An Assessment of the Emissions Inventory Processing Systems EMS-2001 and SMOKE in Grid-Based Air Quality Models

Abstract

In the United States, emission processing models such as Emissions Modeling System-2001 (EMS-2001), Emissions Preprocessor System-Version 2.5 (EPS2.5), and the Sparse Matrix Operator Kernel Emissions (SMOKE) model are currently being used to generate gridded, hourly, speciated emission inputs for urban and regional-scale photochemical models from aggregated pollutant inventories. In this study, two models, EMS-2001 and SMOKE, were applied with their default internal data sets to process a common inventory database for a high ozone (O₃) episode over the eastern United States using the Carbon Bond IV (CB4) chemical speciation mechanism. A comparison of the emissions processed by these systems shows differences in all three of the major processing steps performed by the two models (i.e., in temporal allocation, spatial allocation, and chemical speciation). Results from a simulation with a photochemical model using these two sets of emissions indicate differences on the order of ±20 ppb in the predicted 1-hr daily maximum O₃ concentrations. It is therefore critical to develop and implement more common and synchronized temporal, spatial, and speciation cross-reference systems such that the processes within each emissions model converge toward reasonably similar results. This would also help to increase confidence in the validity of photochemical grid model results by reducing one aspect of modeling uncertainty.     

An assessment of the emissions inventory processing systems EMS-2001 and SMOKE in grid-based air quality models

In the United States, emission processing models such as Emissions Modeling System-2001 (EMS-2001), Emissions Preprocessor System-Version 2.5 (EPS2.5), and the Sparse Matrix Operator Kernel Emissions (SMOKE) model are currently being used to generate gridded, hourly, speciated emission inputs for urban and regional-scale photochemical models from aggregated pollutant inventories. In this study, two models, EMS-2001 and SMOKE, were applied with their default internal data sets to process a common inventory database for a high ozone (O3) episode over the eastern United States using the Carbon Bond IV (CB4) chemical speciation mechanism. A comparison of the emissions processed by these systems shows differences in all three of the major processing steps performed by the two models (i.e., in temporal allocation, spatial allocation, and chemical speciation). Results from a simulation with a photochemical model using these two sets of emissions indicate differences on the order of +/- 20 ppb in the predicted 1-hr daily maximum O3 concentrations. It is therefore critical to develop and implement more common and synchronized temporal, spatial, and speciation cross-reference systems such that the processes within each emissions model converge toward reasonably similar results. This would also help to increase confidence in the validity of photochemical grid model results by reducing one aspect of modeling uncertainty.     

Compilation of a database on the composition of anthropogenic VOC emissions for atmospheric modeling in Europe

To analyse and generate air pollution control strategies and policies, e.g. efficient abatement strategies or action plans that lead to a fulfilment of air quality aims, atmospheric dispersion models (CTMs) have to be used. These models include a chemical model, where the numerous volatile organic compounds (VOCs) species are lumped together in classes. On the other hand, emission inventories usually report only total non-methane VOC (NMVOC), but not a subdivision into these classes. Thus, VOC species profiles are needed that resolve total NMVOC emission data. The objective of this publication is to present the results of a compilation of VOC species profiles that dissolve total VOC into single-species profiles for all relevant anthropogenic emission source categories and the European situation. As in atmospheric dispersion models usually modules for generating biogenic emissions are directly included, only anthropogenic emissions are addressed. VOC species profiles for 87 emission source categories have been developed. The underlying data base can be used to generate the data for all chemical mechanisms. The species profiles have been generated using recent measurements and studies on VOC species resolution and thus represent the current state of knowledge in this area. The results can be used to create input data for atmospheric dispersion models in Europe.The profiles, especially those for solvent use, still show large uncertainties. There is still an enormous need for further measurements to achieve an improved species resolution. In addition, the solvent use directive and the DECOPAINT directive of the European Commission will result in a change of the composition of paints; more water-based and high-solid paints will be used; thus the species resolution will change drastically in the next years. Of course, the species resolution for combustion and production processes also requires further improvement.     

