Evaluating the Impact of Chemical Complexity and Horizontal Resolution on Tropospheric Ozone Over the Conterminous US With a Global Variable Resolution Chemistry Model.

A new configuration of the Community Earth System Model (CESM)/Community Atmosphere Model with full chemistry (CAM-chem) supporting the capability of horizontal mesh refinement through the use of the spectral element (SE) dynamical core is developed and called CESM/CAM-chem-SE. Horizontal mesh refinement in CESM/CAM-chem-SE is unique and novel in that pollutants such as ozone are accurately represented at human exposure relevant scales while also directly including global feedbacks. CESM/CAM-chem-SE with mesh refinement down to ∼14 km over the conterminous US (CONUS) is the beginning of the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICAv0). Here, MUSICAv0 is evaluated and used to better understand how horizontal resolution and chemical complexity impact ozone and ozone precursors over CONUS as compared to measurements from five aircraft campaigns, which occurred in 2013. This field campaign analysis demonstrates the importance of using finer horizontal resolution to accurately simulate ozone precursors such as nitrogen oxides and carbon monoxide. In general, the impact of using more complex chemistry on ozone and other oxidation products is more pronounced when using finer horizontal resolution where a larger number of chemical regimes are resolved. Large model biases for ozone near the surface remain in the Southeast US as compared to the aircraft observations even with updated chemistry and finer horizontal resolution. This suggests a need for adding the capability of replacing sections of global emission inventories with regional inventories, increasing the vertical resolution in the planetary boundary layer, and reducing model biases in meteorological variables such as temperature and clouds.

Large contribution of biomass burning emissions to ozone throughout the global remote troposphere.

Ozone is the third most important anthropogenic greenhouse gas after carbon dioxide and methane but has a larger uncertainty in its radiative forcing, in part because of uncertainty in the source characteristics of ozone precursors, nitrogen oxides, and volatile organic carbon that directly affect ozone formation chemistry. Tropospheric ozone also negatively affects human and ecosystem health. Biomass burning (BB) and urban emissions are significant but uncertain sources of ozone precursors. Here, we report global-scale, in situ airborne measurements of ozone and precursor source tracers from the NASA Atmospheric Tomography mission. Measurements from the remote troposphere showed that tropospheric ozone is regularly enhanced above background in polluted air masses in all regions of the globe. Ozone enhancements in air with high BB and urban emission tracers (2.1 to 23.8 ppbv [parts per billion by volume]) were generally similar to those in BB-influenced air (2.2 to 21.0 ppbv) but larger than those in urban-influenced air (-7.7 to 6.9 ppbv). Ozone attributed to BB was 2 to 10 times higher than that from urban sources in the Southern Hemisphere and the tropical Atlantic and roughly equal to that from urban sources in the Northern Hemisphere and the tropical Pacific. Three independent global chemical transport models systematically underpredict the observed influence of BB on tropospheric ozone. Potential reasons include uncertainties in modeled BB injection heights and emission inventories, export efficiency of BB emissions to the free troposphere, and chemical mechanisms of ozone production in smoke. Accurately accounting for intermittent but large and widespread BB emissions is required to understand the global tropospheric ozone burden.

Global Changes in Secondary Atmospheric Pollutants During the 2020 COVID-19 Pandemic.

We use the global Community Earth System Model to investigate the response of secondary pollutants (ozone O3, secondary organic aerosols SOA) in different parts of the world in response to modified emissions of primary pollutants during the COVID-19 pandemic. We quantify the respective effects of the reductions in NOx and in volatile organic carbon (VOC) emissions, which, in most cases, affect oxidants in opposite ways. Using model simulations, we show that the level of NOx has been reduced by typically 40% in China during February 2020 and by similar amounts in many areas of Europe and North America in mid-March to mid-April 2020, in good agreement with space and surface observations. We show that, relative to a situation in which the emission reductions are ignored and despite the calculated increase in hydroxyl and peroxy radicals, the ozone concentration increased only in a few NOx-saturated regions (northern China, northern Europe, and the US) during the winter months of the pandemic when the titration of this molecule by NOx was reduced. In other regions, where ozone is NOx-controlled, the concentration of ozone decreased. SOA concentrations decrease in response to the concurrent reduction in the NOx and VOC emissions. The model also shows that atmospheric meteorological anomalies produced substantial variations in the concentrations of chemical species during the pandemic. In Europe, for example, a large fraction of the ozone increase in February 2020 was associated with meteorological anomalies, while in the North China Plain, enhanced ozone concentrations resulted primarily from reduced emissions of primary pollutants.

Development of the Low Emissions Analysis Platform - Integrated Benefits Calculator (LEAP-IBC) tool to assess air quality and climate co-benefits: Application for Bangladesh.

