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At least 19 recordsLinked to original sources
PubMed2005

Nonlinear response of ozone to emissions: source apportionment and sensitivity analysis.

For secondary air pollutants, precursor emissions may impact concentrations in nonlinear and interdependent manners. We explore the nonlinear responses of one such pollutant, ozone, to emissions of its precursors, nitrogen oxides (NOx) and volatile organic compounds. Modeling is conducted for a high ozone episode in the southeastern United States, applying a second-order direct sensitivity method in a regional air quality model. As applied here, the sensitivity method neglects most aerosol and aqueous chemistry processes. Inclusion of second-order sensitivities is shown to enable accurate characterization of response to large perturbations in emissions. An index is introduced to characterize the nonlinearity of ozone response to NOx emitted from each source region. Nonlinearity is found to increase with the tonnage and emission density of the source region. Interactions among the impacts of emission sources are shown to lead to discrepancies between source contribution attributed to an ensemble of emitters and the sum of the contributions attributed to each component. A method is introduced for applying these "cross-sensitivity" interactions to assess the uncertainty of sensitivity and source apportionment estimates arising from uncertainty in an emissions inventory. For ozone response to NOx, underestimates in emission rates lead to underprediction of total source contribution but overprediction of per-ton sensitivity.

Air Pollutants↗
PubMed1986

[Formation and transport of ozone and other photochemical oxidants].

Photochemical oxidants (O3, PAN, HCHO) are the typical pollutants in photochemical Smog. They can be formed as the result of the sunlight induced oxidation of precursor pollutants emitted into the atmosphere (NOx, CxHy). Other important precursor substances and reactive intermediates are compounds of the organic hydroxyl group (-O-H, for instance the methoxy radical CH3O), hydroxyl radical .OH, hydroperoxy radical HO2, and singlet oxygen O. For the production of photochemical oxidants in smog, especially ozone, NOx primarily act as catalysator. But CxHy serve as "combustibles". The quantities of the several formed photooxidants are mainly dependent on intensity and duration of daily sunshine, temperature, oxidant concentrations at the beginning of a build-up period, and on emission rates and concentrations of primary pollutants (NO, CxHy). Maximum mixing ratios of secondary pollutants often occur at certain distances downwind of primary pollutant sources, dependent on meteorological conditions (wind velocity, rel. humidity, etc.) and on rate constants for oxidant formation cycles. During the period of July 5 to 11, 1984, for instance, 6 kilometers SW from Zürich we found maximum ground-level mixing ratios of about 150 ppbv ozone, 4 ppbv PAN and 9 ppbv formaldehyde, that is 5 (ozone) to 10 (PAN) times above the supposed oxidant concentrations of unpolluted continental air. The increase in ozone in the late morning and early afternoon is accompanied by an increase in PAN and HCHO and by a decrease in NOx. This shows that in this case HCHO originates from photochemical reactions rather than being emitted directly to the atmosphere from vehicles.(ABSTRACT TRUNCATED AT 250 WORDS)

Acetates↗
PubMed2001

A comparison of measured and simulated ozone concentrations in the rural areas of the eastern United States during summer 1995.

The recent regulatory actions toward a longer-term (i.e., 8-hr) average ozone standard have brought forth the potential for many rural areas in the eastern United States to be in noncompliance. However, since a majority of these rural areas have generally few sources of anthropogenic emissions, the measured ozone levels primarily reflect the effects of the transport of ozone and its precursor pollutants and natural emissions. While photochemical grid models have been applied to urban areas to develop ozone mitigation measures, these efforts have been limited to high ozone episode events only and do not adequately cover rural regions. In this study, we applied a photochemical modeling system, RAMS/UAM-V, to the eastern United States from June 1-August 31, 1995. The purpose of the study is to examine the predictive ability of the modeling system at rural monitoring stations that are part of the Clean Air Status Trends Network (CASTNet) and the Gaseous Pollutant Monitoring Program (GPMP). The results show that the measured daily 1-hr ozone maxima and the seasonal average of the daily 1-hr ozone maxima are in better agreement with the predictions of the modeling system than those for the daily 8-hr ozone maxima. Also, the response of the modeling system in reproducing the measured range of ozone levels over the diurnal cycle is poor, suggesting the need for improvement in the treatment of the physical and chemical processes of the modeling system during the nighttime and morning hours if it is to be used to address the 8-hr ozone standard.