Estimation of atmospheric trace metal emissions in Vilnius City, Lithuania, using vertical concentration gradient and road tunnel measurement data

A new approach for the estimation of trace metal emissions in Vilnius city was implemented, using vertical concentration profiles in the urban boundary layer and road tunnel measurement data. Heavy metal concentrations were examined in fine and coarse particle fractions using a virtual impactor (cut-off size diameter 2.5 μm). Negative vertical concentration gradients were obtained for all metals (Ba, Pb, V, Sb, Zn) and both fractions. It was estimated that the vertical concentration gradient was formed due to emissions from an area of about 12 km². Road tunnel measurements indicated that trace metal concentrations on fine particles were lower than those on coarse particles, which suggested that re-emitted road dust was highly enriched in trace metal due to historic emissions within the tunnel. Emission rates of different pollutants in the road tunnel were calculated using pollutant concentration differences at the tunnel entrance and exit and traffic flow data. Heavy metal emission rates from the area of Vilnius city were estimated using the vertical gradient of heavy metal concentrations and the coefficient of turbulent mixing, as derived from meteorological measurement data. The emission values calculated by the two different methods coincided reasonably well, which indicated that the main source of airborne trace metals in Vilnius city is traffic. The potential of the vertical concentration gradient method for the direct estimation of urban heavy metal emissions was demonstrated.     

Particulate matter speciation profiles for light-duty gasoline vehicles in the United States

Representative profiles for particulate matter particles less than or equal to 2.5 µm (PM_2.5) are developed from the Kansas City Light-Duty Vehicle Emissions Study for use in the U.S. Environmental Protection Agency (EPA) vehicle emission model, the Motor Vehicle Emission Simulator (MOVES), and for inclusion in the EPA SPECIATE database for speciation profiles. The profiles are compatible with the inputs of current photochemical air quality models, including the Community Multiscale Air Quality Aerosol Module Version 6 (AE6). The composition of light-duty gasoline PM_2.5 emissions differs significantly between cold start and hot stabilized running emissions, and between older and newer vehicles, reflecting both impacts of aging/deterioration and changes in vehicle technology. Fleet-average PM_2.5 profiles are estimated for cold start and hot stabilized running emission processes. Fleet-average profiles are calculated to include emissions from deteriorated high-emitting vehicles that are expected to continue to contribute disproportionately to the fleet-wide PM_2.5 emissions into the future. The profiles are calculated using a weighted average of the PM_2.5 composition according to the contribution of PM_2.5 emissions from each class of vehicles in the on-road gasoline fleet in the Kansas City Metropolitan Statistical Area. The paper introduces methods to exclude insignificant measurements, correct for organic carbon positive artifact, and control for contamination from the testing infrastructure in developing speciation profiles. The uncertainty of the PM_2.5 species fraction in each profile is quantified using sampling survey analysis methods. The primary use of the profiles is to develop PM_2.5 emissions inventories for the United States, but the profiles may also be used in source apportionment, atmospheric modeling, and exposure assessment, and as a basis for light-duty gasoline emission profiles for countries with limited data.

Implications: PM_2.5 speciation profiles were developed from a large sample of light-duty gasoline vehicles tested in the Kansas City area. Separate PM_2.5 profiles represent cold start and hot stabilized running emission processes to distinguish important differences in chemical composition. Statistical analysis was used to construct profiles that represent PM_2.5 emissions from the U.S. vehicle fleet based on vehicles tested from the 2005 calendar year Kansas City metropolitan area. The profiles have been incorporated into the EPA MOVES emissions model, as well as the EPA SPECIATE database, to improve emission inventories and provide the PM_2.5 chemical characterization needed by CMAQv5.0 for atmospheric chemistry modeling.     

Evaluation of total volatile organic compound emissions from adhesives based on chamber tests

