Opportunities and Challenges for Filling the Air Quality Data Gap in Low- and Middle-Income Countries.

Given the millions of people suffering from air pollution, filling the air quality monitoring gap in low- and middle-income countries has been recognized as a global challenge. To meet this challenge and make it work will require private enterprise, multiple levels of government, international organizations, academia and civil society to work together toward the common goal of characterizing, understanding better, and then reducing, the air pollution that causes sickness and preventable death for millions of people each year in lowand middle-income countries around the world. This article offers concrete next steps on how to make progress toward increasing air quality monitoring using a combination of emerging technologies, adaptation to country-specific conditions, and building capacity towards the development of lasting institutions.

Climate change impacts of US reactive nitrogen.

Fossil fuel combustion and fertilizer application in the United States have substantially altered the nitrogen cycle, with serious effects on climate change. The climate effects can be short-lived, by impacting the chemistry of the atmosphere, or long-lived, by altering ecosystem greenhouse gas fluxes. Here we develop a coherent framework for assessing the climate change impacts of US reactive nitrogen emissions, including oxides of nitrogen, ammonia, and nitrous oxide (N(2)O). We use the global temperature potential (GTP), calculated at 20 and 100 y, in units of CO(2) equivalents (CO(2)e), as a common metric. The largest cooling effects are due to combustion sources of oxides of nitrogen altering tropospheric ozone and methane concentrations and enhancing carbon sequestration in forests. The combined cooling effects are estimated at -290 to -510 Tg CO(2)e on a GTP(20) basis. However, these effects are largely short-lived. On a GTP(100) basis, combustion contributes just -16 to -95 Tg CO(2)e. Agriculture contributes to warming on both the 20-y and 100-y timescales, primarily through N(2)O emissions from soils. Under current conditions, these warming and cooling effects partially offset each other. However, recent trends show decreasing emissions from combustion sources. To prevent warming from US reactive nitrogen, reductions in agricultural N(2)O emissions are needed. Substantial progress toward this goal is possible using current technology. Without such actions, even greater CO(2) emission reductions will be required to avoid dangerous climate change.

GLIMPSE: a rapid decision framework for energy and environmental policy.

Over the coming decades, new energy production technologies and the policies that oversee them will affect human health, the vitality of our ecosystems, and the stability of the global climate. The GLIMPSE decision model framework provides insights about the implications of technology and policy decisions on these outcomes. Using GLIMPSE, decision makers can identify alternative techno-policy futures, examining their air quality, health, and short- and long-term climate impacts. Ultimately, GLIMPSE will support the identification of cost-effective strategies for simultaneously achieving performance goals for these metrics. Here, we demonstrate the utility of GLIMPSE by analyzing several future energy scenarios under existing air quality regulations and potential CO2 emission reduction policies. We find opportunities for substantial cobenefits in setting both climate change mitigation and health-benefit based air quality improvement targets. Though current policies which prioritize public health protection increase near-term warming, establishing policies that also reduce greenhouse gas emissions may offset warming in the near-term and lead to significant reductions in long-term warming.

Epoxide pathways improve model predictions of isoprene markers and reveal key role of acidity in aerosol formation.

Isoprene significantly contributes to organic aerosol in the southeastern United States where biogenic hydrocarbons mix with anthropogenic emissions. In this work, the Community Multiscale Air Quality model is updated to predict isoprene aerosol from epoxides produced under both high- and low-NOx conditions. The new aqueous aerosol pathways allow for explicit predictions of two key isoprene-derived species, 2-methyltetrols and 2-methylglyceric acid, that are more consistent with observations than estimates based on semivolatile partitioning. The new mechanism represents a significant source of organic carbon in the lower 2 km of the atmosphere and captures the abundance of 2-methyltetrols relative to organosulfates during the simulation period. For the parametrization considered here, a 25% reduction in SOx emissions effectively reduces isoprene aerosol, while a similar reduction in NOx leads to small increases in isoprene aerosol.

Spatially refined aerosol direct radiative forcing efficiencies.

