The sensitivity of the CHIMERE model to emissions reduction scenarios on air quality in Northern Italy

The sensitivity of the CHIMERE model to emission reduction scenarios on particulate matter PM2.5 and ozone (O₃) in Northern Italy is studied. The emissions of NO_x, PM2.5 SO₂, VOC or NH₃ were reduced by 50% for different source sectors for the Lombardy region, together with 5 additional scenarios to estimate the effect of local measures on improving the air quality for the Po valley area. Firstly, we evaluate the model performance by comparing calculated surface aerosol concentrations for the standard case (no emission reductions) with observations for January and June 2005. Calculated monthly mean PM10 concentrations are in general underestimated. For June, modelled PM10 concentrations slightly overestimate the measurements. Calculated monthly mean SO₄, NO₃^?, NH₄⁺ concentrations are in good agreement with the observations for January and June. Secondly, the model sensitivity of emission reduction scenarios on PM2.5 and O₃ calculated concentrations for the Po valley area is evaluated. The most effective scenarios to abate PM2.5 concentration are based on the SNAP2 (non-industrial combustion plants) and SNAP7 (road traffic) sectors, for which the NO_x and PM2.5 emissions are reduced by 50%. The number of days that the 2015 PM2.5 limit value of 25 μg m^?3 in Milan is exceeded by reducing primary PM2.5 and NO_x emissions for SNAP2 and 7 by 50%, does not change in January when compared to the standard case for the Milan area. It appears that 40% of the PM2.5 concentration in the greater Milan area is caused by the emissions surrounding the Lombardy region and from the model boundary conditions.This study also showed that a more effective pollutant reduction (emissions) per ton of pollutant reduced (concentrations) for the greater Milan area is obtained by reducing the primary PM2.5 emissions for SNAP7 by 50%. The most effective scenario on PM2.5 decrease for which precursor emissions are reduced is achieved by reducing SO₂ emissions by 50% for SNAP7.Our study showed that during summer time, the largest reductions in O₃ concentrations are achieved for SNAP7 emission reductions, when volatile organic compounds (VOCs) are reduced by 50%.     

Assessment of air quality benefits from national air pollution control policies in China. Part II: Evaluation of air quality predictions and air quality benefits assessment

Following the meteorological evaluation in Part I, this Part II paper presents the statistical evaluation of air quality predictions by the U.S. Environmental Protection Agency (U.S. EPA)’s Community Multi-Scale Air Quality (Models-3/CMAQ) model for the four simulated months in the base year 2005. The surface predictions were evaluated using the Air Pollution Index (API) data published by the China Ministry of Environmental Protection (MEP) for 31 capital cities and daily fine particulate matter (PM_2.5, particles with aerodiameter less than or equal to 2.5 μm) observations of an individual site in Tsinghua University (THU). To overcome the shortage in surface observations, satellite data are used to assess the column predictions including tropospheric nitrogen dioxide (NO₂) column abundance and aerosol optical depth (AOD). The result shows that CMAQ gives reasonably good predictions for the air quality.The air quality improvement that would result from the targeted sulfur dioxide (SO₂) and nitrogen oxides (NO_x) emission controls in China were assessed for the objective year 2010. The results show that the emission controls can lead to significant air quality benefits. SO₂ concentrations in highly polluted areas of East China in 2010 are estimated to be decreased by 30–60% compared to the levels in the 2010 Business-As-Usual (BAU) case. The annual PM_2.5 can also decline by 3–15 μg m^?3 (4–25%) due to the lower SO₂ and sulfate concentrations. If similar controls are implemented for NO_x emissions, NO_x concentrations are estimated to decrease by 30–60% as compared with the 2010 BAU scenario. The annual mean PM_2.5 concentrations will also decline by 2–14 μg m^?3 (3–12%). In addition, the number of ozone (O₃) non-attainment areas in the northern China is projected to be much lower, with the maximum 1-h average O₃ concentrations in the summer reduced by 8–30 ppb.     