In 1997, Homeswest in western Australia and Murdoch University developed a project to construct low-allergen houses (LAHs) in a newly developed suburb. Before the construction of LAHs, all potential volatile organic compound (VOC) emission materials used in LAHs are required to be measured to ensure that they are low total VOC (TVOC) emission materials. This program was developed based on this purpose. In recent times, the number of complaints about indoor air pollution caused by VOCs has increased. A number of surveys of indoor VOCs have indicated that many indoor materials contribute to indoor air pollution. Although some studies have been conducted on the characteristics of VOC emissions from adhesives, most of them were focused on VOC emissions from floor adhesives. Few measurements of VOC emissions from adhesives used for wood, fabrics, and leather are available. Furthermore, most research on VOC emissions from adhesives has been done in countries with cool climates, where ventilation rates in the indoor environment are lower than those in Mediterranean climates, due to energy conservation. VOCs emitted from adhesives have not been sufficiently researched to prepare an emission inventory to predict indoor air quality and to determine both exposure levels for the Australian population and the most appropriate strategies to reduce exposure. An environmental test chamber with controlled temperature, relative humidity, and airflow rate was used to evaluate emissions of TVOCs from three adhesives used frequently in Australia. The quantity of TVOC emissions was measured by a gas chromatography/flame ionization detector. The primary VOCs emitted from each adhesive were detected by gas chromatography/mass spectrometry. The temporal change of TVOC concentrations emitted from each adhesive was tested. A double-exponential equation was then developed to evaluate the characteristics of TVOC emissions from these three adhesives. With this double-exponential model, the physical processes of TVOC emissions can be explained, and a variety of emission parameters can be calculated. These emission parameters could be used to estimate real indoor TVOC concentrations in Mediterranean climates.     

PCDD/F emissions from heavy duty vehicle diesel engines

The currently available information on PCDD/F emissions from diesel vehicles is briefly surveyed. Considerable uncertainty is identified concerning the emissions from heavy duty diesel trucks which have been measured only twice so far. These measurements led to emission factors differing by a factor of 200; similar discrepancy was also revealed by measurements of ambient air in traffic tunnels. New PCDD/F emission measurement results are presented which have been carried out at the exhaust systems of a stationary engine and of a modern heavy duty vehicle engine at transient operation conditions simulated on a test bench. PCDD/F concentrations in the exhaust gases were found to be in the range of control blank samples. Based on the highest concentration observed in the truck engine exhaust (9.7 pg I-TEQ/dry standard m3) a worst case estimate of the annual PCDD/F emission freight from diesel fuel combustion in the European countries of about 30 g I-TEQ/year is calculated. This emission appears to be irrelevant compared to the overall emission rate of more than 6,000 g I-TEQ/year being inventoried recently. Finally the possibilities to link congener/homologue profiles of diesel emission to profiles found in food or human samples are discussed.     

Modeling emissions for three-dimensional atmospheric chemistry transport models

Poor air quality is still a threat for human health in many parts of the world. In order to assess measures for emission reductions and improved air quality, three-dimensional atmospheric chemistry transport modeling systems are used in numerous research institutions and public authorities. These models need accurate emission data in appropriate spatial and temporal resolution as input. This paper reviews the most widely used emission inventories on global and regional scales and looks into the methods used to make the inventory data model ready. Shortcomings of using standard temporal profiles for each emission sector are discussed, and new methods to improve the spatiotemporal distribution of the emissions are presented. These methods are often neither top-down nor bottom-up approaches but can be seen as hybrid methods that use detailed information about the emission process to derive spatially varying temporal emission profiles. These profiles are subsequently used to distribute bulk emissions such as national totals on appropriate grids. The wide area of natural emissions is also summarized, and the calculation methods are described. Almost all types of natural emissions depend on meteorological information, which is why they are highly variable in time and space and frequently calculated within the chemistry transport models themselves. The paper closes with an outlook for new ways to improve model ready emission data, for example, by using external databases about road traffic flow or satellite data to determine actual land use or leaf area. In a world where emission patterns change rapidly, it seems appropriate to use new types of statistical and observational data to create detailed emission data sets and keep emission inventories up-to-date.

Implications: Emission data are probably the most important input for chemistry transport model (CTM) systems. They need to be provided in high spatial and temporal resolution and on a grid that is in agreement with the CTM grid. Simple methods to distribute the emissions in time and space need to be replaced by sophisticated emission models in order to improve the CTM results. New methods, e.g., for ammonia emissions, provide grid cell–dependent temporal profiles. In the future, large data fields from traffic observations or satellite observations could be used for more detailed emission data.     

Realistic Mixing Depths for Above Ground Aircraft Emissions

Analysis of vertical temperature soundings at Los Angeles International Airport (LAX) shows that a conservative height of the inversion base for pollutant containment purposes is 490 ft (150 m). This altitude is considerably less than the 3000 ft (914 m) pollution containment altitude assumed by the EPA in preparing their emission inventory for the airport. (Figure 1.) After correcting the EPA emission inventory to reflect a real world inversion height, the emission inventory for aircraft at Los Angeles International Airport is estimated to be approximately 50% less. Aircraft thus become a less significant pollution source and consideration should be given to relaxing engine emission control requirements accordingly.

