Tripling of western US particulate pollution from wildfires in a warming climate.

SignificanceRecord-setting fires in the western United States over the last decade caused severe air pollution, loss of human life, and property damage. Enhanced drought and increased biomass in a warmer climate may fuel larger and more frequent wildfires in the coming decades. Applying an empirical statistical model to fires projected by Earth System Models including climate-ecosystem-socioeconomic interactions, we show that fine particulate pollution over the US Pacific Northwest could double to triple during late summer to fall by the late 21st century under intermediate- and low-mitigation scenarios. The historic fires and resulting pollution extremes of 2017-2020 could occur every 3 to 5 y under 21st-century climate change, posing challenges for air quality management and threatening public health.

Large uncertainties in global hydroxyl projections tied to fate of reactive nitrogen and carbon.

The hydroxyl radical (OH) sets the oxidative capacity of the atmosphere and, thus, profoundly affects the removal rate of pollutants and reactive greenhouse gases. While observationally derived constraints exist for global annual mean present-day OH abundances and interannual variability, OH estimates for past and future periods rely primarily on global atmospheric chemistry models. These models disagree ± 30% in mean OH and in its changes from the preindustrial to late 21st century, even when forced with identical anthropogenic emissions. A simple steady-state relationship that accounts for ozone photolysis frequencies, water vapor, and the ratio of reactive nitrogen to carbon emissions explains temporal variability within most models, but not intermodel differences. Here, we show that departure from the expected relationship reflects the treatment of reactive oxidized nitrogen species (NO y ) and the fraction of emitted carbon that reacts within each chemical mechanism, which remain poorly known due to a lack of observational data. Our findings imply a need for additional observational constraints on NO y partitioning and lifetime, especially in the remote free troposphere, as well as the fate of carbon-containing reaction intermediates to test models, thereby reducing uncertainties in projections of OH and, hence, lifetimes of pollutants and greenhouse gases.

Assessing the Influence of COVID-19 on the Shortwave Radiative Fluxes Over the East Asian Marginal Seas.

The Coronavirus Disease 2019 (COVID-19) pandemic led to a widespread reduction in aerosol emissions. Using satellite observations and climate model simulations, we study the underlying mechanisms of the large decreases in solar clear-sky reflection (3.8 W m-2 or 7%) and aerosol optical depth (0.16 W m-2 or 32%) observed over the East Asian Marginal Seas in March 2020. By separating the impacts from meteorology and emissions in the model simulations, we find that about one-third of the clear-sky anomalies can be attributed to pandemic-related emission reductions, and the rest to weather variability and long-term emission trends. The model is skillful at reproducing the observed interannual variations in solar all-sky reflection, but no COVID-19 signal is discerned. The current observational and modeling capabilities will be critical for monitoring, understanding, and predicting the radiative forcing and climate impacts of the ongoing crisis.

Modulation of hydroxyl variability by ENSO in the absence of external forcing.

The hydroxyl radical (OH) is the primary oxidant in the troposphere, and the impact of its fluctuations on the methane budget has been disputed in recent years, however measurements of OH are insufficient to characterize global interannual fluctuations relevant for methane. Here, we use a 6,000-y control simulation of preindustrial conditions with a chemistry-climate model to quantify the natural variability in OH and internal feedbacks governing that variability. We find that, even in the absence of external forcing, maximum OH changes are 3.8 ± 0.8% over a decade, which is large in the context of the recent methane growth from 2007-2017. We show that the OH variability is not a white-noise process. A wavelet analysis indicates that OH variability exhibits significant feedbacks with the same periodicity as the El Niño-Southern Oscillation (ENSO). We find intrinsically generated modulation of the OH variability, suggesting that OH may show periods of rapid or no change in future decades that are solely due to the internal climate dynamics (as opposed to external forcings). An empirical orthogonal function analysis further indicates that ENSO is the dominant mode of OH variability, with the modulation of OH occurring primarily through lightning [Formula: see text] La Niña is associated with an increase in convection in the Tropical Pacific, which increases the simulated occurrence of lightning and allows for more OH production. Understanding this link between OH and ENSO may improve the predictability of the oxidative capacity of the troposphere and assist in elucidating the causes of current and historical trends in methane.

Long-Lived Species Enhance Summertime Attribution of North American Ozone to Upwind Sources.