Aircraft measurements of O3, NOx,CO, VOCs,and SO2 in the Yangtze River Delta region

In this study, air pollutants, including ozone (O₃), nitrogen oxides (NO_x = NO + NO₂), carbon monoxides (CO), sulfur dioxide (SO₂), and volatile organic compounds (VOCs) measured in the Yangtze River Delta (YRD) region during several air flights between September/30 and October/11 are analyzed. This measurement provides horizontal and vertical distributions of air pollutants in the YRD region. The analysis of the result shows that the measured O₃ concentrations range from 20 to 60 ppbv. These values are generally below the US national standard (84 ppbv), suggesting that at the present, the O₃ pollutions are modest in this region. The NO_x concentrations have strong spatial and temporal variations, ranging from 3 to 40 ppbv. The SO₂ concentrations also have large spatial and temporal variations, ranging from 1 to 35 ppbv. The high concentrations of CO are measured with small variations, ranging from 3 to 7 ppmv. The concentrations of VOCs are relatively low, with the total VOC concentrations of less than 6 ppbv. The relative small VOC concentrations and the relative large NO_x concentrations suggest that the O₃ chemical formation is under a strong VOC-limited regime in the YRD region. The measured O₃ and NO_x concentrations are strongly anti-correlated, indicating that enhancement in NO_x concentrations leads to decrease in O₃ concentrations. Moreover, the O₃ concentrations are more sensitive to NO_x concentrations in the rural region than in the city region. The ratios of Δ[O₃]/Δ[NO_x] are ?2.3 and ?0.25 in the rural and in the city region, respectively. In addition, the measured NO_x and SO₂ concentrations are strongly correlated, highlighting that the NO_x and SO₂ are probably originated from same emission sources. Because SO₂ emissions are significantly originated from coal burnings, the strong correlation between SO₂ and NO_x concentrations suggests that the NO_x emission sources are mostly from coal burned sources. As a result, the future automobile increases could lead to rapid enhancements in O₃ concentrations in the YRD region.     

Seasonal variations of acidic air pollutants in Seoul,South Korea

The annular denuder system (ADS) was used to characterize seasonal variations of acidic air pollutants in Seoul, South Korea. Fifty- four 24 h samples were collected over four seasons from October 1996 to September 1997. The annual mean concentrations of HNO₃, HNO₂, SO₂ and NH₃ in the gas phase were 1.09, 4.51, 17.3 and 4.34 μg m^-3, respectively. The annual mean concentrations of PM_2.5(d_p≤2.5 μm in aerodynamic diameter, 50% cutoff), SO^2-₄, NO^-₃ and NH⁺₄ in the particulate phase were 56.9, 8.70, 5.97 and 4.19 μg m^-3, respectively. All chemical species monitored from this study showed statistical seasonal variations. Nitric acid (HNO₃) and ammonia (NH₃) exhibited substantially higher concentrations during the summer, while nitrous acid (HNO₂) and sulfur dioxide(SO₂) were higher during the winter. Concentrations of PM_2.5, SO^2-₄, NO^-₃ and NH⁺₄ in the particulate phase were higher during the winter months. SO^2-₄, NO^-₃ and NH⁺₄ accounted for 26–38% of PM_2.5. High correlations were found among PM_2.5, SO^2-₄, NO^-₃ and NH⁺₄. The mean H⁺ concentration measured only in the fall was 5.19 nmole m^-3.     

The water-soluble ionic composition of PM2.5 in Shanghai and Beijing,China

A year-long field study to characterize the ionic species in PM2.5 was carried out in Shanghai and Beijing, China, in 1999–2000. Weekly samples of PM2.5 were collected using a special low flow rate (0.4 l min⁻¹) sampler. In Shanghai, SO₄²⁻ NO₃⁻ and NH₄⁺ were the dominant ionic species, which accounted for 46%, 18% and 17% of the total mass of ions, respectively. Local SO₂ emissions were an important source of SO₄²⁻ in PM2.5 because the SO₄²⁻ concentration was correlated with the SO₂ concentration (r=0.66). The relatively stable SO₄²⁻/SO₂ mass ratio over a large range of temperatures suggests that gas-phase oxidation of SO₂ played a minor role in the formation of SO₄²⁻. The sum of SO₄²⁻ and NO₃⁻ was highly correlated with NH₄⁺ (r=0.96), but insufficient ammonium was present to totally neutralize the aerosol. In Beijing, SO₄²⁻, NO₃⁻ and NH₄⁺ were also the dominant ionic species, constituting 44%, 25% and 16% of the total mass of water-soluble ions, respectively. Local SO₂ emissions were an important source of SO₄²⁻ in the winter since SO₄²⁻ was correlated with SO₂ (r=0.83). The low-mass SO₄²⁻/SO₂ ratio (0.27) during winter, which had low humidity, suggests that gas-phase oxidation of SO₂ was a major route of sulfate formation. In the summer, however, much higher mass ratios of SO₄²⁻/SO₂ (5.6) were observed and were ascribed to in-cloud sulfate formation. The annual average ratio of NO₃⁻/SO₄²⁻ was 0.4 and 0.6 in Shanghai and in Beijing, respectively, suggesting that stationary emissions were still a dominant source in these two cities.     