This paper examines current emission control philosophy, which according to the EPA should be based upon the significance of the particular polluting source. The problem of accounting for above ground aircraft emissions is then considered. Daily inversion height data are then used to determine a realistic vertical containment altitude for aircraft emissions. Problems in obtaining good inversion data are described. Finally, aircraft emissions at Los Angeles International Airport are adjusted to reflect real world inversion conditions on those days when the inversion height is low enough to influence significantly air pollution levels. Recommendations are made for additional research leading to possible change to NO_x emission control requirements for aircraft.     

Ammonia emissions from naturally ventilated dairy cattle buildings and outdoor concrete yards in Portugal

There is a lack of information on ammonia (NH₃) emissions from cattle housing systems in Mediterranean countries, with most published data deriving from NW Europe. An investigation was carried out in NW Portugal to quantify NH₃ emissions for the main types of dairy cattle buildings in Portugal, i.e. naturally ventilated buildings and outdoor concrete yards, and to derive robust emission factors (EFs) for these conditions and compare with EFs used elsewhere in Europe. Measurements were made throughout a 12-month period using the passive flux sampling method in the livestock buildings and the equilibrium concentration technique in outdoor yards.The mean NH₃ emission factor for the whole housing system (buildings + outdoor yards) was 43.7 g NH₃–N LU^?1 day^?1 and for outdoor concrete yards used by dairy cattle was 26.6 g NH₃–N LU^?1 day^?1. Expressing NH₃ emission in terms of the quantity of liquid milk produced gave similar values across the three dairy farms studied (with a mean of 2.3 kg N ton-milk^?1 produced) and may have advantages when comparing different farming systems. In dairy houses with outdoor yards, NH₃ emissions from the yard area contributed to 69–92% of total emissions from this housing system. Emissions were particularly important during spring and summer seasons from outdoor yards with NH₃ emitted in this period accounting for about 72% of annual emissions from outdoor yards. Mean NH₃ emission factors derived for this freestall housing system and outdoor concrete yards used by dairy cattle in Portugal were higher than those measured in northern Europe. In addition, values of animal N excretion estimated in this study were greater than official National standard values. If these emissions are typical for Portuguese dairy systems, then the current National inventory underestimates emissions from this source in NW of Portugal, because of the use of lower standard values of N excretion by dairy cattle.     

Intra- and inter-annual variability of VOC emissions from natural and semi-natural vegetation in Europe and neighbouring countries

Biogenic VOC emission estimates from the earth's surface are crucial input parameters in air quality models. Knowledge accumulated in the last years about BVOC source distributions and chemical compound species emission profiles in Europe as well as the demand of air quality modellers for a finer resolution in space and time of BVOC estimates have led to the set-up of new emission modelling systems. An updated fast BVOC emission modelling platform explicitly considering the seasonality of emission potentials and leaf temperature gradients in forest canopies by the semi-empirical emission module (seBVOC) will be proposed and used for estimating hourly values of chemical compound-specific emissions in Europe (33–68° north; 10° west to 40° east) in the years 1997, 2000, 2001, and 2003. Spatial resolution will be 10 km by 10 km. The database used contains latest land and forest distributions, updated foliar biomass densities, leaf area indices (LAI), and plant as well as chemical compound-specific emission potentials, if available. Meteorological input parameters for the respective years will be generated using the non-hydrostatic meteorological model MM5. Highest BVOC emissions occur in daytime hours around noon from the end of May to mid-August in the Mediterranean area and from the mid of June to the end of July in the boreal forests. Comparison of 3 BVOC model approaches will reveal that for July 2003, the European isoprene and monoterpene totals range from 1124 Gg to 1446 Gg and from 338 Gg to 1112 Gg, respectively. Small-scale deviations may be as high as ±0.6 Mg km^?2 for July 2003, reflecting the current uncertainty range for BVOC estimates. Key sources of errors in inventories are still insufficiently detailed land use data for some areas and lacking chemically speciated plant-specific emission potentials in particular in boreal, south-eastern, and northern African landscapes. The hourly emissions of isoprene, speciated terpenes, and oxyVOC have been made available by the NatAir database.     

