Air emission inventories in North America: a critical assessment

Although emission inventories are the foundation of air quality management and have supported substantial improvements in North American air quality, they have a number of shortcomings that can potentially lead to ineffective air quality management strategies. Major reductions in the largest emissions sources have made accurate inventories of previously minor sources much more important to the understanding and improvement of local air quality. Changes in manufacturing processes, industry types, vehicle technologies, and metropolitan infrastructure are occurring at an increasingly rapid pace, emphasizing the importance of inventories that reflect current conditions. New technologies for measuring source emissions and ambient pollutant concentrations, both at the point of emissions and from remote platforms, are providing novel approaches to collecting data for inventory developers. Advances in information technologies are allowing data to be shared more quickly, more easily, and processed and compared in novel ways that can speed the development of emission inventories. Approaches to improving quantitative measures of inventory uncertainty allow air quality management decisions to take into account the uncertainties associated with emissions estimates, providing more accurate projections of how well alternative strategies may work. This paper discusses applications of these technologies and techniques to improve the accuracy, timeliness, and completeness of emission inventories across North America and outlines a series of eight recommendations aimed at inventory developers and air quality management decision-makers to improve emission inventories and enable them to support effective air quality management decisions for the foreseeable future.     

Reflecting on progress since the 2005 NARSTO emissions inventory report

Emission inventories are the foundation for cost-effective air quality management activities. In 2005, a report by the public/private partnership North American Research Strategy for Tropospheric Ozone (NARSTO) evaluated the strengths and weaknesses of North American emissions inventories and made recommendations for improving their effectiveness. This paper reviews the recommendation areas and briefly discusses what has been addressed, what remains unchanged, and new questions that have arisen. The findings reveal that all emissions inventory improvement areas identified by the 2005 NARSTO publication have been explored and implemented to some degree. The U.S. National Emissions Inventory has become more detailed and has incorporated new research into previously under-characterized sources such as fine particles and biomass burning. Additionally, it is now easier to access the emissions inventory and the documentation of the inventory via the internet. However, many emissions-related research needs exist, on topics such as emission estimation methods, speciation, scalable emission factor development, incorporation of new emission measurement techniques, estimation of uncertainty, top-down verification, and analysis of uncharacterized sources. A common theme throughout this retrospective summary is the need for increased coordination among stakeholders. Researchers and inventory developers must work together to ensure that planned emissions research and new findings can be used to update the emissions inventory. To continue to address emissions inventory challenges, industry, the scientific community, and government agencies need to continue to leverage resources and collaborate as often as possible. As evidenced by the progress noted, continued investment in and coordination of emissions inventory activities will provide dividends to air quality management programs across the country, continent, and world.

Implications: In 2005, a report by the public/private partnership North American Research Strategy for Tropospheric Ozone (NARSTO) evaluated the strengths and weaknesses of North American air pollution emissions inventories. This paper reviews the eight recommendation areas and briefly discusses what has been addressed, what remains unchanged, and new questions that have arisen. Although progress has been made, many opportunities exist for the scientific agencies, industry, and government agencies to leverage resources and collaborate to continue improving emissions inventories.     

Innovative methods for emission inventory development and evaluation: workshop summary

Emission inventories are an essential tool for evaluating, managing, and regulating air pollution. Refinements and innovations in instruments that measure air pollutants, models that calculate emissions, and techniques for data management and uncertainty assessment are needed to enhance emission inventories. This workshop provided recommendations for improving emission factors, improving emission models, and reducing inventory uncertainty. Communication that increases cooperation between developers and users of inventories is essential. Emission inventories that incorporate these improvements will meet the challenges of the future.     

Real-world vehicle emissions: a summary of the Eleventh Coordinating Research Council On-Road Vehicle Emissions Workshop

The Coordinating Research Council (CRC) held its eleventh workshop in March 2001, focusing on results from the most recent real-world vehicle emissions research. We summarize the presentations from researchers engaged in improving our understanding of the contribution of mobile sources to ambient air quality and emission inventories. Participants in the workshop discussed efforts to improve mobile source emission models and emission inventories, the role of on-board diagnostic (OBD) systems in inspection and maintenance (I/M) programs, particulate matter (PM) emissions, contributions of diesel vehicles to the emission inventory, on-road emissions measurements, fuel effects, unregulated emissions, and microscale and modal emission models, as well as topics for future research.     

