Air pollution is one of the top five risk factors for population health globally. In recent years, advances in air pollution data and modeling have occurred simultaneously with advances in data and methods available for health studies. To realize the potential of such advances, the air quality modeling and public health communities should continue to strengthen their engagements and build effective interdisciplinary teams. These partnerships recognize the tight coupling between air quality and health data and methods and the value of expertise from multiple fields to ensure that this information is applied appropriately with a deep understanding of its capabilities and limitations. Building effective multidisciplinary teams takes a sustained commitment to engage with partners with different expertise to establish working partnerships and collaborations to better address public exposures to air pollution. Effective partnerships enable better targeting of research resources to answer important questions and provide essential information to protect public health.Implications: Air quality models are an effective tool that can be used to estimate air pollution exposure in epidemiologic studies and risk assessments. Working together in collaborative multidisciplinary teams will lead to greater advancements in understanding of air pollution impacts and in useful information informing actions to improve public health.
Abstract Atmospheric transformations determine the contribution of emissions from combustion systems to fine particulate matter (PM) mass. For example, combustion systems emit vapors that condense onto existing particles or form new particles as the emissions are cooled and diluted. Upon entering the atmosphere, emissions are exposed to atmospheric oxidants and sunlight, which causes them to evolve chemically and physically, generating secondary PM. This review discusses these transformations, focusing on organic PM. Organic PM emissions are semi -volatile at atmospheric conditions and thus their partitioning varies continuously with changing temperature and concentration. Because organics contribute a large portion of the PM mass emitted by most combustion sources, these emissions cannot be represented using a traditional, static emission factor. Instead, knowledge of the volatility distribution of emissions is required to explicitly account for changes in gas-particle partitioning. This requires updating how PM emissions from combustion systems are measured and simulated from combustion systems. Secondary PM production often greatly exceeds the direct or primary PM emissions; therefore, secondary PM must be included in any assessment of the contribution of combustion systems to ambient PM concentrations. Low-volatility organic vapors emitted by combustion systems appear to be very important secondary PM precursors that are poorly accounted for in inventories and models. The review concludes by discussing the implications that the dynamic nature of these PM emissions have on source testing for emission inventory development and regulatory purposes. This discussion highlights important linkages between primary and secondary PM, which could lead to simplified certification test procedures while capturing the emission components that contribute most to atmospheric PM mass.
In response to recommendations by the National Research Council in the late 1990 s and early 2000s for critical research into understanding sources and formation mechanisms of PM2.5, EPA created multiple funding opportunities through the Science to Achieve Results (STAR) program: "Measurement, Modeling, and Analysis Methods for Airborne Carbonaceous Fine Particulate Matter" (2003) and "Source Apportionment of Particulate Matter" (2004). The carbonaceous fine PM solicitation resulted in 16 different projects focusing on the measurement methods, source identification, and exploration of the chemical and physical processes important for PM2.5 carbon in the atmosphere. The source apportionment funding opportunity led to 11 projects improving tools and characterization of source-receptor relationships of PM2.5. Many funding mechanisms include a final synopsis of funded research and published manuscripts. Here, this evaluation is extended to include citations of research published as part of these solicitations. These solicitations resulted in 275 publications that included more than 850 unique authors in 37 different journals with a weighted average 2011 impact factor of 4.21. At the time of this assessment, these publications have been cited by 13,612 peer review journal articles with 31 (11%) of the manuscripts being cited over 100 times.
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.
This paper provides a synthesis of results that have emerged from recent modeling studies of the potential sensitivity of U.S. regional ozone (O3) concentrations to global climate change (ca. 2050). This research has been carried out under the auspices of an ongoing U.S. Environmental Protection Agency (EPA) assessment effort to increase scientific understanding of the multiple complex interactions among climate, emissions, atmospheric chemistry, and air quality. The ultimate goal is to enhance the ability of air quality managers to consider global change in their decisions through improved characterization of the potential effects of global change on air quality, including O3 The results discussed here are interim, representing the first phase of the EPA assessment. The aim in this first phase was to consider the effects of climate change alone on air quality, without accompanying changes in anthropogenic emissions of precursor pollutants. Across all of the modeling experiments carried out by the different groups, simulated global climate change causes increases of a few to several parts per billion (ppb) in summertime mean maximum daily 8-h average O3 concentrations over substantial regions of the country. The different modeling experiments in general do not, however, simulate the same regional patterns of change. These differences seem to result largely from variations in the simulated patterns of changes in key meteorological drivers, such as temperature and surface insolation. How isoprene nitrate chemistry is represented in the different modeling systems is an additional critical factor in the simulated O3 response to climate change.