Trends in onroad transportation energy and emissions

Globally, 1.3 billion on-road vehicles consume 79 quadrillion BTU of energy, mostly gasoline and diesel fuels, emit 5.7 gigatonnes of CO₂, and emit other pollutants to which approximately 200,000 annual premature deaths are attributed. Improved vehicle energy efficiency and emission controls have helped offset growth in vehicle activity. New technologies are diffusing into the vehicle fleet in response to fuel efficiency and emission standards. Empirical assessment of vehicle emissions is challenging because of myriad fuels and technologies, intervehicle variability, multiple emission processes, variability in operating conditions, and varying capabilities of measurement methods. Fuel economy and emissions regulations have been effective in reducing total emissions of key pollutants. Real-world fuel use and emissions are consistent with official values in the United States but not in Europe or countries that adopt European standards. Portable emission measurements systems, which uncovered a recent emissions cheating scandal, have a key role in regulatory programs to ensure conformity between “real driving emissions” and emission standards. The global vehicle fleet will experience tremendous growth, especially in Asia. Although existing data and modeling tools are useful, they are often based on convenience samples, small sample sizes, large variability, and unquantified uncertainty. Vehicles emit precursors to several important secondary pollutants, including ozone and secondary organic aerosols, which requires a multipollutant emissions and air quality management strategy. Gasoline and diesel are likely to persist as key energy sources to mid-century. Adoption of electric vehicles is not a panacea with regard to greenhouse gas emissions unless coupled with policies to change the power generation mix. Depending on how they are actually implemented and used, autonomous vehicles could lead to very large reductions or increases in energy consumption. Numerous other trends are addressed with regard to technology, emissions controls, vehicle operations, emission measurements, impacts on exposure, and impacts on public health.

Implications: Without specific policies to the contrary, fossil fuels are likely to continue to be the major source of on-road vehicle energy consumption. Fuel economy and emission standards are generally effective in achieving reductions per unit of vehicle activity. However, the number of vehicles and miles traveled will increase. Total energy use and emissions depend on factors such as fuels, technologies, land use, demographics, economics, road design, vehicle operation, societal values, and others that affect demand for transportation, mode choice, energy use, and emissions. Thus, there are many opportunities to influence future trends in vehicle energy use and emissions.     

Process analysis of a regional air pollution episode over Pearl River Delta Region,China, using the MM5-CMAQ model

This study focuses on the influences of a warm high-pressure meteorological system on aerosol pollutants, employing the simulations by the Models-3/CMAQ system and the observations collected during October 10–12, 2004, over the Pearl River Delta (PRD) region. The results show that the spatial distributions of air pollutants are generally circular near Guangzhou and Foshan, which are cities with high emissions rates. The primary pollutant is particulate matter (PM) over the PRD. MM5 shows reasonable performance for major meteorological variables (i.e., temperature, relative humidity, wind direction) with normalized mean biases (NMB) of 4.5–38.8% and for their time series. CMAQ can capture one peak of all air pollutant concentrations on October 11, but misses other peaks. The CMAQ model systematically underpredicts the mass concentrations of all air pollutants. Compared with chemical observations, SO₂ and O₃ are predicted well with a correlation coefficient of 0.70 and 0.65. PM_2.5 and NO are significantly underpredicted with an NMB of 43% and 90%, respectively. The process analysis results show that the emission, dry deposition, horizontal transport, and vertical transport are four main processes affecting air pollutants. The contributions of each physical process are different for the various pollutants. The most important process for PM₁₀ is dry deposition, and for NO_x it is transport. The contributions of horizontal and vertical transport processes vary during the period, but these two processes mostly contribute to the removal of air pollutants at Guangzhou city, whose emissions are high. For this high-pressure case, the contributions of the various processes show high correlations in cities with the similar geographical attributes. According to the statistical results, cities in the PRD region are divided into four groups with different features. The contributions from local and nonlocal emission sources are discussed in different groups.

Implications: The characteristics of aerosol pollution episodes are intensively studied in this work using the high-resolution modeling system MM5/SMOKE/CMAQ, with special efforts on examining the contributions of different physical and chemical processes to air concentrations for each city over the PRD region by a process analysis method, so as to provide a scientific basis for understanding the formation mechanism of regional aerosol pollution under the high-pressure system over PRD.     