Emission inventory for the road transport sector in Sardinia (Italy)

Atmospheric emission inventories are important tools for studying air quality and to set up possible remediation plans in areas characterised by nonattainment of the limit values established by legislation. In industrialised countries a considerable fraction of the emissions is due to road traffic, in particular in urban areas. For this reason emissions from road traffic must be estimated as accurately as possible, a task that can be performed, for the European vehicle fleet, thanks to the availability of the COPERT III methodology. This methodology is powerful and accurate, even if its algorithms can be difficult to apply in a regional emission inventory; moreover the collection of the necessary input data requires a lot of resources and time. This paper describes the road traffic emission inventory estimated for Region Sardinia (Italy) with a bottom-up approach. The estimation has been done by means of a software tool (EMITRA—EMIssions from road TRAnsport) which implements the COPERT III methodology. The resulting emission inventory has been compared against another emission inventory for Sardinia and against emission inventories for other Italian regions, to evaluate its reliability.     

Preparation of mercury emissions inventory for eastern North America

Point and area inventories of anthropogenic mercury emissions documented by US and Canadian environmental agencies have been aggregated into a single archive for analysis and air pollution modeling work. For 5341 point sources and 1634 aggregated area sources, mercury emissions are apportioned among elemental gaseous [Hg(0)], reactive gaseous[Hg(II)], and particulate [Hg(p)] emissions using speciation factors derived from available monitoring measurements. According to this inventory, 4.82 x 10(5) mol of mercury were emitted in calendar year 1996 in the latitude range 24-51 degrees north, and longitude range 64-91 degrees west, which covers most of North America east of the Mississippi River. Using speciation factors consistent with past emission source studies, we find the relative emission proportions among Hg(0):Hg(II):Hg(p) species are 47:35:18. Maps of the various mercury species' emissions patterns are presented. Gridded emission patterns show local mercury emission extremes associated with individual cement production and municipal incineration facilities, and in contrast to past inventories, population centers do not stand out. Considerable uncertainties are still present in estimating emissions from large point sources, as are methods of apportioning emissions among various mercury species.     

Development of a PM2 5 Emissions Inventory for the South Coast Air Basin

ABSTRACT

With the promulgation of a national PM_2.5 ambient air quality standard, it is important that PM_2.5 emissions inventories be developed as a tool for understanding the magnitude of potential PM2.5 violations. Current PM₁₀ inventories include only emissions of primary particulate matter (1 ^ï PM), whereas, based on ambient measurements, both PM₁₀ and PM2.5 emissions inventories will need to include sources of both 1^ï PM and secondary particulate matter (2^ï PM). Furthermore, the U. S. Environmental Protection Agency’s (EPA) current edition of AP-42 includes size distribution data for 1o PM that overestimate the PM_2.5 fraction of fugitive dust sources by at least a factor of 2 based on recent studies.

This paper presents a PM_2.5 emissions inventory developed for the South Coast Air Basin (SCAB) that for the first time includes both 1^ï PM and 2^ï PM. The former is calculated by multiplying PM₁₀ emissions estimates by the PM_2.5/PM₁₀ ratios for different sources. The latter is calculated from estimated emission rates of gas-phase aerosol precursor and gas to aerosol conversion rates consistent with the measured chemical composition of ambient PM_2.5 concentrations observed in the SCAB. The major finding of this PM_2.5 emissions inventory is that the ^2ï aerosol component is more than twice the ^1ï aerosol component, which may result in widely different control strategies being required for fine PM and coarse PM.     

Conjunctive Use of Models to Design Cost-Effective Ozone Control Strategies

Abstract

The management of tropospheric ozone (O₃) is particularly difficult. The formulation of emission control strategies requires considerable information including: (1) emission inventories, (2) available control technologies, (3) meteorological data for critical design episodes, and (4) computer models that simulate atmospheric transport and chemistry. The simultaneous consideration of this information during control strategy design can be exceedingly difficult for a decision-maker. Traditional management approaches do not explicitly address cost minimization. This study presents a new approach for designing air quality management strategies; a simple air quality model is used conjunctively with a complex air quality model to obtain low-cost management strategies. A simple air quality model is used to identify potentially good solutions, and two heuristic methods are used to identify cost-effective control strategies using only a small number of simple air quality model simulations. Subsequently, the resulting strategies are verified and refined using a complex air quality model. The use of this approach may greatly reduce the number of complex air quality model runs that are required. An important component of this heuristic design framework is the use of the simple air quality model as a screening and exploratory tool. To achieve similar results with the simple and complex air quality models, it may be necessary to “tweak” or calibrate the simple model. A genetic algorithm-based optimization procedure is used to automate this tweaking process. These methods are demonstrated to be computationally practical using two realistic case studies, which are based on data from a metropolitan region in the United States.     

