Development of probabilistic emission inventories of air toxics for Jacksonville, Florida, USA

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.     

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.     

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.     

Air Emission Inventories in North America: A Critical Assessment

Abstract

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.     

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.     

Spatiotemporal analysis of traffic emissions in over 5000 municipal districts in Brazil

Exposure to traffic emission is harmful to human health. Emission inventories are essential to public health policies aiming at protecting human health, especially in areas with incomplete or nonexistent air pollution monitoring networks. In Brazil, for example, only 1.7% of municipal districts have a monitoring network, and only a few studies have reported data on vehicle emission inventories. No studies have presented emission inventories by municipality. In this study, we predicted vehicular emissions for 5570 municipal districts in Brazil during the period 2001–2012. We used a top-down method to estimate emissions. Carbon dioxide (CO₂) is the pollutant with the highest emissions, with approximately 190 million tons per year during the period 2001–2012). For the other traffic-related pollutants, we predicted annual emissions of 1.5 million tons for carbon monoxide (CO), 1.2 million tons of nitrogen oxides (NO_x), 209,000 tons of nonmethane hydrocarbons (NMHC), 58,000 tons of particulate matter (PM), and 42,000 tons for methane (CH₄). From 2001 to 2012, CO, NMHC, and PM emissions decreased by 41, 33, and 47%, respectively, whereas those CH₄, NO_x, and CO₂ increased by 2, 4, and 84%, respectively. We estimated uncertainties in our study and found that NO_x was the pollutant with the lowest percentage difference, 8%, and NMHC with the highest one, 30%. For CO, CH₄, CO₂, and PM, the values were 22, 14, 21, and 20%, respectively. Finally, we found that during 2001 and 2012 emissions increased in the Northwest and Northeast. In contrast, pollutant emissions, except for CO₂, decreased in the Southeast, South, and part of Midwest. Our predictions can be critical to efforts developing cost-effective public policies tailored to individual municipal districts in Brazil.

Implications: Emission inventories may be an alternative approach to provide data for air quality forecasting in areas where air quality data are not available. This approach can be an effective tool in developing spatially resolved emission inventories.     

Real-world vehicle emissions: a summary of the 14th coordinating research council on-road Vehicle Emissions Workshop

The Coordinating Research Council held its 14th Vehicle Emissions Workshop in March 2004, where results of the most recent on-road vehicle emissions research were presented. We summarize ongoing work from researchers who are 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, 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.     

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

The Coordinating Research Council, Inc. (CRC) held its 17th On-Road Vehicle Emissions Workshop in March 2007, where results of the most recent on-road vehicle emissions research were presented. We summarize ongoing work from researchers who are engaged in improving our understanding of the role and contribution of mobile sources to ambient air quality and emission inventories. Participants in the Workshop discussed efforts to improve mobile source emission models, light- and heavy-duty vehicle emissions measurements, on- and off-road emissions measurements, effects of fuels and lubricating oils on emissions, as well as emerging issues and topics for future research.     

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

The Coordinating Research Council held its 16th workshop in March 2006, with 83 presentations describing the most recent mobile source-related emissions research. In this paper, we summarize the presentations from researchers who are engaged in improving our understanding of the contribution of mobile sources to air quality. Participants in the workshop discussed evaluation of in-use emissions control programs, effects of fuels on emissions, emission models and emission inventories, results from gas- and particle-phase emissions studies from spark-ignition and diesel-powered vehicles, and efforts to improve our capabilities in performing on-board emissions measurements, as well as topics for future research.     

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

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.     