Impacts of a strong cold front on concentrations of HONO,HCHO, O3, and NO2 in the heavy traffic urban area of Beijing

Much rain and strong winds caused by a cold front occurred in Beijing during the period of Sep. 27 to Oct. 4, 2004 and led to sharp drops in maximum and mean concentrations of HONO, HCHO, O₃, and NO₂, i.e., the maximum concentrations were reduced by 5.9, 21.3, 45.6, and 44.4 ppb, respectively, and the mean concentrations were decreased by 4.0, 5.5, 30.3, and 32.3 ppb, respectively. For daily HO_x production rates HONO photolysis was the largest contributor and over 90% contributions were from photolysis of HONO and HCHO. Large number and area percentages of soot aggregate from PM10, and high correlations between concentrations of PM10 and chemical formation of HONO suggested that heterogeneous reactions of NO₂ on surfaces of soot aggregate could be a key source of HONO in the heavy traffic areas of Beijing during the night and should be considered in air quality simulations for such areas.     

Defining the Photochemical Contribution to Particulate Matter in Urban Areas Using Time-Series Analysis

Abstract

The objective of this project is to demonstrate how the ambient air measurement record can be used to define the relationship between O₃ (as a surrogate for photochemistry) and secondary particulate matter (PM) in urban air. The approach used is to develop a time-series transfer-function model describing the daily PM₁₀ (PM with less than 10 μm aerodynamic diameter) concentration as a function of lagged PM and current and lagged O₃, NO or NO₂, CO, and SO₂. Approximately 3 years of daily average PM₁₀, daily maximum 8-hr average O₃ and CO, daily 24-hr average SO₂ and NO₂, and daily 6:00 a.m.-9:00 a.m. average NO from the Aerometric Information Retrieval System (AIRS) air quality subsystem are used for this analysis. Urban areas modeled are Chicago, IL; Los Angeles, CA; Phoenix, AZ; Philadelphia, PA; Sacramento, CA; and Detroit, MI. Time-series analysis identified significant autocorrelation in the O₃, PM₁₀, NO, NO₂,CO, and SO₂ series. Cross correlations between PM₁₀ (dependent variable) and gaseous pollutants (independent variables) show that all of the gases are significantly correlated with PM₁₀ and that O₃ is also significantly correlated lagged up to two previous days. Once a transfer-function model of current PM₁₀ is defined for an urban location, the effect of an O₃-control strategy on PM concentrations is estimated by calculating daily PM₁₀ concentrations with reduced O₃ concentrations. Forecasted summertime PM₁₀ reductions resulting from a 5 percent decrease in ambient O₃ range from 1.2 μg/m³ (3.03%) in Chicago to 3.9 μg/m³ (7.65%) in Phoenix.     

Air pollution at a hotspot location in Delhi: Detecting trends,seasonal cycles and oscillations

This paper uses spectral methods to analyze changes in air quality at a single monitoring site in Delhi since 2000. Power spectral density calculations of daily concentration data for particulate matter (PM10), carbon monoxide (CO), oxides of nitrogen (NO_x) and oxides of sulfur (SO_x) reveal the presence of trends and periodic oscillations for all the pollutants. Singular Spectrum Analysis (SSA) is used to decompose daily data into statistically significant non-linear trends, seasonal cycles and other oscillations. Periods of sharp reductions were observed for both SO_x and CO concentrations in 2001 and 2002, respectively. NO_x concentration trends show a sustained rise from 2000 to 2004, followed by small decline thereafter. PM10 concentration trends remain essentially unchanged over the time period. All pollutants also show strong annual and biannual cycles. The observed trends in CO and NO_x likely relate changes in Delhi's vehicular traffic emissions. The sharp drop in both the trend and amplitude of the seasonal cycle of CO coincides with the switch to Compressed Natural Gas (CNG) as a fuel for Delhi's public transport fleet. Observed changes in SO_x and PM10 concentrations were most likely caused by sources unrelated to vehicular traffic.     