Ground-level ozone (O3), harmful to most living things, is produced from both domestic and foreign emissions of anthropogenic precursors. Previous estimates of the linkage from distant sources rely on the sensitivity approach (i.e., modeling the change of ozone concentrations that result from modifying precursor emissions) as well as the tagging approach (i.e., tracking ozone produced from specific O3 precursors emitted from one region). Here, for the first time, we tag all O3 precursors (i.e., nitrogen oxides (NOx), carbon monoxide (CO), and volatile organic compounds (VOCs)) from East Asia and explicitly track their physicochemical evolution without perturbing the nonlinear O3 chemistry. We show that, even in summer, when intercontinental influence on ozone has typically been found to be weakest, nearly 3 parts per billion by volume (ppbv) seasonal average surface O3 over North America can be attributed to East Asian anthropogenic emissions, compared with 0.7 ppbv using the sensitivity approach and 0.5 ppbv by tagging reactive nitrogen oxides. Considering the acute effects of O3 exposure, approximately 670 cardiovascular and 300 respiratory premature mortalities within North America could be attributed to East Asia. CO and longer-lived VOCs, largely overlooked in previous studies, extend the influence of regional ozone precursors emissions and, thus, greatly enhance O3 attribution to source region.

Effect of climate change on surface ozone over North America, Europe, and East Asia.

The effect of future climate change on surface ozone over North America, Europe, and East Asia is evaluated using present-day (2000s) and future (2100s) hourly surface ozone simulated by four global models. Future climate follows RCP8.5, while methane and anthropogenic ozone precursors are fixed at year-2000 levels. Climate change shifts the seasonal surface ozone peak to earlier in the year and increases the amplitude of the annual cycle. Increases in mean summertime and high-percentile ozone are generally found in polluted environments, while decreases are found in clean environments. We propose climate change augments the efficiency of precursor emissions to generate surface ozone in polluted regions, thus reducing precursor export to neighboring downwind locations. Even with constant biogenic emissions, climate change causes the largest ozone increases at high percentiles. In most cases, air quality extreme episodes become larger and contain higher ozone levels relative to the rest of the distribution.

Last millennium hurricane activity linked to endogenous climate variability.

Despite increased Atlantic hurricane risk, projected trends in hurricane frequency in the warming climate are still highly uncertain, mainly due to short instrumental record that limits our understanding of hurricane activity and its relationship to climate. Here we extend the record to the last millennium using two independent estimates: a reconstruction from sedimentary paleohurricane records and a statistical model of hurricane activity using sea surface temperatures (SSTs). We find statistically significant agreement between the two estimates and the late 20th century hurricane frequency is within the range seen over the past millennium. Numerical simulations using a hurricane-permitting climate model suggest that hurricane activity was likely driven by endogenous climate variability and linked to anomalous SSTs of warm Atlantic and cold Pacific. Volcanic eruptions can induce peaks in hurricane activity, but such peaks would likely be too weak to be detected in the proxy record due to large endogenous variability.

Global air quality and climate.

Emissions of air pollutants and their precursors determine regional air quality and can alter climate. Climate change can perturb the long-range transport, chemical processing, and local meteorology that influence air pollution. We review the implications of projected changes in methane (CH(4)), ozone precursors (O(3)), and aerosols for climate (expressed in terms of the radiative forcing metric or changes in global surface temperature) and hemispheric-to-continental scale air quality. Reducing the O(3) precursor CH(4) would slow near-term warming by decreasing both CH(4) and tropospheric O(3). Uncertainty remains as to the net climate forcing from anthropogenic nitrogen oxide (NO(x)) emissions, which increase tropospheric O(3) (warming) but also increase aerosols and decrease CH(4) (both cooling). Anthropogenic emissions of carbon monoxide (CO) and non-CH(4) volatile organic compounds (NMVOC) warm by increasing both O(3) and CH(4). Radiative impacts from secondary organic aerosols (SOA) are poorly understood. Black carbon emission controls, by reducing the absorption of sunlight in the atmosphere and on snow and ice, have the potential to slow near-term warming, but uncertainties in coincident emissions of reflective (cooling) aerosols and poorly constrained cloud indirect effects confound robust estimates of net climate impacts. Reducing sulfate and nitrate aerosols would improve air quality and lessen interference with the hydrologic cycle, but lead to warming. A holistic and balanced view is thus needed to assess how air pollution controls influence climate; a first step towards this goal involves estimating net climate impacts from individual emission sectors. Modeling and observational analyses suggest a warming climate degrades air quality (increasing surface O(3) and particulate matter) in many populated regions, including during pollution episodes. Prior Intergovernmental Panel on Climate Change (IPCC) scenarios (SRES) allowed unconstrained growth, whereas the Representative Concentration Pathway (RCP) scenarios assume uniformly an aggressive reduction, of air pollutant emissions. New estimates from the current generation of chemistry-climate models with RCP emissions thus project improved air quality over the next century relative to those using the IPCC SRES scenarios. These two sets of projections likely bracket possible futures. We find that uncertainty in emission-driven changes in air quality is generally greater than uncertainty in climate-driven changes. Confidence in air quality projections is limited by the reliability of anthropogenic emission trajectories and the uncertainties in regional climate responses, feedbacks with the terrestrial biosphere, and oxidation pathways affecting O(3) and SOA.

