Integrated Assessment Modeling of Atmospheric Pollutants in the Southern Appalachian Mountains. Part I: Hourly and Seasonal Ozone

Abstract

Recently, a comprehensive air quality modeling system was developed as part of the Southern Appalachians Mountains Initiative (SAMI) with the ability to simulate meteorology, emissions, ozone, size- and composition-resolved particulate matter, and pollutant deposition fluxes. As part of SAMI, the RAMS/EMS-95/URM-1ATM modeling system was used to evaluate potential emission control strategies to reduce atmospheric pollutant levels at Class I areas located in the Southern Appalachians Mountains. This article discusses the details of the ozone model performance and the methodology that was used to scale discrete episodic pollutant levels to seasonal and annual averages. The daily mean normalized bias and error for 1-hr and 8-hr ozone were within U.S. Environment Protection Agency guidance criteria for urban-scale modeling. The model typically showed a systematic overestimation for low ozone levels and an underestimation for high levels. Because SAMI was primarily interested in simulating the growing season ozone levels in Class I areas, daily and seasonal cumulative ozone exposure, as characterized by the W126 index, were also evaluated. The daily ozone W126 performance was not as good as the hourly ozone performance; however, the seasonal ozone W126 scaled up from daily values was within 17% of the observations at two typical Class I areas of the SAMI region. The overall ozone performance of the model was deemed acceptable for the purposes of SAMI’s assessment.     

A New Method to Assess Mercury Emissions: A Study of Three Coal-Fired Electric-Generating Power Station Configurations

Abstract

U.S. Environmental Protection Agency (EPA) Method 7473 for the analysis of mercury (Hg) by thermal decomposition, amalgamation, and atomic absorption spectroscopy has proved successful for use in Hg assessment at coal-fired power stations. In an analysis time of ～5 min per sample, this instrumental methodology can directly analyze total Hg—with no discrete sample preparation—in the solid matrices associated with a coal-fired power plant, including coal, fly ash, bottom ash, and flue gas desulfurization (FGD) material. This analysis technique was used to investigate Hg capture by coal combustion byproducts (CCBs) in three different coal-fired power plant configurations. Hg capture and associated emissions were estimated by partial mass balance. The station equipped with an FGD system demonstrated 68% capture on FGD material and an emissions estimate of 18% (11 kg/yr) of total Hg input. The power plant equipped with low oxides of nitrogen burners and an electrostatic precipitator (ESP) retained 43% on the fly ash and emitted 57% (51 kg/yr). The station equipped with conventional burners and an ESP retained less than 1% on the fly ash, emitting an estimated 99% (88 kg/yr) of Hg. Estimated Hg emissions demonstrate good agreement with EPA data for the power stations investigated.     

Quantifying the sources of ozone, fine particulate matter, and regional haze in the Southeastern United States

A detailed sensitivity analysis was conducted to quantify the contributions of various emission sources to ozone (O₃), fine particulate matter (PM_2.5), and regional haze in the Southeastern United States. O₃ and particulate matter (PM) levels were estimated using the Community Multiscale Air Quality (CMAQ) modeling system and light extinction values were calculated from modeled PM concentrations. First, the base case was established using the emission projections for the year 2009. Then, in each model run, SO₂, primary carbon (PC), NH₃, NO_x or VOC emissions from a particular source category in a certain geographic area were reduced by 30% and the responses were determined by calculating the difference between the results of the reduced emission case and the base case.The sensitivity of summertime O₃ to VOC emissions is small in the Southeast and ground-level NO_x controls are generally more beneficial than elevated NO_x controls (per unit mass of emissions reduced). SO₂ emission reduction is the most beneficial control strategy in reducing summertime PM_2.5 levels and improving visibility in the Southeast and electric generating utilities are the single largest source of SO₂. Controlling PC emissions can be very effective locally, especially in winter. Reducing NH₃ emissions is an effective strategy to reduce wintertime ammonium nitrate (NO₃NH₄) levels and improve visibility; NO_x emissions reductions are not as effective. The results presented here will help the development of specific emission control strategies for future attainment of the National Ambient Air Quality Standards in the region.     