Retrospective assessment of air quality management practices in Taiwan

In 1995, Taiwan's Environmental Protection Administration (EPA/TW) instituted a policy of levying emission taxes on polluters in order to combat the rampant national issue of pollution. Since that time, pollution control strategies, tightening exhaust emission standards for industry, improvements in fuel quality, and new stricter vehicle emission standards, etc., have been implemented. This study evaluates the effectiveness of these measures and examines the improvement of Taiwan's air quality. In this paper, we conduct a detailed analysis of change in the concentrations of pollutants (SO₂, NO_x and particulate matter [PM]) between two three-year periods (from 1996 to1998 and from 2000 to 2002). The pollution levels were generally lower in the latter period. Concentrations at 14 EPA/TW stations in central Taiwan were simulated and source apportionment analyses in three of Central Taiwan's largest cities were conducted using a trajectory transfer-coefficient air quality model. Correlation coefficients (r) between simulations and observations for the monthly means of the concentrations of SO₂, NO_x, PM_2.5 and PM₁₀ during the study periods at the 14 stations are 0.56, 0.63, 0.70 and 0.31, respectively. The sulfur control policy greatly reduced SO₂ concentration island-wide, a stringent emission standard put into place for gasoline vehicles reduced NO_x concentration along highways, and an emissions tax placed on construction sites, as well as a regular program for road-dust sweeping, reduced primary particulate matter. Among all of the pollution abatement policies implemented, the most effective method for reducing PM_2.5 concentrations in the three largest cities involved the reduction of fine ammonium sulfate aerosols from point sources (56–63% of net PM_2.5 reduction). The next largest reduction was attributed to a diminishment in primary PM_2.5 emanating from point sources (27–56% of net PM_2.5 reduction). Secondary particulate matter, especially sulfate, was reduced from distances up to 150 km leeward of major pollution point sources such as Taichung Power Plant.     

Measurements of primary trace gases and NOY composition in Houston,Texas

Concentrations of CO, SO₂, NO, NO₂, and NO_Y were measured atop the University of Houston's Moody Tower supersite during the 2006 TexAQS-II Radical and Aerosol Measurement Project (TRAMP). The lowest concentrations of all primary and secondary species were observed in clean marine air in southerly flow. SO₂ concentrations were usually low, but increased dramatically in sporadic midday plumes advected from sources in the Houston Ship Channel (HSC), located NE of the site. Concentrations of CO and NO_x displayed large diurnal variations in keeping with their co-emission by mobile sources in the Houston Metropolitan Area (HMA). CO/NO_x emission ratios of 5.81 ± 0.94 were observed in the morning rush hour. Nighttime concentrations of NO_x (NO_x = NO + NO₂) and NO_Y (NO_Y = NO + NO₂ + NO₃ + HNO₃ + HONO + 21N₂O₅ + HO₂NO₂ + PANs + RONO₂ + p-NO₃^? + …) were highest in winds from the NNW-NE due to emission from mobile sources. Median ratios of NO_x/NO_Y were approximately 0.9 overnight, reflecting the persistence and/or generation of NO_Z (NO_Z = NO_Y ? NO_x) species in the nighttime Houston boundary layer, and approached unity in the morning rush hour. Daytime concentrations of NO_x and NO_Y were highest in winds from the HSC. NO_x/NO_Y ratios reached their minimum values (median ca 0.63) from 1300 to 1500 CST, near local solar noon, and air masses often retained enough NO_x to sustain additional O₃ formation farther downwind. HNO₃ and PANs comprised the dominant NO_Z species in the HMA, and on a median basis represented 17–20% and 12–15% of NO_Y, respectively, at midday. Concentrations of HNO₃, PANs, and NO_Z, and fractional contributions of these species to NO_Y, were at a maximum in NE flow, reflecting the source strength and reactivity of precursor emissions in the HSC. As a result, daytime O₃ concentrations were highest in air masses with HSC influence. Overall, our findings confirm the impact of the HSC as a dominant source region within the HMA. A comparison of total NO_Y measurements with the sum of measured NO_Y species (NO_Yi = NO_x + HNO₃ + PANs + HONO + p-NO₃^?) yielded excellent overall agreement during both day ([NO_Y](ppb) = ([NO_Yi](ppb)11.03 ± 0.16) ? 0.42; r² = 0.9933) and night ([NO_Y](ppb) = ([NO_Yi](ppb)11.01 ± 0.16) + 0.18; r² = 0.9975). A similar comparison between NO_Y–NO_x concentrations and the sum of NO_Zi (NO_Zi = HNO₃ + PANs + HONO + p-NO₃^?) yielded good overall agreement during the day ([NO_Z](ppb) = ([NO_Zi](ppb)11.01 ± 0.30) + 0.044 ppb; r² = 0.8527) and at night ([NO_Z](ppb) = ([NO_Zi](ppb)11.12 ± 0.69) + 0.16 ppb; r² = 0.6899). Median ratios of NO_Z/NO_Zi were near unity during daylight hours but increased to approximately 1.2 overnight, a difference of 0.15–0.50 ppb. Differences between NO_Z and NO_Zi rarely exceeded combined measurement uncertainties, and variations in NO_Z/NO_Zi ratios may have resulted solely from errors in conversion efficiencies of NO_Y species and changes in NO_Y composition. However, nighttime NO_Z/NO_Zi ratios and the magnitude of NO_Z ? NO_Zi differences were generally consistent with recent observations of ClNO₂ in the nocturnal Houston boundary layer.     