Southeast Atmosphere Studies: learning from model-observation syntheses.

Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes) elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS) conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales. This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA) and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and elsewhere. Here we address questions surrounding four key themes: gas-phase chemistry, aerosol chemistry, regional climate and chemistry interactions, and natural and anthropogenic emissions. We expect this review to serve as a guidance for future modeling efforts.

A potential large and persistent black carbon forcing over Northern Pacific inferred from satellite observations.

Black carbon (BC) aerosol strongly absorbs solar radiation, which warms climate. However, accurate estimation of BC's climate effect is limited by the uncertainties of its spatiotemporal distribution, especially over remote oceanic areas. The HIAPER Pole-to-Pole Observation (HIPPO) program from 2009 to 2011 intercepted multiple snapshots of BC profiles over Pacific in various seasons, and revealed a 2 to 5 times overestimate of BC by current global models. In this study, we compared the measurements from aircraft campaigns and satellites, and found a robust association between BC concentrations and satellite-retrieved CO, tropospheric NO2, and aerosol optical depth (AOD) (R2 > 0.8). This establishes a basis to construct a satellite-based column BC approximation (sBC*) over remote oceans. The inferred sBC* shows that Asian outflows in spring bring much more BC aerosols to the mid-Pacific than those occurring in other seasons. In addition, inter-annual variability of sBC* is seen over the Northern Pacific, with abundances varying consistently with the springtime Pacific/North American (PNA) index. Our sBC* dataset infers a widespread overestimation of BC loadings and BC Direct Radiative Forcing by current models over North Pacific, which further suggests that large uncertainties exist on aerosol-climate interactions over other remote oceanic areas beyond Pacific.

Global O3-CO Correlations in a Chemistry and Transport Model During July-August: Evaluation with TES Satellite Observations and Sensitivity to Input Meteorological Data and Emissions.

We examine the capability of the Global Modeling Initiative (GMI) chemistry and transport model to reproduce global mid-tropospheric (618hPa) O3-CO correlations determined by the measurements from Tropospheric Emission Spectrometer (TES) aboard NASA's Aura satellite during boreal summer (July-August). The model is driven by three meteorological data sets (fvGCM with sea surface temperature for 1995, GEOS4-DAS for 2005, and MERRA for 2005), allowing us to examine the sensitivity of model O3-CO correlations to input meteorological data. Model simulations of radionuclide tracers (222Rn, 210Pb, and 7Be) are used to illustrate the differences in transport-related processes among the meteorological data sets. Simulated O3 values are evaluated with climatological ozone profiles from ozonesonde measurements and satellite tropospheric O3 columns. Despite the fact that three simulations show significantly different global and regional distributions of O3 and CO concentrations, all simulations show similar patterns of O3-CO correlations on a global scale. These patterns are consistent with those derived from TES observations, except in the tropical easterly biomass burning outflow regions. Discrepancies in regional O3-CO correlation patterns in the three simulations may be attributed to differences in convective transport, stratospheric influence, and subsidence, among other processes. To understand how various emissions drive global O3-CO correlation patterns, we examine the sensitivity of GMI/MERRA model-calculated O3 and CO concentrations and their correlations to emission types (fossil fuel, biomass burning, biogenic, and lightning NOx emissions). Fossil fuel and biomass burning emissions are mainly responsible for the strong positive O3-CO correlations over continental outflow regions in both hemispheres. Biogenic emissions have a relatively smaller impact on O3-CO correlations than other emissions, but are largely responsible for the negative correlations over the tropical eastern Pacific, reflecting the fact that O3 is consumed and CO generated during the atmospheric oxidation process of isoprene under low NOx conditions. We find that lightning NOx emissions degrade both positive correlations at mid-/high- latitudes and negative correlations in the tropics because ozone production downwind of lightning NOx emissions is not directly related to the emission and transport of CO. Our study concludes that O3-CO correlations may be used effectively to constrain the sources of regional tropospheric O3 in global 3-D models, especially for those regions where convective transport of pollution plays an important role.