Endosulfan in China 2—emissions and residues

Background, aim, and scope  Endosulfan is one of the organochlorine pesticides (OCPs) and also a candidate to be included in a group of new persistent organic pollutants (UNEP 2007). The first national endosulfan usage inventories in China with 1/4° longitude by 1/6° latitude resolution has been reported in an accompanying paper. In the second part of the paper, we compiled the gridded historical emissions and soil residues of endosulfan in China from the usage inventories. Based on the residue/emission data, gridded concentrations of endosulfan in Chinese soil and air have been calculated. These inventories will provide valuable data for the further study of endosulfan. Methods  Emission and residue of endosulfan were calculated from endosulfan usage by using a simplified gridded pesticide emission and residue model—SGPERM, which is an integrated modeling system combining mathematical model, database management system, and geographic information system. By using the emission and residue inventories, annual air and soil concentrations of endosulfan in each cell were determined. Results and discussion  Historical gridded emission and residue inventories of α- and β-endosulfan in agricultural soil in China with 1/4° longitude by 1/6° latitude resolution have been created. Total emissions were around 10,800 t, with α-endosulfan at 7,400 t and β-endosulfan at 3,400 t from 1994 to 2004. The highest residues were 140 t for α-endosulfan and 390 t for β-endosulfan, and the lowest residues were 0.7 t for α-endosulfan and 170 t for β-endosulfan in 2004 in Chinese agricultural soil where endosulfan was applied. Based on the emission and residue inventories, concentrations of α- and β-endosulfan in Chinese air and agricultural surface soil were also calculated for each grid cell. We have estimated annual averaged air concentrations and the annual minimum and maximum soil concentrations across China. The real concentrations will be different from season to season. Although our model does not consider the transport of the insecticide in the atmosphere, which could be very important in some areas during some special time, the estimated concentrations of endosulfan in Chinese air and soil derived from the endosulfan emission and residue inventories are in general consistent with the published monitoring data. Conclusions  To our knowledge, this work is the first inventory of this kind for endosulfan published on a national scale. Concentrations of the chemical in Chinese air and agricultural surface soil were calculated for each grid cell. Results show that the estimated concentrations of endosulfan in Chinese air and soil agree reasonably well with the monitoring data in general. Recommendations and perspectives  The gridded endosulfan emission/residue inventories and also the air and soil concentration inventories created in this study will be updated upon availability of new information, including usage and monitoring data. The establishment of these inventories for the OCP is important for both scientific communities and policy makers.     

A socio-economic method for estimating future air pollutant emissions—Chicago case study

This paper presents the development of an econometric-emission model to formulate future anthropogenic emission inventories for different societal and climate change scenarios. Our approach is to formulate the emission projections for a given scenario into growth factors that can be used to project forward the 1999 National Emission Inventory (NEI99). The process involves (1) mapping NEI99 source classification code (SCC)-based emissions into the sector or standard industrial classification (SIC)-based representation used by the econometric model, (2) developing a sectoral emission intensity (EMI) defined as the sector emissions per unit of sector economic output and the mechanism to consider EMI variations over time, (3) using the resulting EMI with econometric models and future emission activities to project future emissions, (4) and then mapping the emissions back to the original NEI99 format. As a case study, we apply the model to project emissions in the Chicago metropolitan area. The results show that the model is a fast, flexible, yet reasonable tool to produce a wide range of emission scenarios that are specific to regions, and would prove valuable for future air quality and other impact studies.     

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.     

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.     

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

The Coordinating Research Council (CRC) held its 12th workshop in April 2002, with nearly 90 presentations on the most recent on-road vehicle emissions research. This paper summarizes the presentations from researchers who are engaged in improving understanding of the contribution of mobile sources to air quality. Participants in the workshop discussed mobile source emission models and emission inventories, results from gas- and particle-phase emissions studies from spark-ignition and diesel-powered vehicles (with an emphasis in this workshop on particle emissions), effects of fuels on emissions, evaluation of in-use emissions control programs, and efforts to improve our capabilities in performing on-board emissions measurements, as well as topics for future research.     

Real-world vehicle emissions: A summary of the 15th coordinating research council on-road vehicle emissions workshop

The Coordinating Research Council held its 15th workshop in April 2005, with nearly 90 presentations describing the most recent mobile source-related emissions research. In this paper, the authors summarize the presentations from researchers who are engaged in improving our understanding of the contribution of mobile sources to air quality. Participants in the workshop discussed emission models and emission inventories, results from gas- and particle-phase emissions studies from spark-ignition and diesel-powered vehicles (with an emphasis in this workshop on particle emissions), effects of fuels on emissions, evaluation of in-use emissions control programs, and efforts to improve our capabilities in performing on-board emissions measurements, as well as topics for future research.     

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.     

Survey of dioxin sources in the Baltic Region (extended summary)

The present paper summarises the results of the project: 'Survey of Anthropogenic Sources of Dioxins and Furans in the Baltic Region'. As a part of the project, inventories have been carried out in Estonia, Latvia, Lithuania and Poland by applying the toolkit for quantification of dioxin and furan releases developed by UNEP Chemicals. The main route of direct releases to the environment is emission to air. Total emission to air from Poland was estimated at 490 (88-1,300) g I-TEQ/year, whereas the emissions from Estonia, Latvia and Lithuania were estimated as being 14 (2.4-54), 23 (2.6-63) and 17 (2.6-38) g I-TEQ, respectively. In general, the uncertainty on the estimates is very high, and recommendations regarding further development of the inventories have been made, and measures for reducing the releases have been provided.