PM2.5–10, PM2.5 and associated water-soluble inorganic species at a coastal urban site in the metropolitan region of Rio de Janeiro

The concentrations of PM_2.5−10, PM_2.5 and associated water-soluble inorganic species (WSIS) were determined in a coastal site of the metropolitan region of Rio de Janeiro, Southeastern Brazil, from October 1998 to September 1999 (n=50). Samples were dissolved in water and analyzed for major inorganic ions. The mean (± standard deviation; median) concentrations of PM_2.5−10 and PM_2.5 were, respectively, 26 (± 16; 21) μg m⁻³ and 17 (± 13; 14) μg m⁻³. Their mean concentrations were 1.7–1.8 times higher in dry season (May–October) than in rainy season (November–April). The WSIS comprised, respectively, 34% and 28% of the PM_2.5−10 and PM_2.5 masses. Chloride, Na⁺ and Mg²⁺ were the predominant ions in PM_2.5−10, indicating a significant influence of sea-salt aerosols. In PM_2.5, SO₄²⁻ (∼97% nss-SO₄²⁻) and NH₄⁺ were the most abundant ions and their equivalent concentration ratio (SO₄²⁻/NH₄⁺ ∼1.0) suggests that they were present as (NH₄)₂SO₄ particles. The mean concentration of (NH₄)₂SO₄ was 3.4 μg m⁻³. The mean equivalent PM_2.5 NO₃⁻ concentration was eight times smaller than those of SO₄²⁻ and NH₄⁺. The PM_2.5 NO₃⁻ concentration in dry season was three times higher than in rainy season, probably due to reaction of NaCl (sea salt) with HNO₃ as a result of higher levels of NO_y during the dry season and/or reduced volatilization of NH₄NO₃ due to lower wintertime temperature. Chloride depletion was observed in both size ranges, although more pronouncely in PM_2.5.     

