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Background: Exposure to ozone and fine particulate matter (PM2.5) can cause adverse health effects, including premature mortality due to cardiopulmonary diseases and lung cancer. Recent studies quantify global air pollution mortality but not the contribution of different emissions sectors, or they focus on a specific sector. Objectives: We estimated the global mortality burden of anthropogenic ozone and PM2.5, and the impact of five emissions sectors, using a global chemical transport model at a finer horizontal resolution (0.67° × 0.5°) than previous studies. Methods: We performed simulations for 2005 using the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4), zeroing out all anthropogenic emissions and emissions from specific sectors (All Transportation, Land Transportation, Energy, Industry, and Residential and Commercial). We estimated premature mortality using a log-linear concentration–response function for ozone and an integrated exposure–response model for PM2.5. Results: We estimated 2.23 (95% CI: 1.04, 3.33) million deaths/year related to anthropogenic PM2.5, with the highest mortality in East Asia (48%). The Residential and Commercial sector had the greatest impact globally—675 (95% CI: 428, 899) thousand deaths/year—and in most regions. Land Transportation dominated in North America (32% of total anthropogenic PM2.5 mortality), and it had nearly the same impact (24%) as Residential and Commercial (27%) in Europe. Anthropogenic ozone was associated with 493 (95% CI: 122, 989) thousand deaths/year, with the Land Transportation sector having the greatest impact globally (16%). Conclusions: The contributions of emissions sectors to ambient air pollution–related mortality differ among regions, suggesting region-specific air pollution control strategies. Global sector-specific actions targeting Land Transportation (ozone) and Residential and Commercial (PM2.5) sectors would particularly benefit human health. Citation: Silva RA, Adelman Z, Fry MM, West JJ. 2016. The impact of individual anthropogenic emissions sectors on the global burden of human mortality due to ambient air pollution. Environ Health Perspect 124:1776–1784; http://dx.doi.org/10.1289/EHP177

The impacts of aviation emissions on current and future year fine particulate matter (PM2.5) were investigated using the Community Multiscale Air Quality model, accounting for aviation emissions from 99 airports and below 3 km during landing and takeoff (LTO) cycles. Results indicated that current year aviation emissions increased annual average PM2.5 concentrations by 3.2 ng m−3 (0.05%) in the continental U.S. while projected 2025 aviation emissions increased annual average PM2.5 by 11.2 ng m−3 (0.20%). Ammonium nitrate aerosol was the largest contributor to the increase in PM2.5 concentrations, particularly in the future year. Using an indicator of inorganic PM2.5 change, we attributed ammonium nitrate aerosol contributions in both years to excess free ammonia (8% higher NH3 and 35% lower NOx emissions from non-aviation sources in 2025 than 2005), and higher aircraft emissions of NOx (which when converted to HNO3 forms ammonium nitrate aerosol) than SO2 (a precursor of ammonium sulfate aerosol). Our findings highlight the critical role that non-aviation emissions play in assessing the air quality impacts of aviation emissions in a future year scenario.

Excess wet and dry deposition of nitrogen-containing compounds is a concern at a number of national parks. The Rocky Mountain Atmospheric Nitrogen and Sulfur Study (RoMANS) was conducted during the spring and summer of 2006 to identify the overall mix of ambient and deposited sulfur and nitrogen at Rocky Mountain National Park (RMNP), in north-central Colorado. The Comprehensive Air Quality Model with extensions (CAMx) was used to simulate the fate of gaseous and particulate species subjected to multiple chemical and physical processes during RoMANS. This study presents an operational evaluation with a special emphasis on the model performance of reduced nitrogen species. The evaluation showed large negative biases and errors at RMNP and the entire domain for ammonia; therefore the model was considered inadequate for future source apportionment applications. The CAMx Integrated Processes Rate (IPR) analysis tool was used to elucidate the potential causes behind the poor model performance. IPR served as a tool to diagnose the relative contributions of individual physical and chemical processes to the final concentrations of reduced nitrogen species. The IPR analysis revealed that dry deposition is the largest sink of ammonia in the model, with some cells losing almost 100% of the available mass. Closer examination of the ammonia dry deposition velocities in CAMx found that they were up to a factor of 10 larger than those reported in the literature. A series of sensitivity simulations were then performed by changing the original deposition velocities with a simple multiplicative scaling factor. These simulations showed that even when the dry deposition values were altered to reduce their influence, the model was still unable to replicate the observed time series; i.e., it fixed the average bias, but it did not improve the precision.