Air Pollutants↗
PubMed2002

Visibility: science and regulation.

The 1999 Regional Haze Rule provides a context for this review of visibility, the science that describes it, and the use of that science in regulatory guidance. The scientific basis for the 1999 regulation is adequate. The deciview metric that tracks progress is an imperfect but objective measure of what people see near the prevailing visual range. The definition of natural visibility conditions is adequate for current planning, but it will need to be refined as visibility improves. Emissions from other countries will set achievable levels above those produced by natural sources. Some natural events, notably dust storms and wildfires, are episodic and cannot be represented by annual average background values or emission estimates. Sulfur dioxide (SO2) emission reductions correspond with lower sulfate (SO4(2-)) concentrations and visibility improvements in the regions where these have occurred. Non-road emissions have been growing more rapidly than emissions from other sources, which have remained stable or decreased since 1970. Simpler models representing transport, limiting precursor pollutants, and gas-to-particle equilibrium should be used to understand where and when emission reductions will be effective, rather than large complex models that have insufficient input and validation measurements. Examples of model-based source attribution show large differences among estimates from various modeling systems and with ambient measurements.

Air Pollutants↗
PubMed2003

Diurnal and weekday variations in the source contributions of ozone precursors in California's South Coast Air Basin.

For at least 30 years, ozone (O3) levels on weekends in parts of California's South Coast (Los Angeles) Air Basin (SoCAB) have been as high as or higher than on weekdays, even though ambient levels of O3 precursors are lower on weekends than on weekdays. A field study was conducted in the Los Angeles area during fall 2000 to test whether proposed relationships between emission sources and ambient nonmethane hydrocarbon (NMHC) and oxides of nitrogen (NOx) levels can account for observed diurnal and day-of-week variations in the concentration and proportions of precursor pollutants that may affect the efficiency and rate of O3 formation. The contributions to ambient NMHC by motor vehicle exhaust and evaporative emissions, estimated using chemical mass balance (CMB) receptor modeling, ranged from 65 to 85% with minimal day-of-week variation. Ratios of ambient NOx associated with black carbon (BC) to NOx associated with carbon monoxide (CO) were approximately 1.25 +/- 0.22 during weekdays and 0.76 +/- 0.07 and 0.52 +/- 0.07 on Saturday and Sunday, respectively. These results demonstrate that lower NOx emissions from diesel exhaust can be a major factor causing lower NOx mixing ratios and higher NMHC/NOx ratios on weekends. Nonmobile sources showed no significant day-of-week variations in their contributions to NMHC. Greater amounts of gasoline emissions are carried over on Friday and Saturday evenings but are, at most, a minor factor contributing to higher NMHC/NOx ratios on weekend mornings.

Air Pollutants↗
PubMed2006

The health benefits of reduced tropospheric ozone in California.

Californians are exposed daily to concentrations of ozone (O3) that are among the highest in the United States. Recently, the state adopted a new 8-hr ambient standard of 0.070 ppm, more stringent than the current federal standard. The new standard is based on controlled human studies and on dozens of epidemiologic studies reporting associations between O3 at current ambient levels and a wide range of adverse health outcomes. Clearly, the new O3 standards will require further reductions in the precursor pollutants and additional expenditures for pollution control. Therefore, it is important to quantify the incremental health benefits of moving from current conditions to the new California standard. In this paper, a standard methodology is applied to quantify the health benefits associated with O3 concentration reductions in California. O3 concentration reductions are estimated using ambient monitoring data and a proportional rollback approach in which changes are specific to each air basin, and control strategies may impact concentrations both below and above the standard. Health impacts are based on published epidemiologic studies, including O3-related mortality and morbidity, and economic values are assigned to these outcomes based on willingness-to-pay and cost-of-illness studies. Central estimates of this research indicate that attaining the California 8-hr standard, relative to current concentrations, would result in annual reductions of 630 cases of premature mortality, 4200 respiratory hospital admissions, 660 pediatric emergency room visits for asthma, 4.7 million days of school loss, and 3.1 million minor restricted activity days, with a median estimated economic value of dollar 4.5 billion. Sensitivity analyses indicate that these findings are robust with respect to exposure assessment methods but are influenced by assumptions about the slope of the concentration-response function in threshold models and the magnitude of the O3-mortality relationship. Although uncertainties exist for several components of the methodology, these results indicate that the benefits of reducing O3 to the California standard may be substantial and that further research on the shape of the O3-mortality concentration-response function and economic value of O3-related mortality would best reduce these uncertainties.