Low- and middle-income countries have the largest health burdens associated with air pollution exposure, and are particularly vulnerable to climate change impacts. Substantial opportunities have been identified to simultaneously improve air quality and mitigate climate change due to overlapping sources of greenhouse gas and air pollutant emissions and because a subset of pollutants, short-lived climate pollutants (SLCPs), directly contribute to both impacts. However, planners in low- and middle-income countries often lack practical tools to quantify the air pollution and climate change impacts of different policies and measures. This paper presents a modelling framework implemented in the Low Emissions Analysis Platform - Integrated Benefits Calculator (LEAP-IBC) tool to develop integrated strategies to improve air quality, human health and mitigate climate change. The framework estimates emissions of greenhouse gases, SLCPs and air pollutants for historical years, and future projections for baseline and mitigation scenarios. These emissions are then used to quantify i) population-weighted annual average ambient PM2.5 concentrations across the target country, ii) household PM2.5 exposure of different population groups living in households cooking using different fuels/technologies and iii) radiative forcing from all emissions. Health impacts (premature mortality) attributable to ambient and household PM2.5 exposure and changes in global average temperature change are then estimated. This framework is applied in Bangladesh to evaluate the air quality and climate change benefits from implementation of Bangladesh's Nationally Determined Contribution (NDC) and National Action Plan to reduce SLCPs. Results show that the measures included to reduce GHGs in Bangladesh's NDC also have substantial benefits for air quality and human health. Full implementation of Bangladesh's NDC, and National SLCP Plan would reduce carbon dioxide, methane, black carbon and primary PM2.5 emissions by 25%, 34%, 46% and 45%, respectively in 2030 compared to a baseline scenario. These emission reductions could reduce population-weighted ambient PM2.5 concentrations in Bangladesh by 18% in 2030, and avoid approximately 12,000 and 100,000 premature deaths attributable to ambient and household PM2.5 exposures, respectively, in 2030. As countries are simultaneously planning to achieve the climate goals in the Paris Agreement, improve air quality to reduce health impacts and achieve the Sustainable Development Goals, the LEAP-IBC tool provides a practical framework by which planners can develop integrated strategies, achieving multiple air quality and climate benefits.

Methods, availability, and applications of PM2.5 exposure estimates derived from ground measurements, satellite, and atmospheric models.

Fine particulate matter (PM2.5) is a well-established risk factor for public health. To support both health risk assessment and epidemiological studies, data are needed on spatial and temporal patterns of PM2.5 exposures. This review article surveys publicly available exposure datasets for surface PM2.5 mass concentrations over the contiguous U.S., summarizes their applications and limitations, and provides suggestions on future research needs. The complex landscape of satellite instruments, model capabilities, monitor networks, and data synthesis methods offers opportunities for research development, but would benefit from guidance for new users. Guidance is provided to access publicly available PM2.5 datasets, to explain and compare different approaches for dataset generation, and to identify sources of uncertainties associated with various types of datasets. Three main sources used to create PM2.5 exposure data are ground-based measurements (especially regulatory monitoring), satellite retrievals (especially aerosol optical depth, AOD), and atmospheric chemistry models. We find inconsistencies among several publicly available PM2.5 estimates, highlighting uncertainties in the exposure datasets that are often overlooked in health effects analyses. Major differences among PM2.5 estimates emerge from the choice of data (ground-based, satellite, and/or model), the spatiotemporal resolutions, and the algorithms used to fuse data sources.Implications: Fine particulate matter (PM2.5) has large impacts on human morbidity and mortality. Even though the methods for generating the PM2.5 exposure estimates have been significantly improved in recent years, there is a lack of review articles that document PM2.5 exposure datasets that are publicly available and easily accessible by the health and air quality communities. In this article, we discuss the main methods that generate PM2.5 data, compare several publicly available datasets, and show the applications of various data fusion approaches. Guidance to access and critique these datasets are provided for stakeholders in public health sectors.

Updated Emission Factors from Diffuse Combustion Sources in Sub-Saharan Africa and Their Effect on Regional Emission Estimates.

Diffuse emission sources outside of kitchen areas are poorly understood, and measurements of their emission factors (EFs) are sparse for regions of sub-Saharan Africa. Thirty-one in-field emission measurements were taken in northern Ghana from combustion sources common to rural regions worldwide. Sources sampled included commercial cooking, trash burning, kerosene lanterns, and diesel generators. EFs were calculated for carbon monoxide (CO), carbon dioxide (CO2), as well as carbonaceous particulate matter, specifically elemental carbon (EC) and organic carbon (OC). EC and OC emissions were measured from kerosene lighting events (EFEC = 25.1 g/kg-fuel SD = 25.7, EFOC = 9.5 g/kg-fuel SD = 10.0). OC emissions from trash burning events were large and highly variable (EFOC = 38.9 g/kg-fuel SD = 30.5). Combining our results with other recent in-field emission factors for rural Ghana, we explored updated emission estimates for Ghana using a region specific emissions inventory. Large differences are calculated for all updated source emissions, showing a 96% increase in OC and 78% decrease in EC compared to prior estimates for Ghana's emissions. Differences for carbon monoxide were small when averaged across all updated source types (-1%), though the household wood use and trash burning categories individually show large differences.