A prototype online photolysis module has been developed for the Community Multiscale Air Quality (CMAQ) modeling system. The module calculates actinic fluxes and photolysis rates (j values) at every vertical level in each of seven wavelength intervals from 291 to 850 nm, as well as the total surface irradiance and aerosol optical depth within each interval. The module incorporates updated opacity at each time step, based on changes in local ozone, nitrogen dioxide, and particle concentrations. The module is computationally efficient and requires less than 5% more central processing unit time than using the existing CMAQ “lookup” table method for calculating j values. The main focus of the work presented here is to describe the new online module as well as to highlight the differences between the effective cross sections from the lookup-table method currently being used and the updated effective cross sections from the new online approach. Comparisons of the vertical profiles for the photolysis rates for nitrogen dioxide (NO2) and ozone (O3) from the new online module with those using the effective cross sections from a standard CMAQ simulation show increases in the rates of both NO2 and O3 photolysis.

Non-methane volatile organic compounds (NMVOCs) influence air quality and global climate change through their effects on secondary air pollutants and climate forcers. Here we simulate the air quality and radiative forcing (RF) impacts of changes in ozone, methane, and sulfate from halving anthropogenic NMVOC emissions globally and from 10 regions individually, using a global chemical transport model and a standalone radiative transfer model. Halving global NMVOC emissions decreases global annual average tropospheric methane and ozone by 36.6 ppbv and 3.3 Tg, respectively, and surface ozone by 0.67 ppbv. All regional reductions slow the production of peroxyacetyl nitrate (PAN), resulting in regional to intercontinental PAN decreases and regional NOx increases. These NOx increases drive tropospheric ozone increases nearby or downwind of source regions in the Southern Hemisphere (South America, Southeast Asia, Africa, and Australia). Some regions' NMVOC emissions contribute importantly to air pollution in other regions, such as East Asia, the Middle East, and Europe, whose impact on US surface ozone is 43%, 34%, and 34% of North America's impact. Global and regional NMVOC reductions produce widespread negative net RFs (cooling) across both hemispheres from tropospheric ozone and methane decreases, and regional warming and cooling from changes in tropospheric ozone and sulfate (via several oxidation pathways). The 100 yr and 20 yr global warming potentials (GWP100, GWP20) are 2.36 and 5.83 for the global reduction, and 0.079 to 6.05 and −1.13 to 18.9 among the 10 regions. The NMVOC RF and GWP estimates are generally lower than previously modeled estimates, due to the greater NMVOC/NOx emissions ratios simulated, which result in less sensitivity to NMVOC emissions changes and smaller global O3 burden responses, in addition to differences in the representation of NMVOCs and oxidation chemistry among models. Accounting for a fuller set of RF contributions may change the relative magnitude of each region's impacts. The large variability in the RF and GWP of NMVOCs among regions suggest that regionally specific metrics may be necessary to include NMVOCs in multi-gas climate trading schemes.

Carbon monoxide (CO) emissions influence global and regional air quality and global climate change by affecting atmospheric oxidants and secondary species. We simulate the influence of halving anthropogenic CO emissions globally and individually from 10 regions on surface and tropospheric ozone, methane, and aerosol concentrations using a global chemical transport model (MOZART-4 for the year 2005). Net radiative forcing (RF) is then estimated using the GFDL (Geophysical Fluid Dynamics Laboratory) standalone radiative transfer model. We estimate that halving global CO emissions decreases global annual average concentrations of surface ozone by 0.45 ppbv, tropospheric methane by 73 ppbv, and global annual net RF by 36.1 mW m−2, nearly equal to the sum of changes from the 10 regional reductions. Global annual net RF per unit change in emissions and the 100 yr global warming potential (GWP100) are estimated as −0.124 mW m−2 (Tg CO)−1 and 1.34, respectively, for the global CO reduction, and ranging from −0.115 to −0.131 mW m−2 (Tg CO)−1 and 1.26 to 1.44 across 10 regions, with the greatest sensitivities for regions in the tropics. The net RF distributions show widespread cooling corresponding to the O3 and CH4 decreases, and localized positive and negative net RFs due to changes in aerosols. The strongest annual net RF impacts occur within the tropics (28° S–28° N) followed by the northern midlatitudes (28° N–60° N), independent of reduction region, while the greatest changes in surface CO and ozone concentrations occur within the reduction region. Some regional reductions strongly influence the air quality in other regions, such as East Asia, which has an impact on US surface ozone that is 93% of that from North America. Changes in the transport of CO and downwind ozone production clearly exceed the direct export of ozone from each reduction region. The small variation in CO GWPs among world regions suggests that future international climate agreements could adopt a globally uniform metric for CO with little error, or could use different GWPs for each continent. Doing so may increase the incentive to reduce CO through coordinated policies addressing climate and air quality.