Comprehensive primary particulate organic characterization of vehicular exhaust emissions in France

A study to characterize primary particulate matter (PM_2.5 and PM₁₀) from the French vehicular fleet was conducted during winter 2008, in a tunnel in Marseille, France. The carbonaceous fraction represents 70% of the aerosol mass and elemental carbon fraction (EC) represent 60% of the carbonaceous fraction. The organic carbon OC was characterized in term of its water soluble fraction, functionalization rate and HULIS content. Seventy trace organic compounds including alkanes, polycyclic aromatic hydrocarbons (PAH), petroleum biomarkers and carboxylic acids were also quantified, in order to determine an organic emission profile for chemical mass balance modeling studies. Such source profiles were still missing in Europe and particularly in France. The profile obtained in this study is consistent with profiles determined in tunnel or dynamometer studies performed in other countries during the last ten years. These results suggest that organic compounds profiles from vehicular exhaust emissions are not significantly influenced by the geographic area and are thus suitable for use in aerosol source apportionment modeling applied across extensive regions. The chemical profile determined here is very similar to those obtained for diesel emissions with high concentrations of EC relative to OC (EC/OC = 1.8) and low concentrations of the higher molecular weight PAH. These results are consistent with the high proportion of diesel vehicles in the French fleet (49%).     

Quality considerations of European PM emission inventories

This paper reviews information on emission inventories of particulate matter (PM) in Europe. A large body of scientific literature is available to cover many different aspects. Studies focus on specific sources or source sectors (road transport as well as off-road machinery, domestic heating, industry, agriculture, and natural sources), among which especially road transport emissions are clearly best established. Emission inventories comprising all sources are available for specific European regions, often pointing out regional differences, but also for the entire continent. Still these inventories often are not able to satisfy the needs. Due to PM specific circumstances such as the large number of sources, very different release pathways and differences of the individual particles in terms of chemical composition or size, it is very difficult to appropriately handle measurement conditions to arrive at adequate emission factors, especially when emission points cannot be defined clearly. Information on fugitive emissions (caused by wind shear, material transfer processes or other mechanical forces from non-point sources) is sparse, except for road traffic emissions where recent data seems to converge. The problem of data gaps concerns activities in industry (quarries), agriculture, but also natural particles like sea salt and wind-blown dust. Comparing complete inventories to independent efforts in assessing emissions, e.g. atmospheric measurements combined with source apportionment, allows to better understand and quantify the reliability of inventory data. Methodological improvements and harmonization currently under way in Europe will focus efforts and allow for more reliable PM inventories in the near future.     

Quantification of emission factor uncertainty

Emissions factors are important for estimating and characterizing emissions from sources of air pollution. There is no quantitative indication of uncertainty for these emission factors, most factors do not have an adequate data set to compute uncertainty, and it is very difficult to locate the data for those that do. The objectives are to compare the current emission factors of Electric Generating Unit NOx sources with currently available continuous emission monitoring data, develop quantitative uncertainty indicators for the Environmental Protection Agency (EPA) data quality rated emission factors, and determine the possible ranges of uncertainty associated with EPA's data quality rating of emission factors. EPA's data letter rating represents a general indication of the robustness of the emission factor and is assigned based on the estimated reliability of the tests used to develop the factor and on the quantity and representativeness of the data. Different sources and pollutants that have the same robustness in the measured emission factor and in the representativeness of the measured values are assumed to have a similar quantifiable uncertainty. For the purposes of comparison, we assume that the emission factor estimates from source categories with the same letter rating have enough robustness and consistency that we can quantify the uncertainty of these common emission factors based on the qualitative indication of data quality which is known for almost all factors. The results showed that EPA's current emission factor values for NOx emissions from combustion sources were found to be reasonably representative for some sources; however AP-42 values should be updated for over half of the sources to reflect current data. The quantified uncertainty ranges were found to be 25-62% for A rated emission factors, 45-75% for B rated emission factors, 60-82% for C rated emission factors, and 69-86% for D rated emission factors, and 82-92% for E rated emission factors.     