Improving present day and future estimates of anthropogenic sectoral emissions and the resulting air quality impacts in Africa.

The African continent is undergoing immense social and economic change, particularly regarding population growth and urbanization, where the urban population in Africa is anticipated to increase by a factor of 3 over the next 40 years. To understand the potential health impacts from this demographical shift and design efficient emission mitigation strategies, we used improved Africa-specific emissions that account for inefficient combustion sources for a number of sectors such as transportation, household energy generation, waste burning, and home heating and cooking. When these underrepresented emissions sources are combined with the current estimates of emissions in Africa, ambient particulate matter concentrations from present-day anthropogenic activity contribute to 13 210 annual premature deaths, with the largest contributions (38%) coming from residential emissions. By scaling both the population and the emissions for projected national-scale levels of growth, the predicted health impact grows to approximately 78 986 annual premature deaths by 2030 with 45% now resulting from emissions related to energy combustion. In order to mitigate this resulting increase in premature deaths, three scenarios have been developed which reduce sector-specific future emissions based on prior targets for technological improvements and emission controls in transportation, energy production and residential activities. These targeted potential mitigation strategies can avoid up to 37% of the estimated annual premature deaths by 2030 with the largest opportunity being a reduction of 10 868 annual deaths from switching half of the energy generation in South Africa to renewable technologies.

Impacts and mitigation of excess diesel-related NOx emissions in 11 major vehicle markets.

Vehicle emissions contribute to fine particulate matter (PM2.5) and tropospheric ozone air pollution, affecting human health, crop yields and climate worldwide. On-road diesel vehicles produce approximately 20 per cent of global anthropogenic emissions of nitrogen oxides (NOx), which are key PM2.5 and ozone precursors. Regulated NOx emission limits in leading markets have been progressively tightened, but current diesel vehicles emit far more NOx under real-world operating conditions than during laboratory certification testing. Here we show that across 11 markets, representing approximately 80 per cent of global diesel vehicle sales, nearly one-third of on-road heavy-duty diesel vehicle emissions and over half of on-road light-duty diesel vehicle emissions are in excess of certification limits. These excess emissions (totalling 4.6 million tons) are associated with about 38,000 PM2.5- and ozone-related premature deaths globally in 2015, including about 10 per cent of all ozone-related premature deaths in the 28 European Union member states. Heavy-duty vehicles are the dominant contributor to excess diesel NOx emissions and associated health impacts in almost all regions. Adopting and enforcing next-generation standards (more stringent than Euro 6/VI) could nearly eliminate real-world diesel-related NOx emissions in these markets, avoiding approximately 174,000 global PM2.5- and ozone-related premature deaths in 2040. Most of these benefits can be achieved by implementing Euro VI standards where they have not yet been adopted for heavy-duty vehicles.

Transient climate and ambient health impacts due to national solid fuel cookstove emissions.

Residential solid fuel use contributes to degraded indoor and ambient air quality and may affect global surface temperature. However, the potential for national-scale cookstove intervention programs to mitigate the latter issues is not yet well known, owing to the spatial heterogeneity of aerosol emissions and impacts, along with coemitted species. Here we use a combination of atmospheric modeling, remote sensing, and adjoint sensitivity analysis to individually evaluate consequences of a 20-y linear phase-out of cookstove emissions in each country with greater than 5% of the population using solid fuel for cooking. Emissions reductions in China, India, and Ethiopia contribute to the largest global surface temperature change in 2050 [combined impact of -37 mK (11 mK to -85 mK)], whereas interventions in countries less commonly targeted for cookstove mitigation such as Azerbaijan, Ukraine, and Kazakhstan have the largest per cookstove climate benefits. Abatement in China, India, and Bangladesh contributes to the largest reduction of premature deaths from ambient air pollution, preventing 198,000 (102,000-204,000) of the 260,000 (137,000-268,000) global annual avoided deaths in 2050, whereas again emissions in Ukraine and Azerbaijan have the largest per cookstove impacts, along with Romania. Global cookstove emissions abatement results in an average surface temperature cooling of -77 mK (20 mK to -278 mK) in 2050, which increases to -118 mK (-11 mK to -335 mK) by 2100 due to delayed CO2 response. Health impacts owing to changes in ambient particulate matter with an aerodynamic diameter of 2.5 µm or less (PM2.5) amount to ∼22.5 million premature deaths prevented between 2000 and 2100.