concentrations developed as O₃ and ozone precursors were generated in the vicinity of New York City and then drifted inland into Connecticut on the afternoon sea breeze.

It appears to be unrealistic to develop a hydrocarbon control strategy for Connecticut in order to meet the photochemical oxidant ambient air quality standard when O₃ and/or ozone precursors ad-vectively transported into the State cause oxidant levels to exceed the standard. The complete cessation of all anthropogenic hydrocarbon emissions in Connecticut would not necessarily assure that the standard would be attained here. The implication is that a regional (i.e., the eastern part of the United States) hydrocarbon control strategy is needed to reduce adequately ozone formation and transport so as to allow Connecticut to meet the current oxidant standard.     

Air Pollution Patterns In New York City

Some preliminary analyses of data selected from three years of smoke shade and sulfur dioxide measurements from the forty air monitoring stations in New York City are presented. The purpose of these analyses is to investigate the spatial-temporal variation in concentration of these pollutants throughout the five boroughs of the city. Air pollution health effects studies in New York City have often used city-wide daily morbidity or mortality statistics and related them to air pollution levels obtained from a single monitoring station. The question of whether readings at one station in New York City can adequately represent the air pollution exposure for the population in the five boroughs is examined in this paper. Some samples of correlation matrices of daily pollution averages obtained from the forty air monitoring stations are presented to illustrate the day-to-day variation in pollution in various sections of New York City. It was found that interstation correlations are not high enough to justify the use of one central pollution measuring station as representative of a large metropolitan area. Sulfur dioxide correlates better between stations than smoke shade; this may reflect the different nature and spatial distribution of sources of the two pollutants. Close proximity of stations, or the fact that they were at similar heights above street or sea level did not necessarily lead to higher correlation coefficients.     

Seasonal Ozone Levels and Control by Seasonal Meteorology

Meteorological data, particularly 850-MB level temperatures, for Fort Totten, New York (1980) and Atlantic City, New Jersey (1981-1988) were examined for any relationship to seasonal ozone levels. Other radiosonde stations in the Northeast were utilized for 1983 and 1986, years of widely differing ozone levels. Statistics for selected parameters and years are presented.

Emphasis is placed on recurring warm temperature regimes in high ozone years. Successive occurrences or episodes of high temperatures characterize seasonally high ozone years. Seasonally persistent high temperatures are related to seasonally chronic high ozone. An example is presented relating the broad-scale climatologlcally anomalous pattern of high temperatures to anomalous circulation patterns at the 700-MB level.     

Fine urban and precursor emissions control for diesel urban transit buses

Particulate emission from diesel engines is one of the most important pollutants in urban areas. As a result, particulate emission control from urban bus diesel engines using particle filter technology is being evaluated at several locations in the US. A project entitled "Clean Diesel Air Quality Demonstration Program" has been initiated by the New York City Metropolitan Transit Authority (MTA) under the supervision of New York State Department of Environmental Conservation and with active participation from Johnson Matthey, Corning, Equilon, Environment Canada and RAD Energy. Under this program, several MTA transit buses with DDC Series 50 engines were equipped with Continuously Regenerating Technology (CRTTM) particulate filter systems and have been operated with ultra low sulfur diesel (<30 ppm S) in transit service in Manhattan since February 2000. These buses were evaluated over a 9-month period for durability and maintainability of the particulate filter. In addition, an extensive emissions testing program was carried out using transient cycles on a chassis dynamometer to evaluate the emissions reductions obtained with the particle filter. In this paper, the emissions testing data from the Clean Diesel Air Quality Demonstration Program are discussed in detail.