Prospects for a prolonged slowdown in global warming in the early 21st century.

Global mean temperature over 1998 to 2015 increased at a slower rate (0.1 K decade-1) compared with the ensemble mean (forced) warming rate projected by Coupled Model Intercomparison Project 5 (CMIP5) models (0.2 K decade-1). Here we investigate the prospects for this slower rate to persist for a decade or more. The slower rate could persist if the transient climate response is overestimated by CMIP5 models by a factor of two, as suggested by recent low-end estimates. Alternatively, using CMIP5 models' warming rate, the slower rate could still persist due to strong multidecadal internal variability cooling. Combining the CMIP5 ensemble warming rate with internal variability episodes from a single climate model-having the strongest multidecadal variability among CMIP5 models-we estimate that the warming slowdown (<0.1 K decade-1 trend beginning in 1998) could persist, due to internal variability cooling, through 2020, 2025 or 2030 with probabilities 16%, 11% and 6%, respectively.

Co-benefits of global and regional greenhouse gas mitigation on U.S. air quality in 2050.

Policies to mitigate greenhouse gas (GHG) emissions will not only slow climate change, but can also have ancillary benefits of improved air quality. Here we examine the co-benefits of both global and regional GHG mitigation on U.S. air quality in 2050 at fine resolution, using dynamical downscaling methods, building on a previous global co-benefits study (West et al., 2013). The co-benefits for U.S. air quality are quantified via two mechanisms: through reductions in co-emitted air pollutants from the same sources, and by slowing climate change and its influence on air quality, following West et al. (2013). Additionally, we separate the total co-benefits into contributions from domestic GHG mitigation versus mitigation in foreign countries. We use the WRF model to dynamically downscale future global climate to the regional scale, the SMOKE program to directly process global anthropogenic emissions into the regional domain, and we provide dynamical boundary conditions from global simulations to the regional CMAQ model. The total co-benefits of global GHG mitigation from the RCP4.5 scenario compared with its reference are estimated to be higher in the eastern U.S. (ranging from 0.6-1.0 µg m-3) than the west (0-0.4 µg m-3) for PM2.5, with an average of 0.47 µg m-3 over U.S.; for O3, the total co-benefits are more uniform at 2-5 ppb with U.S. average of 3.55 ppb. Comparing the two mechanisms of co-benefits, we find that reductions of co-emitted air pollutants have a much greater influence on both PM2.5 (96% of the total co-benefits) and O3 (89% of the total) than the second co-benefits mechanism via slowing climate change, consistent with West et al. (2013). GHG mitigation from foreign countries contributes more to the U.S. O3 reduction (76% of the total) than that from domestic GHG mitigation only (24%), highlighting the importance of global methane reductions and the intercontinental transport of air pollutants. For PM2.5, the benefits of domestic GHG control are greater (74% of total). Since foreign contributions to co-benefits can be substantial, with foreign O3 benefits much larger than those from domestic reductions, previous studies that focus on local or regional co-benefits may greatly underestimate the total co-benefits of global GHG reductions. We conclude that the U.S. can gain significantly greater domestic air quality co-benefits by engaging with other nations to control GHGs.

The effect of future ambient air pollution on human premature mortality to 2100 using output from the ACCMIP model ensemble.