Air Pollution↗
PubMed1982

Ozone precursor monitor for investigating air pollution.

Ozone is designated by the Environmental Protection Agency as one of six principal air pollutants. Of the six, ozone alone is classified as a secondary pollutant since it is not emitted by a specific source. Ozone is formed in the lower atmosphere by photochemical reactions involving the precursors of ozone: gaseous organic compounds (mostly hydrocarbons), nitric oxide, and nitrogen dioxide. This paper describes a new automated method for quantifying the precursors of ozone. An ozone analyzer is coupled to a reaction vessel contained in an irradiation chamber. At timed intervals discrete samples of outside air are drawn into the reaction vessel and irradiated with ultraviolet light. The amount of ozone produced is a measure of the photochemical reactivity potential of the precursor blend. The ozone precursor monitor (OPM) is designed for urban air sampling stations where analyzers for the principal air pollutants are routinely operated. The monitor, however, has other uses. Among special applications of the method that are discussed are its use as an early warning device for forecasting elevated ozone concentrations, a screening system for assessing the photoreactivity of solvents, and a procedure for investigating the transport of ozone precursors from urban to rural areas.

Air Pollutants↗
PubMed2001

[Determination of volatile organic compounds in atmospheric environment].

It is well known that volatile organic compounds (VOCs) are the main photochemical pollutants and ozone precursors of the photochemical smog. Investigation of photochemical pollution in the ambient air must focus on VOCs, but the concentration of VOCs in ambient air is in a very low level (10(-9)-10(-12), volume fraction), so there are difficulties in the determination of VOCs. In this work, based on the TO14A and TO15 methods recommended by the Environmental Protection Agency of United States, an improved method for the determination of fifty-six VOCs, mainly O3 precursors, in atmospheric environment was developed. Operating conditions of VOCs preconcentrator, gas chromatography (GC) and gas chromatography-mass spectrometry (GC-MS) were optimized. Air sample was first frozen by liquid nitrogen, and then H2O and CO2 were eliminated in the VOCs preconcentrator. The preconcentrated VOCs sample was injected to GC and detected by MS or hydrogen flame ionization detector (FID). The C2-C10 hydrocarbons were separated effectively in capillary columns under the high concentration of CO2. The detection limits were 0.1 microgram.m-3 and the relative standard deviations were in the range from 2.57% to 9.82%. This method has been used for the determination of VOCs in real samples. The results were satisfactory.

Air Pollutants↗
PubMed2000

Development of a speciated, hourly, and gridded air pollutants emission modeling system--a case study on the precursors of photochemical smog in the Seoul metropolitan area, Korea.

A speciated, hourly, and gridded air pollutants emission modeling system (SHEMS) was developed and applied in predicting hourly nitrogen dioxide (NO2) and ozone (O3) levels in the Seoul Metropolitan Area (SMA). The primary goal of the SHEMS was to produce a systemized emission inventory for air pollutants including ozone precursors for modeling air quality in urban areas. The SHEMS is principally composed of three parts: (1) a pre-processor to process emission factors, activity levels, and spatial and temporal information using a geographical information system; (2) an emission model for each source type; and (3) a post-processor to produce report and input data for air quality models through database modeling. The source categories in SHEMS are point, area, mobile, natural, and other sources such as fugitive emissions. The emission database produced by SHEMS contains 22 inventoried compounds: sulfur dioxide, NO2, carbon monoxide, and 19 speciated volatile organic compounds. To validate SHEMS, the emission data were tested with the Urban Airshed Model to predict NO2 and O3 concentrations in the SMA during selected episode days in 1994. The results turned out to be reliable in describing temporal variation and spatial distribution of those pollutants.

Air Pollutants↗
PubMed2003

Outdoor air pollution activities at the Wisconsin State Laboratory of Hygiene.