Models that accurately predict atmospheric composition and correctly respond to tested policy scenarios aid air quality managers in the development of effective strategies to protect human health. Controllable emissions from human activity interact with natural emissions from plants and trees from the biosphere through complex chemistry to form ozone (O3) and organic fine particulate matter (PM2.5), criteria air pollutants that induce a variety of adverse health effects. While organic gases emitted from plants and trees are natural, some fraction of the subsequent O3 and PM2.5 is not. Accurate assessment of the extent to which human activity and natural emissions interact to form pollution can be achieved when models are constructed from first principle chemical and physical laws, and tested and evaluated with laboratory and field observations. In the summer of 2013, hundreds of scientists descended on the southeast U.S. to coordinate an atmospheric chemistry campaign with the ultimate goal of understanding complex biosphere-atmosphere interactions, the subsequent formation of O3 and PM2.5, and accurate incorporation of the chemistry into atmospheric models. A main finding from the campaign is that anthropogenic emissions facilitate formation of organic PM2.5 derived from biogenic VOCs. This fraction of PM2.5 is controllable pollution. Mechanistic insight from that campaign was recently incorporated into EPA's air quality model, improving the model representation of the atmospheric modeling and informing air quality management strategies for PM2.5. Emission reductions in SO2 and NOx in the southeast U.S. are found to reduce non-fossil, presumably biogenic, organic PM2.5 mass concentrations, suggesting existing Federal rules have been more successful than anticipated. Additional potential feedback mechanisms may become important as emissions reductions bring the atmosphere into new chemical regimes.
The reaction of ozone with aqueous sodium bromide particles is investigated with a combination of aerosol chamber experiments, kinetics modeling, and molecular dynamics simulations. The molecular bromine production in the chamber experiments is approximately an order of magnitude greater than that predicted by known chemistry in the gas and bulk aqueous phases with use of a comprehensive computer kinetics model. Molecular dynamics simulations indicate that ozone has significant residence time at the air−solution interface, while making frequent contacts with bromide ions for as long as 50 ps in the surface layer of a 6.1 M NaBr solution. The formation of a complex between ozone and bromide ion, [O3···Br-], which can lead to production of Br2 by reaction at the air−water interface, is therefore feasible. Experimentally observed Br2 is well predicted by including an interface process with a reaction probability of [1.9 ± 0.8] × 10-6 (1 s) as the first step in a surface mechanism to produce additional gas-phase Br2. An estimate of the impact of this interface reaction on bromine formation in the marine boundary layer shows that several ppt of bromine could potentially be produced during the night from this proposed surface chemistry.
Despite the challenges in linking global and regional processes, evidence from recent studies suggests that the effects of a changing climate should not be neglected when planning for the future attainment of regional-scale ozone standards such as the U.S. NAAQS. Research underway should provide insight regarding the impact of climate change on Ozone and PM2.5 and of the complex interaction of climate, land-use, and technology change.
Abstract The Southeast Atmosphere Studies (SAS), which included the Southern Oxidant and Aerosol Study (SOAS); the Southeast Nexus (SENEX) study; and the Nitrogen, Oxidants, Mercury and Aerosols: Distributions, Sources and Sinks (NOMADSS) study, was deployed in the field from 1 June to 15 July 2013 in the central and eastern United States, and it overlapped with and was complemented by the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. SAS investigated atmospheric chemistry and the associated air quality and climate-relevant particle properties. Coordinated measurements from six ground sites, four aircraft, tall towers, balloon-borne sondes, existing surface networks, and satellites provide in situ and remotely sensed data on trace-gas composition, aerosol physicochemical properties, and local and synoptic meteorology. Selected SAS findings indicate 1) dramatically reduced NOx concentrations have altered ozone production regimes; 2) indicators of “biogenic” secondary organic aerosol (SOA), once considered part of the natural background, were positively correlated with one or more indicators of anthropogenic pollution; and 3) liquid water dramatically impacted particle scattering while biogenic SOA did not. SAS findings suggest that atmosphere–biosphere interactions modulate ambient pollutant concentrations through complex mechanisms and feedbacks not yet adequately captured in atmospheric models. The SAS dataset, now publicly available, is a powerful constraint to develop predictive capability that enhances model representation of the response and subsequent impacts of changes in atmospheric composition to changes in emissions, chemistry, and meteorology.