Ambient air pollution from ground-level ozone and fine particulate matter (PM2.5) is associated with premature mortality. Future concentrations of these air pollutants will be driven by natural and anthropogenic emissions and by climate change. Using anthropogenic and biomass burning emissions projected in the four Representative Concentration Pathway scenarios (RCPs), the ACCMIP ensemble of chemistry-climate models simulated future concentrations of ozone and PM2.5 at selected decades between 2000 and 2100. We use output from the ACCMIP ensemble, together with projections of future population and baseline mortality rates, to quantify the human premature mortality impacts of future ambient air pollution. Future air pollution-related premature mortality in 2030, 2050 and 2100 is estimated for each scenario and for each model using a health impact function based on changes in concentrations of ozone and PM2.5 relative to 2000 and projected future population and baseline mortality rates. Additionally, the global mortality burden of ozone and PM2.5 in 2000 and each future period is estimated relative to 1850 concentrations, using present-day and future population and baseline mortality rates. The change in future ozone concentrations relative to 2000 is associated with excess global premature mortality in some scenarios/periods, particularly in RCP8.5 in 2100 (316 thousand deaths/year), likely driven by the large increase in methane emissions and by the net effect of climate change projected in this scenario, but it leads to considerable avoided premature mortality for the three other RCPs. However, the global mortality burden of ozone markedly increases from 382,000 (121,000 to 728,000) deaths/year in 2000 to between 1.09 and 2.36 million deaths/year in 2100, across RCPs, mostly due to the effect of increases in population and baseline mortality rates. PM2.5 concentrations decrease relative to 2000 in all scenarios, due to projected reductions in emissions, and are associated with avoided premature mortality, particularly in 2100: between -2.39 and -1.31 million deaths/year for the four RCPs. The global mortality burden of PM2.5 is estimated to decrease from 1.70 (1.30 to 2.10) million deaths/year in 2000 to between 0.95 and 1.55 million deaths/year in 2100 for the four RCPs, due to the combined effect of decreases in PM2.5 concentrations and changes in population and baseline mortality rates. Trends in future air pollution-related mortality vary regionally across scenarios, reflecting assumptions for economic growth and air pollution control specific to each RCP and region. Mortality estimates differ among chemistry-climate models due to differences in simulated pollutant concentrations, which is the greatest contributor to overall mortality uncertainty for most cases assessed here, supporting the use of model ensembles to characterize uncertainty. Increases in exposed population and baseline mortality rates of respiratory diseases magnify the impact on premature mortality of changes in future air pollutant concentrations and explain why the future global mortality burden of air pollution can exceed the current burden, even where air pollutant concentrations decrease.

Observational constraints on glyoxal production from isoprene oxidation and its contribution to organic aerosol over the Southeast United States.

We use a 0-D photochemical box model and a 3-D global chemistry-climate model, combined with observations from the NOAA Southeast Nexus (SENEX) aircraft campaign, to understand the sources and sinks of glyoxal over the Southeast United States. Box model simulations suggest a large difference in glyoxal production among three isoprene oxidation mechanisms (AM3ST, AM3B, and MCM v3.3.1). These mechanisms are then implemented into a 3-D global chemistry-climate model. Comparison with field observations shows that the average vertical profile of glyoxal is best reproduced by AM3ST with an effective reactive uptake coefficient γglyx of 2 × 10-3, and AM3B without heterogeneous loss of glyoxal. The two mechanisms lead to 0-0.8 µg m-3 secondary organic aerosol (SOA) from glyoxal in the boundary layer of the Southeast U.S. in summer. We consider this to be the lower limit for the contribution of glyoxal to SOA, as other sources of glyoxal other than isoprene are not included in our model. In addition, we find that AM3B shows better agreement on both formaldehyde and the correlation between glyoxal and formaldehyde (RGF = [GLYX]/[HCHO]), resulting from the suppression of δ-isoprene peroxy radicals (δ-ISOPO2). We also find that MCM v3.3.1 may underestimate glyoxal production from isoprene oxidation, in part due to an underestimated yield from the reaction of IEPOX peroxy radicals (IEPOXOO) with HO2. Our work highlights that the gas-phase production of glyoxal represents a large uncertainty in quantifying its contribution to SOA.

Climate variability modulates western US ozone air quality in spring via deep stratospheric intrusions.

Evidence suggests deep stratospheric intrusions can elevate western US surface ozone to unhealthy levels during spring. These intrusions can be classified as 'exceptional events', which are not counted towards non-attainment determinations. Understanding the factors driving the year-to-year variability of these intrusions is thus relevant for effective implementation of the US ozone air quality standard. Here we use observations and model simulations to link these events to modes of climate variability. We show more frequent late spring stratospheric intrusions when the polar jet meanders towards the western United States, such as occurs following strong La Niña winters (Niño3.4<-1.0 °C). While El Niño leads to enhancements of upper tropospheric ozone, we find this influence does not reach surface air. Fewer and weaker intrusion events follow in the two springs after the 1991 volcanic eruption of Mt. Pinatubo. The linkage between La Niña and western US stratospheric intrusions can be exploited to provide a few months of lead time during which preparations could be made to deploy targeted measurements aimed at identifying these exceptional events.

Co-benefits of Global Greenhouse Gas Mitigation for Future Air Quality and Human Health.