Locating the Offender

Abstract

The Coordinating Research Council held its thirteenth Vehicle Emissions Workshop in April 2003, when results of the most recent on-road vehicle emissions research were presented. Ongoing work from researchers who are engaged in improving understanding of the contribution of mobile sources to ambient air quality and emission inventories is summarized here. Participants in the workshop discussed efforts to improve mobile source emission models, the role of on-board diagnostic systems in inspection and maintenance programs, light- and heavy-duty vehicle emissions measurements, on- and off-road emissions measurements, effects of fuels and lubricating oils on emissions, as well as topics for future research.     

Fine Particulate Matter Emissions Inventories: Comparisons of Emissions Estimates with Observations from Recent Field Programs

Abstract

Emissions inventories of fine particulate matter (PM_2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM_2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM_2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5–20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM_2.5 are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM_2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Receptor Model Evaluation of the Southeast Michigan Ozone Study Ambient NMOC Measurements

Abstract

Large-scale studies like the Southeast Michigan Ozone Study (SEMOS) have focused attention on quantifying and spedating inventories for volatile organic compounds (VOCs). One approach for evaluating the accuracy of a VOC emission inventory is the development of a chemical mass balance (CMB) receptor model for ambient non-methane organic compound (NMOC) measurements. CMB evaluations of ambient hydrocarbon data provide a sample-specific allocation of emissions to individual source categories. This study summarizes the results of an application of the CMB model to the NMOC data from the SEMOS study. Comparison of CMB results with emission inventory values for the Detroit area show that vehicle emissions are well represented by the inventory, as are architectural coatings and coke ovens. Estimated emissions from petroleum refineries and graphic arts industries are much lower in the inventory than determined from the receptor allocation. Under-reporting of fugitive VOC emissions from petroleum refineries is an ongoing problem. Emissions from graphic arts industries are underestimated in the inventory partly because of the broad characterization of the emission factor (i.e., mass emitted/capita), which may be less useful when specific locations and days are under consideration. This study also demonstrates the effectiveness of the CMB approach when used prospectively to track the implementation of emission control strategies. While vehicle emission concentrations were unchanged from 1988 to 1993, measurement-based CMB results suggest a decrease in evaporative emissions during this time period resulting from Reid vapor pressure (RVP) reductions (from 11.0 psi in 1988 to 8.6 psi in 1993) and fleet turnover. Changes in emissions from coke plants and petroleum refineries were also seen in the CMB allocations for these sources.     

Comparison of air pollutant emissions among mega-cities

Ambient measurements of hydrocarbons, carbon monoxide and nitrogen oxides from three mega-cities (Beijing, Mexico City, Tokyo) are compared with similar measurements from US cities in the mid-1980s and the early 2000s. The common hydrocarbon pattern seen in all data sets suggests that emissions associated with gasoline-fueled vehicles dominate in all of these cities. This commonality suggests that it will be efficient and, ultimately, cost effective to proceed with vehicular emission controls in most emerging mega-cities, while proceeding with development of more locally appropriate air quality control strategies through emissions inventory development and ambient air monitoring. Over the three decades covered by the US data sets, the hydrocarbon emissions decreased by a significant factor (something like an order of magnitude), which is greater than suggested by emission inventories, particularly the EDGAR international inventory. The ambient hydrocarbon and CO concentrations reported for the three non-US mega-cities are higher than present US ambient concentrations, but lower than those observed in the 1980s in the US. The one exception to the preceding statement is the high concentrations of CO observed in Beijing, which apparently have a large regional contribution.     

On-road traffic emissions in a megacity

A new annual bottom–up emission inventory of criteria pollutants and greenhouse gases from on-road mobile sources was developed for 2006 for the metropolitan area of Buenos Aires, Argentina, within a four-year regional project aimed at providing tools for chemical weather forecast in South America. Under the scarcity of local emission factors, we collected data from measuring campaigns performed in Argentina, Brazil, Chile and Colombia and compiled a data set of regional emission factors representative of Latin American fleets and driving conditions. The estimated emissions were validated with respect to downscaled national estimates and the EDGAR global emission database. Our results highlight the role of older technologies accounting in average for almost 80% of the emissions of all species. The area exhibits higher specific emissions than developed countries, with figures two times higher for criteria pollutants. We analyzed the effect on emissions of replacing gasoline by compressed natural gas, occurring in Argentina since 1995. We identified (i) a relationship between number of vehicles and a compound socioeconomic indicator, and (ii) time-lags in vehicle technologies between developed and developing countries, which can be respectively applied for spatial disaggregation and the development of projections for other Latin American cities. The results may also be employed to complement global emission inventories and by local policy makers as an environmental management tool.     