Toward verifying fossil fuel CO2 emissions with the CMAQ model: Motivation,model description and initial simulation

Motivated by the question of whether and how a state-of-the-art regional chemical transport model (CTM) can facilitate characterization of CO₂ spatiotemporal variability and verify CO₂ fossil-fuel emissions, we for the first time applied the Community Multiscale Air Quality (CMAQ) model to simulate CO₂. This paper presents methods, input data, and initial results for CO₂ simulation using CMAQ over the contiguous United States in October 2007. Modeling experiments have been performed to understand the roles of fossil-fuel emissions, biosphere–atmosphere exchange, and meteorology in regulating the spatial distribution of CO₂ near the surface over the contiguous United States. Three sets of net ecosystem exchange (NEE) fluxes were used as input to assess the impact of uncertainty of NEE on CO₂ concentrations simulated by CMAQ. Observational data from six tall tower sites across the country were used to evaluate model performance. In particular, at the Boulder Atmospheric Observatory (BAO), a tall tower site that receives urban emissions from Denver, CO, the CMAQ model using hourly varying, high-resolution CO₂ fossil-fuel emissions from the Vulcan inventory and CarbonTracker optimized NEE reproduced the observed diurnal profile of CO₂ reasonably well but with a low bias in the early morning. The spatial distribution of CO₂ was found to correlate with NOx, SO₂, and CO, because of their similar fossil-fuel emission sources and common transport processes. These initial results from CMAQ demonstrate the potential of using a regional CTM to help interpret CO₂ observations and understand CO₂ variability in space and time. The ability to simulate a full suite of air pollutants in CMAQ will also facilitate investigations of their use as tracers for CO₂ source attribution. This work serves as a proof of concept and the foundation for more comprehensive examinations of CO₂ spatiotemporal variability and various uncertainties in the future.

Implications: Atmospheric CO₂ has long been modeled and studied on continental to global scales to understand the global carbon cycle. This work demonstrates the potential of modeling and studying CO₂ variability at fine spatiotemporal scales with CMAQ, which has been applied extensively, to study traditionally regulated air pollutants. The abundant observational records of these air pollutants and successful experience in studying and reducing their emissions may be useful for verifying CO₂ emissions. Although there remains much more to further investigate, this work opens up a discussion on whether and how to study CO₂ as an air pollutant.     

Integrated assessment modeling of atmospheric pollutants in the Southern Appalachian Mountains: Part II. Fine particulate matter and visibility

As part of the Southern Appalachian Mountains Initiative, a comprehensive air quality modeling system was developed to evaluate potential emission control strategies to reduce atmospheric pollutant levels at the Class I areas located in the Southern Appalachian Mountains. Six multiday episodes between 1991 and 1995 were simulated, and the skill of the modeling system was evaluated. Two papers comprise various parts of this study. Part I details the ozone model performance and the methodology that was used to scale discrete episodic pollutant levels to seasonal and annual averages. This paper (part II) addresses issues involved with modeling particulate matter (PM) and its relationship to visibility. For most of the episodes, the fractional error was approximately 50% or less for the major constituents of the fine PM (i.e., sulfate [SO4] and organics) in the region. The mean normalized errors and fractional errors are generally larger for the NO3 and soil components, but these components are relatively small. Variations in modeling bias with pollutant levels were also examined. The model showed a systematic overestimation for low levels and an underestimation for high levels for most PM species. For ammonium, the model showed better performance at lower SO4 concentrations when the measured SO4 was assumed to be completely neutralized (ammonium sulfate) and better performance at higher SO4 concentrations when the partially neutralized (ammonium bisulfate) assumption was made. The contributions of various components of PM to reductions in visibility were also calculated; SO4 was found to be the major contributor.     

Selenium content of rice,mixed plant foods and fish from Bangladesh

Static and dynamic adsorption studies of Co (II) ions have been undertaken at fixed pH and ionic strength taking binary biopolymeric beads of cross-linked calcium alginate and carboxy methylcellulose as biosorbents. The adsorption data were applied to Langmuir and Freundlich isotherm equations and various static parameters were calculated. The dynamic nature of adsorption process was quantified in terms of several kinetic constants such as rate constants for adsorption (K) and Lagergreen rate constant (K _ad). The influence of various experimental parameters such as solid-to-liquid ratio, pH, and temperature, the presence of salts and chemical composition of biopolymeric beads were investigated on the adsorption of cobalt ions.     

Preliminary evaluation of the Community Multiscale Air Quality model for 2002 over the Southeastern United States

The Visibility Improvement State and Tribal Association of the Southeast (VISTAS) is one of five Regional Planning Organizations that is charged with the management of haze, visibility, and other regional air quality issues in the United States. The VISTAS Phase I work effort modeled three episodes (January 2002, July 1999, and July 2001) to identify the optimal model configuration(s) to be used for the 2002 annual modeling in Phase II. Using model configurations recommended in the Phase I analysis, 2002 annual meteorological (Mesoscale Meterological Model [MM5]), emissions (Sparse Matrix Operator Kernal Emissions [SMOKE]), and air quality (Community Multiscale Air Quality [CMAQ]) simulations were performed on a 36-km grid covering the continental United States and a 12-km grid covering the Eastern United States. Model estimates were then compared against observations. This paper presents the results of the preliminary CMAQ model performance evaluation for the initial 2002 annual base case simulation. Model performance is presented for the Eastern United States using speciated fine particle concentration and wet deposition measurements from several monitoring networks. Initial results indicate fairly good performance for sulfate with fractional bias values generally within +/-20%. Nitrate is overestimated in the winter by approximately +50% and underestimated in the summer by more than -100%. Organic carbon exhibits a large summer underestimation bias of approximately -100% with much improved performance seen in the winter with a bias near zero. Performance for elemental carbon is reasonable with fractional bias values within +/- 40%. Other fine particulate (soil) and coarse particular matter exhibit large (80-150%) overestimation in the winter but improved performance in the summer. The preliminary 2002 CMAQ runs identified several areas of enhancements to improve model performance, including revised temporal allocation factors for ammonia emissions to improve nitrate performance and addressing missing processes in the secondary organic aerosol module to improve OC performance.     