Actions to reduce greenhouse gas (GHG) emissions often reduce co-emitted air pollutants, bringing co-benefits for air quality and human health. Past studies1-6 typically evaluated near-term and local co-benefits, neglecting the long-range transport of air pollutants7-9, long-term demographic changes, and the influence of climate change on air quality10-12. Here we simulate the co-benefits of global GHG reductions on air quality and human health using a global atmospheric model and consistent future scenarios, via two mechanisms: a) reducing co-emitted air pollutants, and b) slowing climate change and its effect on air quality. We use new relationships between chronic mortality and exposure to fine particulate matter13 and ozone14, global modeling methods15, and new future scenarios16. Relative to a reference scenario, global GHG mitigation avoids 0.5±0.2, 1.3±0.5, and 2.2±0.8 million premature deaths in 2030, 2050, and 2100. Global average marginal co-benefits of avoided mortality are $50-380 (ton CO2)-1, which exceed previous estimates, exceed marginal abatement costs in 2030 and 2050, and are within the low range of costs in 2100. East Asian co-benefits are 10-70 times the marginal cost in 2030. Air quality and health co-benefits, especially as they are mainly local and near-term, provide strong additional motivation for transitioning to a low-carbon future.

An estimate of the global burden of anthropogenic ozone and fine particulate matter on premature human mortality using atmospheric modeling.

BACKGROUND: Ground-level concentrations of ozone (O3) and fine particulate matter [< or = 2.5 microm in aerodynamic diameter (PM2.5)] have increased since preindustrial times in urban and rural regions and are associated with cardiovascular and respiratory mortality. OBJECTIVES: We estimated the global burden of mortality due to O3 and PM2.5 from anthropogenic emissions using global atmospheric chemical transport model simulations of preindustrial and present-day (2000) concentrations to derive exposure estimates. METHODS: Attributable mortalities were estimated using health impact functions based on long-term relative risk estimates for O3 and PM2.5 from the epidemiology literature. Using simulated concentrations rather than previous methods based on measurements allows the inclusion of rural areas where measurements are often unavailable and avoids making assumptions for background air pollution. RESULTS: Anthropogenic O3 was associated with an estimated 0.7 +/- 0.3 million respiratory mortalities (6.3 +/- 3.0 million years of life lost) annually. Anthropogenic PM2.5 was associated with 3.5 +/- 0.9 million cardiopulmonary and 220,000 +/- 80,000 lung cancer mortalities (30 +/- 7.6 million years of life lost) annually. Mortality estimates were reduced approximately 30% when we assumed low-concentration thresholds of 33.3 ppb for O3 and 5.8 microg/m3 for PM2.5. These estimates were sensitive to concentration thresholds and concentration-mortality relationships, often by > 50%. CONCLUSIONS: Anthropogenic O3 and PM2.5 contribute substantially to global premature mortality. PM2.5 mortality estimates are about 50% higher than previous measurement-based estimates based on common assumptions, mainly because of methodologic differences. Specifically, we included rural populations, suggesting higher estimates; however, the coarse resolution of the global atmospheric model may underestimate urban PM(2.5) exposures.

Global health benefits of mitigating ozone pollution with methane emission controls.

Methane (CH(4)) contributes to the growing global background concentration of tropospheric ozone (O(3)), an air pollutant associated with premature mortality. Methane and ozone are also important greenhouse gases. Reducing methane emissions therefore decreases surface ozone everywhere while slowing climate warming, but although methane mitigation has been considered to address climate change, it has not for air quality. Here we show that global decreases in surface ozone concentrations, due to methane mitigation, result in substantial and widespread decreases in premature human mortality. Reducing global anthropogenic methane emissions by 20% beginning in 2010 would decrease the average daily maximum 8-h surface ozone by approximately 1 part per billion by volume globally. By using epidemiologic ozone-mortality relationships, this ozone reduction is estimated to prevent approximately 30,000 premature all-cause mortalities globally in 2030, and approximately 370,000 between 2010 and 2030. If only cardiovascular and respiratory mortalities are considered, approximately 17,000 global mortalities can be avoided in 2030. The marginal cost-effectiveness of this 20% methane reduction is estimated to be approximately 420,000 US dollars per avoided mortality. If avoided mortalities are valued at 1 US dollars million each, the benefit is approximately 240 US dollars per tone of CH(4) ( approximately 12 US dollars per tone of CO(2) equivalent), which exceeds the marginal cost of the methane reduction. These estimated air pollution ancillary benefits of climate-motivated methane emission reductions are comparable with those estimated previously for CO(2). Methane mitigation offers a unique opportunity to improve air quality globally and can be a cost-effective component of international ozone management, bringing multiple benefits for air quality, public health, agriculture, climate, and energy.