Influence of boundary conditions on CMAQ simulations over the Iberian Peninsula

The influence of chemical boundary conditions (BC) on the response of the Community Multiscale Air Quality (CMAQ) model over the Iberian Peninsula was investigated in this study. Three strategies to supply boundary conditions in the context of the Integrated Assessment Modelling System for the Iberian Peninsula (SIMCA) were tested. Alternative methods consist in providing BC from (1) fixed, time-independent, concentration profiles, (2) concentrations predicted in a CMAQ mother domain (48 km, 1 h resolution) and (3) concentration values from the GEOS-Chem chemical-transport global model (2 × 2.5°, 3 h resolution). High resolution (3 km) simulated concentrations of the main pollutants (NO₂, NO, SO₂, O₃, PM₁₀ and PM_2.5) were compared through a comprehensive statistical analysis including observational data from 165 monitoring stations all over the Iberian Peninsula. It was found that model sensitivity to BC for nitrogen and sulphur oxides was limited, being restricted to the vicinity of model boundaries. However, significant domain-wide differences were found when modelling ozone and PM depending on the BC provided to run the tests. Although model performance was affected by spatial and seasonal factors, the results indicate that model-derived, dynamic BC improved CMAQ predictions when compared to those based on static concentrations prescribed in the boundaries. Aggregated statistics suggest that the GEOS-Chem produced the best results for O₃ and PM_2.5 while NO₂ and PM₁₀ were slightly better predicted under the CMAQ nesting approach. Besides the statistical evaluation some other relevant issues in the context of Integrated Assessment Modelling (IAM) are discussed to gain a better insight into the suitability of the methods analyzed and limitations of downscaling methods. Despite being useful to get a better understanding of the role of BC in SIMCA, this study contributed to highlight model deficiencies and therefore to point out future research needs to improve IAM activities in the Iberian Peninsula.     

FT-IR product study of the OH-initiated oxidation of DMS in the presence of NOx

The influence of NO_x (NO+NO₂) concentrations on the product distribution of the OH-initiated oxidation of DMS has been studied at room temperature using total NO_x concentrations varying from 0 to ∼1800 ppbv (30–600 ppbv NO₂ and 140–1760 ppbv NO). Clear trends in the formation yields of the products SO₂, COS, MSA, MTF (methyl thiolformate), MSPN (methanesulphonyl peroxynitrate), DMSO and DMSO₂ have been observed with variation in NO_x. The presence of low levels of NO reduces the yields of both MTF and COS to zero. The formation yields of MSA and DMSO₂ increase with increasing NO_x concentration, whereas the yields of DMSO and SO₂ decrease. The following approximate changes in the yield, not corrected for possible loss processes, have been measured for variation of NO_x between 0 and ∼1800 ppbv: DMSO decreases from 20 to 3%S; DMSO₂ increases from 3 to 15%S, SO₂ decreases from 70 to 30%S and MSA increases from 4 to 17%S. Under the experiments conditions NO_x levels of several tens of ppbv are required before a perceptible change is observed in the MSA yield. If applicable to the atmosphere such a situation is only likely to be observed near coastal areas affected by pollution. MSPN (CH₃SO₂O₂NO₂) is observed as an oxidation product in the presence of NO₂ even at low levels (e.g. 60 ppbv). Its possible role as a NO_x reservoir in the troposphere is considered.     

Photochemical model performance for PM2.5 sulfate,nitrate, ammonium,and precursor species SO2, HNO3, and NH3 at background monitor locations in the central and eastern United States

Health studies have shown premature death is statistically associated with exposure to particulate matter <2.5 μm in diameter (PM2.5). The United States Environmental Protection Agency requires all States with PM2.5 non-attainment counties or with sources contributing to visibility impairment at Class I areas to submit an emissions control plan. These emission control plans will likely focus on reducing emissions of sulfur oxides and nitrogen oxides, which form two of the largest chemical components of PM2.5 in the eastern United States: ammonium sulfate and ammonium nitrate. Emission control strategies are simulated using three-dimensional Eulerian photochemical transport models.A monitor study was established using one urban (Detroit) and nine rural locations in the central and eastern United States to simultaneously measure PM2.5 sulfate ion (SO₄²⁻), nitrate ion (NO₃⁻), ammonium ion (NH₄⁺), and precursor species sulfur dioxide (SO₂), nitric acid (HNO₃), and ammonia (NH₃). This monitor study provides a unique opportunity to assess how well the modeling system predicts the spatial and temporal variability of important precursor species and co-located PM2.5 ions, which is not well characterized in the central and eastern United States.The modeling system performs well at estimating the PM2.5 species, but does not perform quite as well for the precursor species. Ammonia is under-predicted in the coldest months, nitric acid tends to be over-predicted in the summer months, and sulfur dioxide appears to be systematically over-predicted. Several indicators of PM2.5 ammonium sulfate and ammonium nitrate formation and chemical composition are estimated with the ambient data and photochemical model output. PM2.5 sulfate ion is usually not fully neutralized to ammonium sulfate in ambient measurements and is usually fully neutralized in model estimates. The model and ambient estimates agree that the ammonia study monitors tend to be nitric acid limited for PM2.5 nitrate formation. Regulatory strategies in this part of the country should focus on reductions in NO_X rather than ammonia to control PM2.5 ammonium nitrate.     