Outdoor air quality testing at the Wisconsin State Laboratory of Hygiene (WSLH) began in the 1970s with the advent of the federal Clean Air Act. Since then, air quality has emerged as a major environmental issue equal to or more important, from a public health standpoint, than water pollution. Epidemiological studies have shown that health issues are not limited to highly urbanized areas. In Wisconsin, local climatic conditions caused by the Great Lakes can result in unhealthy conditions even in relatively pristine areas. Air pollution affects thousands of Wisconsin residents each year, and it can be severe enough to require a physician's care. Although certain air testing (e.g., ozone) is done regionally by in situ monitors, the WSLH analyzes a variety of air pollutants including ozone precursor hydrocarbons, air particulates, and toxic metals. Exposure to aerosols containing metals may not follow typical patterns of air pollution based on routinely monitored particle mass.

Air Pollutants↗
PubMed1996

Geographical distribution of benzene in air in northwestern Italy and personal exposure.

Benzene is a solvent strictly related to some industrial activities and to automotive emissions. After the reduction in lead content of fuel gasoline, and the consequent decrease in octane number, an increase in benzene and other aromatic hydrocarbons in gasoline occurred. Therefore, an increase in the concentration of these chemicals in the air as primary pollutants and as precursors of photochemical smog could occur in the future. The objectives of this study were to describe the benzene air pollution at three sites in northwestern Italy throughout 1991 and 1994; to examine the relationship between benzene air pollution in indoor, outdoor, and personal air as measured by a group of nonsmoking university students; and to determine the influence of environmental tobacco smoke on the level of benzene exposure in indoor air environments. The results indicate a direct relationship between population density and levels of contamination; an indoor/outdoor ratio of benzene air pollution higher than 1 during day and night; a similar level of personal and indoor air contamination; and a direct relationship between levels of personal exposure to benzene and intensity of exposure to tobacco smoke. Human exposure to airborne benzene has been found to depend principally on indoor air contamination not only in the home but also in many other confined environments.

Air Pollutants↗
PubMed2026

Three-dimensional source apportionment and quantitative characterization of horizontal and vertical transport fluxes of O3 and its precursors in the Beijing-Tianjin-Hebei region, China.

Persistent surface ozone (O3) pollution in the Beijing-Tianjin-Hebei (BTH) region is driven by coupled precursor emissions and multi-scale transport, yet its altitude-dependent transport and source contributions remain insufficiently quantified. Here we integrated the Weather Research and Forecasting and the Comprehensive Air Quality Model with Extensions with the Ozone Source Apportionment Technology and a quantitative transport-flux framework to characterize three-dimensional source apportionment and horizontal/vertical fluxes of O3, Volatile Organic Compounds‌ (VOCs), and Nitrogen Oxides (NOx) across dynamic meteorological scenarios. Simulations showed that VOCs and NOx were dominated by local emissions near the surface (73.61 %-82.18 %), whereas surface O3 was primarily controlled by regional transport, with local contributions of only 11.01 %-13.75 %. Notably, the transport dominance further strengthened with altitude, exceeding 93 % at 1.8 km. Industrial and transportation emissions together contributed more than 75 % of precursor emissions and account for approximately 80 % of O3 formation, while favorable/unfavorable meteorological years modulated long-range transport efficiency and the vertical distribution of contributions. Horizontal flux analysis highlighted three major pathways (Northwest-Southeast, Southeast-Northwest, and Southwest-Northeast), with Shijiazhuang serving as a critical pollutant "sink" across altitude layers. Vertical fluxes revealed an altitude transition near 600 m: net downward transport dominated below 600 m, whereas enhanced summer convection promoted upward transport above 600 m. These results support altitude-dependent, scenario-specific strategies for coordinated regional O3 mitigation in the BTH region.

Ozone↗
PubMed1988

Dry deposition of airborne sulfate and nitrate to soybeans.