Development of Probabilistic Emission Inventories of Air Toxics for Jacksonville,Florida

Abstract

Probabilistic emission inventories were developed for 1,3-butadiene, mercury (Hg), arsenic (As), benzene, formaldehyde, and lead for Jacksonville, FL. To quantify inter-unit variability in empirical emission factor data, the Maximum Likelihood Estimation (MLE) method or the Method of Matching Moments was used to fit parametric distributions. For data sets that contain nondetected measurements, a method based upon MLE was used for parameter estimation. To quantify the uncertainty in urban air toxic emission factors, parametric bootstrap simulation and empirical bootstrap simulation were applied to uncensored and censored data, respectively. The probabilistic emission inventories were developed based on the product of the uncertainties in the emission factors and in the activity factors. The uncertainties in the urban air toxics emission inventories range from as small as –25 to +30% for Hg to as large as –83 to +243% for As. The key sources of uncertainty in the emission inventory for each toxic are identified based upon sensitivity analysis. Typically, uncertainty in the inventory of a given pollutant can be attributed primarily to a small number of source categories. Priorities for improving the inventories and for refining the probabilistic analysis are discussed.     

Analysis of emission databases for regional models

General procedures for adapting emission inventories to regional models and for studying the impact of differences in inventories on model predictions are outlined. To illustrate the methods, analysis of two inventories which are still being validated is presented. The inventories together satisfy current requirements for the NCAR regional acid deposition model (RADM). These include anthropogenic emissions of SO₂, sulfate aerosol, NO, NO₂, NH₃ and volatile organic compounds (VOC) in 10 reactivity classes, from United States and Canadian point and area sources on 80-km grid resolutions, for weekend and weekday seasonally representative days on a diurnal basis during the 1980–1982 period. Application of checking procedures, designed by our group to screen for subtle anomalies not identified at previous stages of quality assurance employed by the inventory developers, resulted in adjustments primarily to VOC emissions. Comparisons of the modified inventories, which provide an indication of uncertainties in emissions due to variations in inventory development procedures, revealed differences in the eastern United States total daily emissions to be at most on the order of 5 % for SO_x, and NO_x, 20% for VOC and 85% for NH₃. Studies of the impact of inventory differences on predictions of RADM were conducted for the 22–24 April 1981 period, which was monitored as part of the Oxidation and Scavenging Characteristics of April Rains program. Event total wet sulfate deposition differed by 10% or less while midday O₃ concentrations differed by 1% or less for individual grids over the modeling domain.     

CAREAIR: A Computer Aided Modeling Toolbox to Generate and Analyze Emission Data in High Temporal and Spatial Resolution

ABSTRACT

For the evaluation of air quality improvement strategies, emission data in high temporal and spatial resolution is necessary, including all emission sources and all relevant pollutant species. Computer aided models are usually used to generate this emission data because it is not possible to obtain measurements from all sources, and, furthermore, a large amount of data has to be handled. For the development of emission modeling systems, a software tool called CAREAIR has been created. The intention of this paper is to introduce CAREAIR to the international community dealing with emission inventories and air quality improvement strategies.

CAREAIR is not just a single emission model but a flexible modeling toolbox. The database contains data and formulas for data manipulation, which is performed by using a set of flexible operators with different specifications. The emission calculation is carried out by combining several data manipulation operators. The CAREAIR modeling toolbox allows model implementation for the calculation of emissions from different pollutants in a high spatial and temporal resolution. The application of CAREAIR within various investigation projects in Germany, Europe, and Nigeria shows that CAREAIR is an appropriate instrument for the development of flexible emission models by meeting the various demands of these projects. The function and the data structures of this modeling toolbox are described and, towards the end of the paper, an example of an emission calculation with CAREAIR is given.     