Assessing the Relationship between Personal Particulate and Gaseous Exposures of Senior Citizens Living in Baltimore,MD

ABSTRACT

We conducted a multi-pollutant exposure study in Baltimore, MD, in which 15 non-smoking older adult subjects (>64 years old) wore a multi-pollutant sampler for 12 days during the summer of 1998 and the winter of 1999. The sampler measured simultaneous 24-hr integrated personal exposures to PM₂₅, PM₁₀, SO₄ ^2-, O₃, NO₂, SO₂, and exhaust-related VOCs.

Results of this study showed that longitudinal associations between ambient PM_2.5 concentrations and corresponding personal exposures tended to be high in the summer (median Spearman's r = 0.74) and low in the winter (median Spearman's r = 0.25). Indoor ventilation was an important determinant of personal PM_2.5 exposures and resulting personal-ambient associations. Associations between personal PM₂₅ exposures and corresponding ambient concentrations were strongest for well-ventilated indoor environments and decreased with ventilation. This decrease was attributed to the increasing influence of indoor PM_{2 5} sources. Evidence for this was provided by SO₄ ^2-measurements, which can be thought of as a tracer for ambient PM₂₅. For SO₄ ^2-, personal-ambient associations were strong even in poorly ventilated indoor environments, suggesting that personal exposures to PM_2.5 of ambient origin are strongly associated with corresponding ambient concentrations. The results also indicated that the contribution of indoor PM_2.5 sources to personal PM_2.5 exposures was lowest when individuals spent the majority of their time in well-ventilated indoor environments.

Results also indicate that the potential for confounding by PM_2.5 co-pollutants is limited, despite significant correlations among ambient pollutant concentrations. In contrast to ambient concentrations, PM_2.5 exposures were not significantly correlated with personal exposures to PM_2.5-10, PM_2.5 of non-ambient origin, O₃, NO₂, and SO₂. Since a confounder must be associated with the exposure of interest, these results provide evidence that the effects observed in the PM_2.5 epidemiologic studies are unlikely to be due to confounding by the PM_2.5 co-pollutants measured in this study.     

Statistical distributions of particulate matter and the error associated with sampling frequency

The distribution of particulate matter (PM) concentrations has an impact on human health effects and the setting of PM regulations. Since PM is commonly sampled on less than daily schedules, the magnitude of sampling errors needs to be determined. Daily PM data from Spokane, Washington were resampled to simulate common sampling schedules and the sampling error was computed for regulatory and distribution statistics. Probability density functions (pdf's) were fit to the annual daily data to determine the shape of the PM_2.5 and PM₈ concentration distributions and they were also fit to the less than daily sampling to determine if pdf's could be used to predict the daily high-concentration percentiles. There is an error when using a less than daily sampling schedule for all statistics. The error expressed as a percentage difference from the everyday sampling for the PM_2.5 mean was as large as 1.7, 3.4 and 7.7% and the 98th percentile error was as great as 8.8, 18 and 67% for 1-in-2 day, 1-in-3 day and 1-in-6 day sampling, respectively. For PM₈ the error in the mean was 2.5, 4.7 and 8.6% for and the error in the 99th percentile was 27, 18 and 46% for 1-in-2 day, 1-in-3 day, and 1-in-6 day sampling, respectively. The PM_2.5 and PM₈ concentration data were best fit by a three-parameter lognormal distribution and a generalized extreme value distribution, respectively. For PM_2.5 and PM₈, as the annual mean increased the mode concentration increased, but for PM₈ the shape of the distribution also flattened. Predicting the daily high percentiles from pdf's that were fit to the less than daily sampled data produced mixed results. For PM₈, the pdf's predicted high concentrations were closer to the daily percentiles than the actual less-than-daily sampling percentile while for PM_2.5 they were not.     