An Integrated Framework for Multipollutant Air Quality Management and Its Application in Georgia

Air protection agencies in the United States increasingly confront non-attainment of air quality standards for multiple pollutants sharing interrelated emission origins. Traditional approaches to attainment planning face important limitations that are magnified in the multipollutant context. Recognizing those limitations, the Georgia Environmental Protection Division has adopted an integrated framework to address ozone, fine particulate matter, and regional haze in the state. Rather than applying atmospheric modeling merely as a final check of an overall strategy, photochemical sensitivity analysis is conducted upfront to compare the effectiveness of controlling various precursor emission species and source regions. Emerging software enables the modeling of health benefits and associated economic valuations resulting from air pollution control. Photochemical sensitivity and health benefits analyses, applied together with traditional cost and feasibility assessments, provide a more comprehensive characterization of the implications of various control options. The fuller characterization both informs the selection of control options and facilitates the communication of impacts to affected stakeholders and the public. Although the integrated framework represents a clear improvement over previous attainment-planning efforts, key remaining shortcomings are also discussed.     

Integrated assessment modeling of atmospheric pollutants in the Southern Appalachian Mountains. Part I: hourly and seasonal ozone

Recently, a comprehensive air quality modeling system was developed as part of the Southern Appalachians Mountains Initiative (SAMI) with the ability to simulate meteorology, emissions, ozone, size- and composition-resolved particulate matter, and pollutant deposition fluxes. As part of SAMI, the RAMS/EMS-95/URM-1ATM modeling system was used to evaluate potential emission control strategies to reduce atmospheric pollutant levels at Class I areas located in the Southern Appalachians Mountains. This article discusses the details of the ozone model performance and the methodology that was used to scale discrete episodic pollutant levels to seasonal and annual averages. The daily mean normalized bias and error for 1-hr and 8-hr ozone were within U.S. Environment Protection Agency guidance criteria for urban-scale modeling. The model typically showed a systematic overestimation for low ozone levels and an underestimation for high levels. Because SAMI was primarily interested in simulating the growing season ozone levels in Class I areas, daily and seasonal cumulative ozone exposure, as characterized by the W126 index, were also evaluated. The daily ozone W126 performance was not as good as the hourly ozone performance; however, the seasonal ozone W126 scaled up from daily values was within 17% of the observations at two typical Class I areas of the SAMI region. The overall ozone performance of the model was deemed acceptable for the purposes of SAMI's assessment.     

Selenium and arsenic content of agricultural soils from Bangladesh and Nepal

Arsenic (As) contamination of the available domestic drinking water from shallow aquifers to villagers in Bangladesh often exceeds the newest WHO standard of <10 µg As L^?1 and the older Bangladeshi standard of <50 µg As L^?1. An estimated 9.2 million shallow tube wells in Bangladesh deliver water to 97% of the rural population, placing an estimated 57 million people at risk for arsenicosis. The contamination of drinking water by As extends to W. Bengal, India and Nepal. The same shallow aquifers used for domestic water are also used to irrigate food crops, particularly rice. Irrigation adds As to soils and increases exposure of the population to additional As via foods consumed. Selenium (Se), an essential trace mineral found in soils, is absorbed by plants, entering the human food chain. It was suggested that a low dietary intake of Se may be contributing to the problem of human arsenicosis in Bangladesh. Dietary Se acts as a natural antidote to As by (1) accelerating As excretion, (2) sequestering As by complexation and (3) as an antioxidant component of the enzyme glutathione peroxidase that may counteract the prooxidant effects of As that contribute to arsenicosis and cancer. Analysis of 70 agricultural soil samples from Bangladesh by fluorimetry, ICP-AES and Neutron Activation Analysis showed the soils analyzed to be high in As (～33 µg g^?1) and biologically low in soluble Se (～0.02 µg g^?1). A low dietary intake of Se related to low soil content and this mineral in foods may be contributing to human arsenicosis in the Ganges–Brahmaputra delta.