Spatial surrogates for the disaggregation of CORINAIR emission inventories

CORINAIR atmospheric emission inventories are frequently used input data for air quality models with a domain situated in Europe. In CORINAIR emission inventories, sources are broken down over 11 major source categories. This paper presents spatial surrogates for the disaggregation of CORINAIR atmospheric emission inventories for input of air pollutants and particulate matter to grid or polygon based air quality model domains inside Europe. The basis for the disaggregation model was the CLC2000 land cover data to which statistical weights were added. Weights were population census data for residential emissions, employment statistics for agricultural and industrial area emissions, livestock statistics for ammonia emissions and annual aircraft movements for emissions realized by air transport. Additional road and off-road network information was used to disaggregate emissions realized by traffic. A comparison of top down produced emission estimates with spatially resolved national emission data for The Netherlands and the United Kingdom gave confidence in the present spatial surrogates as a tool for the top down production of atmospheric emission maps. Explained variance at a spatial resolution of 5 km was >70% for CO, NMVOC and NO_x, >60% for PM10 and almost 50% for SO₂.     

Conjunctive use of models to design cost-effective ozone control strategies

The management of tropospheric ozone (O3) is particularly difficult. The formulation of emission control strategies requires considerable information including: (1) emission inventories, (2) available control technologies, (3) meteorological data for critical design episodes, and (4) computer models that simulate atmospheric transport and chemistry. The simultaneous consideration of this information during control strategy design can be exceedingly difficult for a decision-maker. Traditional management approaches do not explicitly address cost minimization. This study presents a new approach for designing air quality management strategies; a simple air quality model is used conjunctively with a complex air quality model to obtain low-cost management strategies. A simple air quality model is used to identify potentially good solutions, and two heuristic methods are used to identify cost-effective control strategies using only a small number of simple air quality model simulations. Subsequently, the resulting strategies are verified and refined using a complex air quality model. The use of this approach may greatly reduce the number of complex air quality model runs that are required. An important component of this heuristic design framework is the use of the simple air quality model as a screening and exploratory tool. To achieve similar results with the simple and complex air     

The impact of transportation control measures on emission reductions during the 2008 Olympic Games in Beijing,China

Traffic congestion and air pollution were two major challenges for the planners of the 2008 Olympic Games in Beijing. The Beijing municipal government implemented a package of temporary transportation control measures during the event. In this paper, we report the results of a recent research project that investigated the effects of these measures on urban motor vehicle emissions in Beijing. Bottom–up methodology has been used to develop grid-based emission inventories with micro-scale vehicle activities and speed-dependent emission factors. The urban traffic emissions of volatile organic compounds (VOC), carbon monoxide (CO), nitrogen oxides (NO_x) and particulate matter with an aerodynamic diameter of 10 μm or less (PM₁₀) during the 2008 Olympics were reduced by 55.5%, 56.8%, 45.7% and 51.6%, respectively, as compared to the grid-based emission inventory before the Olympics. Emission intensity was derived from curbside air quality monitoring at the North 4th Ring Road site, located about 7 km from the National Stadium. Comparison between the emission intensity before and during the 2008 Olympics shows a reduction of 44.5% and 49.0% in daily CO and NO_x emission from motor vehicles. The results suggest that reasonable traffic system improvement strategies along with vehicle technology improvements can contribute to controlling total motor vehicle emissions in Beijing after the Olympic Games.     

Assessment of contribution of SO2 and NO2 from different sources in Jamshedpur region, India

Contribution of pollution from different types of sources in Jamshedpur, the steel city of India, has been estimated in winter 1993 using two approaches in order to delineate and prioritize air quality management strategies for the development of region in an environmental friendly manner. The first approach mainly aims at preparation of a comprehensive emission inventory and estimation of spatial distribution of pollution loads in terms of SO₂ and NO₂ from different types of industrial, domestic and vehicular sources in the region. The results indicate that industrial sources account for 77% and 68% of the total emissions of SO₂ and NO₂, respectively, in the region, whereas vehicular emissions contributed to about 28% of the total NO₂ emissions. In the second approach, contribution of these sources to ambient air quality levels to which the people are exposed to, was assessed through air pollution dispersion modelling. Ambient concentration levels of SO₂ and NO₂ have been predicted in winter season using the ISCST3 model. The analysis indicates that emissions from industrial sources are responsible for more than 50% of the total SO₂ and NO₂ concentration levels. Vehicular activities contributed to about 40% of NO₂ pollution and domestic fuel combustion contributed to about 38% of SO₂ pollution. Predicted 24-h concentrations were compared with measured concentrations at 11 ambient air monitoring stations and good agreement was noted between the two values. In-depth zone-wise analysis of the above indicates that for effective air quality management, industrial source emissions should be given highest priority, followed by vehicular and domestic sources in Jamshedpur region.