Simulation of long-range transport of acidic pollutants in East Asia during the Yellow Sand event

The atmospheric chemical process was simulated using the Carbon Bond 4 (CB-4) model, the aqueous-phase chemistry in Regional Acid Deposition Model and the thermodynamic equilibrium relation of aerosols with the emission inventories of the Emission Database for Global Atmospheric Research, the database of China and South Korea and the Mesoscale Model version 2 (MM5) meteorological fields to examine the spatial distributions of the acidic pollutant concentrations in East Asia for the case of the long-lasting Yellow Sand event in April 1998. The present models simulate quite well the observed general trend and the diurnal variation of concentrations of gaseous pollutants, especially for O₃ concentration. However, the model underestimates SO₂ and NO_x concentration but overestimates O₃ concentration largely due to uncertainty in NO_x and VOC emissions. It is found that the simulated gaseous pollutants such as SO₂, NO_x, and NH₃ are not transported far away from the source regions but show significant diurnal variations of their concentrations. However, the daily variations of the concentrations are not significant due to invariant emission rates. On the other hand, concentrations of the transformed pollutants including SO₄²⁻, NH₄⁺, and NO₃⁻ are found to have significant daily variations but little diurnal variations. The model-estimated deposition indicates that dry deposition is largely contributed by gaseous pollutants while wet deposition of pollutants is mainly contributed by the transformed pollutants.     

Characteristics and origins of air pollutants in Wuhan,China, based on observations and hybrid receptor models

To identify the characteristics of air pollutants and factors attributing to the formation of haze in Wuhan, this study analyzed the hourly observations of air pollutants (PM_2.5, PM₁₀, NO₂, SO₂, O₃, and CO) from March 1, 2013, to February 28, 2014, and used hybrid receptor models for a case study. The results showed that the annual average concentrations for PM_2.5, PM₁₀, NO₂, SO₂, O₃, and CO during the whole period were 89.6 μg m^?3, 134.9 μg m^?3, 54.9 μg m^?3, 32.4 μg m^?3, 62.3 μg m^?3, and 1.1 mg m^?3, respectively. The monthly variations revealed that the peak values of PM_2.5, PM₁₀, NO₂, SO₂, and CO occurred in December because of increased local emissions and severe weather conditions, while the lowest values occurred in July mainly due to larger precipitation. The maximum O₃ concentrations occurred in warm seasons from May to August, which may be partly due to the high temperature and solar radiation. Diurnal analysis showed that hourly PM_2.5, PM₁₀, NO₂, and CO concentrations had two ascending stages accompanying by the two traffic peaks. However, the O₃ concentration variations were different with the highest concentration in the afternoon. A case study utilizing hybrid receptor models showed the significant impact of regional transport on the haze formation in Wuhan and revealed that the mainly potential polluted sources were located in the north and south of Wuhan, such as Baoding and Handan in Hebei province, and Changsha in Hunan province. Implications: Wuhan city requires a 5% reduction of the annual mean of PM_2.5 concentration by the end of 2017. In order to accomplish this goal, Wuhan has adopted some measures to improve its air quality. This work has determined the main pollution sources that affect the formation of haze in Wuhan by transport. We showed that apart from the local emissions, north and south of Wuhan were the potential sources contributing to the high PM_2.5 concentrations in Wuhan, such as Baoding and Handan in Hebei province, Zhumadian and Jiaozuo in Henan province, and Changsha and Zhuzhou in Hunan province.     

An empirical approach for the prediction of annual mean nitrogen dioxide concentrations in London

Annual mean limits for NO₂ concentrations have been set in the European Union, which will be most challenging to meet in large urban conurbations. In this paper, we discuss techniques that have been developed to predict current and future NO₂ concentrations in London, utilising ambient data. Hourly average NO_x (NO+NO₂) and NO₂ concentrations are used to calculate NO_x frequency distributions. By defining relationships between the annual mean NO_x and NO₂ at different sites, it is possible to investigate different NO_x reduction strategies. The application of the frequency distribution approach to monitoring sites in London shows that given the likely change in emissions by 2005, it is unlikely that much of central and inner London will meet the objective. The approaches used suggest that meeting the objective in central London will be the most challenging for policy makers requiring NO_x concentrations as low as 30 ppb, compared with values closer to 36–40 ppb for outer London. Predictions for 2005 indicate that concentrations of NO₂ up to 6 ppb in excess of the objective are likely in central London.