Global aerosol direct radiative forcing (DRF) is an important metric for assessing potential climate impacts of future emissions changes. However, the radiative consequences of emissions perturbations are not readily quantified nor well understood at the level of detail necessary to assess realistic policy options. To address this challenge, here we show how adjoint model sensitivities can be used to provide highly spatially resolved estimates of the DRF from emissions of black carbon (BC), primary organic carbon (OC), sulfur dioxide (SO(2)), and ammonia (NH(3)), using the example of emissions from each sector and country following multiple Representative Concentration Pathway (RCPs). The radiative forcing efficiencies of many individual emissions are found to differ considerably from regional or sectoral averages for NH(3), SO(2) from the power sector, and BC from domestic, industrial, transportation and biomass burning sources. Consequently, the amount of emissions controls required to attain a specific DRF varies at intracontinental scales by up to a factor of 4. These results thus demonstrate both a need and means for incorporating spatially refined aerosol DRF into analysis of future emissions scenario and design of air quality and climate change mitigation policies.

Model representation of secondary organic aerosol in CMAQv4.7.

Numerous scientific upgrades to the representation of secondary organic aerosol (SOA) are incorporated into the Community Multiscale Air Quality (CMAQ) modeling system. Additions include several recently identified SOA precursors: benzene, isoprene, and sesquiterpenes; and pathways: in-cloud oxidation of glyoxal and methylglyoxal, particle-phase oligomerization, and acid enhancement of isoprene SOA. NO(x)-dependent aromatic SOA yields are also added along with new empirical measurements of the enthalpies of vaporization and organic mass-to-carbon ratios. For the first time, these SOA precursors, pathways and empirical parameters are included simultaneously in an air quality model for an annual simulation spanning the continental U.S. Comparisons of CMAQ-modeled secondary organic carbon (OC(sec)) with semiempirical estimates screened from 165 routine monitoring sites across the U.S. indicate the new SOA module substantially improves model performance. The most notable improvement occurs in the central and southeastern U.S. where the regionally averaged temporal correlations (r) between modeled and semiempirical OC(sec) increase from 0.5 to 0.8 and 0.3 to 0.8, respectively, when the new SOA module is employed. Wintertime OC(sec) results improve in all regions of the continental U.S. and the seasonal and regional patterns of biogenic SOA are better represented.

Analysis of coupled model uncertainties in source-to-dose modeling of human exposures to ambient air pollution: A PM(2.5) case study.

Quantitative assessment of human exposures and health effects due to air pollution involve detailed characterization of impacts of air quality on exposure and dose. A key challenge is to integrate these three components on a consistent spatial and temporal basis taking into account linkages and feedbacks. The current state-of-practice for such assessments is to exercise emission, meteorology, air quality, exposure, and dose models separately, and to link them together by using the output of one model as input to the subsequent downstream model. Quantification of variability and uncertainty has been an important topic in the exposure assessment community for a number of years. Variability refers to differences in the value of a quantity (e.g., exposure) over time, space, or among individuals. Uncertainty refers to lack of knowledge regarding the true value of a quantity. An emerging challenge is how to quantify variability and uncertainty in integrated assessments over the source-to-dose continuum by considering contributions from individual as well as linked components. For a case study of fine particulate matter (PM(2.5)) in North Carolina during July 2002, we characterize variability and uncertainty associated with each of the individual concentration, exposure and dose models that are linked, and use a conceptual framework to quantify and evaluate the implications of coupled model uncertainties. We find that the resulting overall uncertainties due to combined effects of both variability and uncertainty are smaller (usually by a factor of 3-4) than the crudely multiplied model-specific overall uncertainty ratios. Future research will need to examine the impact of potential dependencies among the model components by conducting a truly coupled modeling analysis.

Towards a climate-dependent paradigm of ammonia emission and deposition.

Existing descriptions of bi-directional ammonia (NH3) land-atmosphere exchange incorporate temperature and moisture controls, and are beginning to be used in regional chemical transport models. However, such models have typically applied simpler emission factors to upscale the main NH3 emission terms. While this approach has successfully simulated the main spatial patterns on local to global scales, it fails to address the environment- and climate-dependence of emissions. To handle these issues, we outline the basis for a new modelling paradigm where both NH3 emissions and deposition are calculated online according to diurnal, seasonal and spatial differences in meteorology. We show how measurements reveal a strong, but complex pattern of climatic dependence, which is increasingly being characterized using ground-based NH3 monitoring and satellite observations, while advances in process-based modelling are illustrated for agricultural and natural sources, including a global application for seabird colonies. A future architecture for NH3 emission-deposition modelling is proposed that integrates the spatio-temporal interactions, and provides the necessary foundation to assess the consequences of climate change. Based on available measurements, a first empirical estimate suggests that 5°C warming would increase emissions by 42 per cent (28-67%). Together with increased anthropogenic activity, global NH3 emissions may increase from 65 (45-85) Tg N in 2008 to reach 132 (89-179) Tg by 2100.