Dry deposition contributes a substantial part of the total deposition of acidic pollutants and acid precursors to agricultural systems. However, because of the relative intractability of measurement of dry deposition fluxes, little work has been done to directly quantify dry inputs of pollutants to crops. In this research, foliar surface sampling ('leaf-washing') methods were developed and shown to be a practical and fairly precise means of monitoring the accumulation of dry-deposited SO4(2-) and NO3- on plant surfaces. Leaching of these ions from plant tissues was shown to be negligible; however, uptake by plants (e.g. stomatal gas exchange of SO2 or HNO3 and/or assimilation of surface accumulations of materials) is not accounted for by the sampling method. The significance of dry deposition to modification of the chemical microenvironment of leaf surfaces appears to be a factor of 3 to 20 or more greater than that of wet deposition alone. This is due to the cyclic reactivation of accumulated materials by dew and light rains, which may dissolve and mobilize, but not remove, the pollutant surface deposit. Therefore, while dry deposition of SO2 and SO4(2-) containing particles may contribute only part of the total mass of sulfur inputs to crop systems, the exposure of plant surface tissue to pollutants can be dominated by the dry-deposited material. The alteration of leaf surface chemistry may contribute to possible stress-producing mechanisms such as reduction of cuticular integrity, cellular injury and death, enhanced leaching of primary and secondary metabolites, and changes in pathogen infection efficiency.

Journal Article↗
PubMed2004

Multi-objective analysis of ground-level ozone concentration control.

To develop sound air quality plans, regional authorities should have instruments that link the complex behaviour of pollutants both in time and space with costs of emission reduction. The problem is particularly important for ground level ozone which forms kilometres away, hours later from the emission of its precursors. To approach this problem, a method (1) to identify local pollutant-precursor models on the basis of results from a large photochemical model (CALGRID), (2) to integrate them in a multi-objective mathematical program, together with an estimate of the emission reduction costs, is suggested. The method has been used to assess action priorities in Lombardy (Northern Italy). This area, characterised by a complex terrain, high urban and industrial emissions and a dense road network is often affected by severe photochemical pollution episodes during summer.

Air Pollution↗
PubMed2005

Development of the high spatial resolution EMICAT2000 emission model for air pollutants from the north-eastern Iberian Peninsula (Catalonia, Spain).

Ozone (O(3)) pollution episodes take place in Catalonia (NE of the Iberian Peninsula), mainly during summertime. The complex O(3) behaviour could be understood by using a Chemical Transport Model (CTM). Emission inventories provide the spatial and temporal emissions distribution of the O(3) precursors and other pollutants required by this approach. We developed the EMICAT2000 model with high spatial (cells of 1 km(2)) and temporal (1h) resolutions, to estimate the emissions during the year 2000 from Catalonia. Total annual emissions were 107 kt yr(-1) of NO(x), 137 kt yr(-1) of NMVOC, 267 kt yr(-1) of CO, 65 kt yr(-1) of SO(2), 24 kt yr(-1) of TSP and 32,175 kt yr(-1) of equivalent CO(2). Main NO(x) sources are on-road traffic (58%) and industries (38%). Main NMVOC sources are on-road traffic (36%), vegetation (34%) and use of solvents (13%). Speciation was established according to the Carbon Bond IV mechanism. EMICAT2000 generates directly the data files required for the third generation CTM Models-3/CMAQ.

Air Pollutants↗
PubMed2005

A comparative study of US EPA 1996 and 1999 emission inventories in the west Gulf of Mexico coast region, USA.

Emission inventory is one of the required inputs to air quality models. To assist in the urban and regional modeling efforts, United States Environmental Protection Agency (EPA) has compiled a National Emission Inventory (NEI) for criterion pollutants, and the precursors of ozone and particulate matter (PM). In December 2002, EPA released the 1999 NEI estimates (NEI99), which represent the most recent national emission data. However, the data sets are not in model-ready format for air quality simulations. This present work converts the NEI99 Final Version 2 data sets into Inventory Data Analyzer (IDA) format and processes the data using the Sparse Matrix Operator Kernel Emissions (SMOKE) modeling system to generate a gridded emission inventory in a domain covering the west Gulf Coast Region, USA. The spatial and diurnal emission characteristics of the gridded emission inventories are then assessed and compared with those of the National Emission Trend 1996 (NET96). The NEI99 database contains more complete emission records in both area and point sources. It is also found that NEI99 data exhibit greater emissions with respect to point and mobile sources but smaller emissions with respect to area sources when compared to the corresponding gridded NET96 data in the same study domain. The most distinct differences between the NEI99 and NET96 databases are CO emission of mobile sources, SO2 emissions of point sources, and VOC/PM/NH3/NOx emissions of area and non-road sources. The gridded NEI99 data show low VOC/NOx ratios (<2-5) in the urban areas of the study domain.

Air Pollutants↗