Lidar-assisted measurement of PM10 emissions from agricultural tilling in California's San Joaquin Valley – Part II: emission factors

Emission factors for agricultural operations are needed in order to develop reliable PM₁₀ emissions inventories and air quality models for air basins with significant agricultural land use. A framework was developed to analyze the PM₁₀ vertical profiles collected downwind of tilling operations in the San Joaquin Valley. The methods calculate emission factors on the basis of profile shape and assign quality ratings to each land preparation test. Uncertainties in the calculated emission factors and plume heights were used as one criterion for evaluating the relative quality of the reported emission factor. Other quality ratings were based on the magnitude of the difference in measured up- and downwind concentrations, wind direction, whether the tests were conducted near the edges of the field, and how well the proposed model fit the profile data. The emission factors from different operations were compared taking the quality of the emission factor into account. Plume heights and emission factors for 24 valid test profiles ranged from 2 to 20 m (mean=9.8; SD=3.6; median=9.8) and zero to 800 mg m⁻² (mean=152; SD=240; median=43), respectively. Key environmental properties governing PM₁₀ emission from these operations include relative humidity, soil moisture and vertical temperature gradient. Surprisingly, no discernable relationships were found between implement type or wind speed and the measured emission factors.     

Development of a United States-Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study

The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was commissioned to investigate the sources of haze at Big Bend National Park in southwest Texas. The modeling domain of the BRAVO Study includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The first regional-scale Mexican emissions inventory designed for air-quality modeling applications was developed for 10 northern Mexican states, the Tula Industrial Park in the state of Hidalgo, and the Popocatépetl volcano in the state of Puebla. Emissions data were compiled from numerous sources, including the U.S. Environmental Protection Agency (EPA), the Texas Natural Resources Conservation Commission (now Texas Commission on Environmental Quality), the Eastern Research Group, the Minerals Management Service, the Instituto Nacional de Ecología, and the Instituto Nacional de Estadistica Geografía y Informática. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) < 10 microm in aerodynamic diameter, and PM < 2.5 microm in aerodynamic diameter. Wind-blown dust and biomass burning were not included in the inventory, although high concentrations of dust and organic PM attributed to biomass burning have been observed at Big Bend National Park. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions inventory for Mexico with other emerging Mexican emission inventories illustrates their uncertainty.     

Development of a database for chemical mechanism assignments for volatile organic emissions

The development of a database for making model species assignments when preparing total organic gas (TOG) emissions input for atmospheric models is described. This database currently has assignments of model species for 12 different gas-phase chemical mechanisms for over 1700 chemical compounds and covers over 3000 chemical categories used in five different anthropogenic TOG profile databases or output by two different biogenic emissions models. This involved developing a unified chemical classification system, assigning compounds to mixtures, assigning model species for the mechanisms to the compounds, and making assignments for unknown, unassigned, and nonvolatile mass. The comprehensiveness of the assignments, the contributions of various types of speciation categories to current profile and total emissions data, inconsistencies with existing undocumented model species assignments, and remaining speciation issues and areas of needed work are also discussed. The use of the system to prepare input for SMOKE, the Speciation Tool, and for biogenic models is described in the supplementary materials. The database, associated programs and files, and a users manual are available online at http://www.cert.ucr.edu/~carter/emitdb.

Implications: Assigning air quality model species to the hundreds of emitted chemicals is a necessary link between emissions data and modeling effects of emissions on air quality. This is not easy and makes it difficult to implement new and more chemically detailed mechanisms in models. If done incorrectly, it is similar to errors in emissions speciation or the chemical mechanism used. Nevertheless, making such assignments is often an afterthought in chemical mechanism development and emissions processing, and existing assignments are usually undocumented and have errors and inconsistencies. This work is designed to address some of these problems.     

A Top-Down Regional Assessment of Urban Greenhouse Gas Emissions in Europe

This paper provides an account of urban greenhouse gas (GHG) emissions from 40 countries in Europe and examines covariates of emissions levels. We use a “top-down” analysis of emissions as spatially reported in the Emission Dataset for Global Atmospheric Research supplemented by Carbon Monitoring for Action from 1153 European cities larger than 50 000 population in 2000 (comprising >81 % of the total European urban population). Urban areas are defined spatially and demographically by the Global Rural Urban Mapping Project. We compare these results with “bottom-up” carbon accounting method results for cities in the region. Our results suggest that direct (Scopes 1 and 2) GHG emissions from urban areas range between 44 and 54 % of total anthropogenic emissions for the region. While individual urban GHG footprints vary from bottom-up studies, both the mean differences and the regional energy-related GHG emission share support previous findings. Correlation analysis indicates that the urban GHG emissions in Europe are mainly influenced by population size, density, and income and not by biophysical conditions. We argue that these data and methods of analysis are best used at the regional or higher scales.