Trends in atmospheric reactive nitrogen for the Eastern United States.

Reactive nitrogen can travel far from emission sources and impact sensitive ecosystems. From 2002 to 2006, policy actions have led to decreases in NO(x) emissions from power plants and motor vehicles. In this study, atmospheric chemical transport modeling demonstrates that these emissions reductions have led to a downward trend in ambient measurements of transported reactive nitrogen, especially atmospheric concentrations and wet deposition of nitrate. The trend in reduced nitrogen, namely ammonium, is ambiguous. As reduced nitrogen becomes a larger fraction of the reactive nitrogen budget, wide-spread NH(3) measurements and improved NH(3) emissions assessments are a critical need.

To what extent can biogenic SOA be controlled?

The implicit assumption that biogenic secondary organic aerosol (SOA) is natural and can not be controlled hinders effective air quality management. Anthropogenic pollution facilitates transformation of naturally emitted volatile organic compounds (VOCs) to the particle phase, enhancing the ambient concentrations of biogenic secondary organic aerosol (SOA). It is therefore conceivable that some portion of ambient biogenic SOA can be removed by controlling emissions of anthropogenic pollutants. Direct measurement of the controllable fraction of biogenic SOA is not possible, but can be estimated through 3-dimensional photochemical air quality modeling. To examine this in detail, 22 CMAQ model simulations were conducted over the continental U.S. (August 15 to September 4, 2003). The relative contributions of five emitted pollution classes (i.e., NO(x), NH(3), SO(x), reactive non methane carbon (RNMC) and primary carbonaceous particulate matter (PCM)) on biogenic SOA were estimated by removing anthropogenic emissions of these pollutants, one at a time and all together. Model results demonstrate a strong influence of anthropogenic emissions on predicted biogenic SOA concentrations, suggesting more than 50% of biogenic SOA in the eastern U.S. can be controlled. Because biogenic SOA is substantially enhanced by controllable emissions, classification of SOA as biogenic or anthropogenic based solely on VOC origin is not sufficient to describe the controllable fraction.

Efficient probabilistic estimates of surface ozone concentration using an ensemble of model configurations and direct sensitivity calculations.

Because all models are a simplification of the phenomenon they aim to represent, it is often more useful to estimate the probability of an event rather than a single "best" model result. Previous air quality ensemble approaches have used computationally expensive simulations of separately developed modeling systems. We present an efficient method to generate ensembles with hundreds of members based on several structural configurations of a single air quality modeling system. We use the Decoupled Direct Method in three dimensions to directly calculate how ozone concentrations change as a result of changes in input parameters. The modeled probability estimate is compared to observations and is shown to have a high level of skill and improved resolution and sharpness. This approach can help resolve the practical limits of incorporating uncertainty estimation into deterministic air quality management modeling applications.

Ammonia emission controls as a cost-effective strategy for reducing atmospheric particulate matter in the Eastern United States.

Current regulation aimed at reducing inorganic atmospheric fine particulate matter (PM2.5) is focused on reductions in sulfur dioxide (SO2) and oxides of nitrogen (NO(x) = NO + NO2); however, controls on these pollutants are likely to increase in cost and decrease in effectiveness in the future. A supplementary strategy is reduction in ammonia (NH3) emissions, yet an evaluation of controls on ammonia has been limited by uncertainties in emission levels and in the cost of control technologies. We use state of the science emission inventories, an emission-based regional air quality model, and an explicit treatment of uncertainty to estimate the cost-effectiveness and uncertainty of ammonia emission reductions on inorganic particulate matter in the Eastern United States. Since a paucity of data on agricultural operations precludes a direct calculation of the costs of ammonia control, we calculate the "ammonia savings potential", defined as the minimum cost of applying SO2 and NO(x) emission controls in order to achieve the same reduction in ambient inorganic PM2.5 concentration as obtained from a 1 ton decrease in ammonia emissions. Using 250 scenarios of NH3, SO2, and NO(x) emission reductions, we calculate the least-cost SO2 and NO(x) control scenarios that achieve the same reduction in ambient inorganic PM2.5 concentration as a decrease in ammonia emissions. We find that the lower-bound ammonia savings potential in the winter is $8,000 per ton NH3; therefore, many currently available ammonia control technologies are cost-effective compared to current controls on SO2 and NO(x) sources. Larger reductions in winter inorganic particulate matter are available at lower cost through controls on ammonia emissions.