Transboundary health impacts of transported global air pollution and international trade.

Millions of people die every year from diseases caused by exposure to outdoor air pollution. Some studies have estimated premature mortality related to local sources of air pollution, but local air quality can also be affected by atmospheric transport of pollution from distant sources. International trade is contributing to the globalization of emission and pollution as a result of the production of goods (and their associated emissions) in one region for consumption in another region. The effects of international trade on air pollutant emissions, air quality and health have been investigated regionally, but a combined, global assessment of the health impacts related to international trade and the transport of atmospheric air pollution is lacking. Here we combine four global models to estimate premature mortality caused by fine particulate matter (PM2.5) pollution as a result of atmospheric transport and the production and consumption of goods and services in different world regions. We find that, of the 3.45 million premature deaths related to PM2.5 pollution in 2007 worldwide, about 12 per cent (411,100 deaths) were related to air pollutants emitted in a region of the world other than that in which the death occurred, and about 22 per cent (762,400 deaths) were associated with goods and services produced in one region for consumption in another. For example, PM2.5 pollution produced in China in 2007 is linked to more than 64,800 premature deaths in regions other than China, including more than 3,100 premature deaths in western Europe and the USA; on the other hand, consumption in western Europe and the USA is linked to more than 108,600 premature deaths in China. Our results reveal that the transboundary health impacts of PM2.5 pollution associated with international trade are greater than those associated with long-distance atmospheric pollutant transport.

Natural gas shortages during the "coal-to-gas" transition in China have caused a large redistribution of air pollution in 2017.

The Chinese "coal-to-gas" and "coal-to-electricity" strategies aim at reducing dispersed coal consumption and related air pollution by promoting the use of clean and low-carbon fuels in northern China. Here, we show that on top of meteorological influences, the effective emission mitigation measures achieved an average decrease of fine particulate matter (PM2.5) concentrations of ∼14% in Beijing and surrounding areas (the "2+26" pilot cities) in winter 2017 compared to the same period of 2016, where the dispersed coal control measures contributed ∼60% of the total PM2.5 reductions. However, the localized air quality improvement was accompanied by a contemporaneous ∼15% upsurge of PM2.5 concentrations over large areas in southern China. We find that the pollution transfer that resulted from a shift in emissions was of a high likelihood caused by a natural gas shortage in the south due to the coal-to-gas transition in the north. The overall shortage of natural gas greatly jeopardized the air quality benefits of the coal-to-gas strategy in winter 2017 and reflects structural challenges and potential threats in China's clean-energy transition.

Disentangling the Impact of the COVID-19 Lockdowns on Urban NO2 From Natural Variability.

TROPOMI satellite data show substantial drops in nitrogen dioxide (NO2) during COVID-19 physical distancing. To attribute NO2 changes to NO x emissions changes over short timescales, one must account for meteorology. We find that meteorological patterns were especially favorable for low NO2 in much of the United States in spring 2020, complicating comparisons with spring 2019. Meteorological variations between years can cause column NO2 differences of ~15% over monthly timescales. After accounting for solar angle and meteorological considerations, we calculate that NO2 drops ranged between 9.2% and 43.4% among 20 cities in North America, with a median of 21.6%. Of the studied cities, largest NO2 drops (>30%) were in San Jose, Los Angeles, and Toronto, and smallest drops (<12%) were in Miami, Minneapolis, and Dallas. These normalized NO2 changes can be used to highlight locations with greater activity changes and better understand the sources contributing to adverse air quality in each city.

Enhanced Capabilities of TROPOMI NO2: Estimating NOX from North American Cities and Power Plants.

The TROPOspheric Monitoring Instrument (TROPOMI) is used to derive top-down NOX emissions for two large power plants and three megacities in North America. We first re-process the vertical column NO2 with an improved air mass factor to correct for a known systematic low bias in the operational retrieval near urban centers. For the two power plants, top-down NOX emissions agree to within 10% of the emissions reported by the power plants. We then derive top-down NOX emissions rates for New York City, Chicago, and Toronto, and compare them to projected bottom-up emissions inventories. In this analysis of 2018 NOX emissions, we find a +22% overestimate for New York City, a -21% underestimate in Toronto, and good agreement in Chicago in the projected bottom-up inventories when compared to the top-down emissions. Top-down NOX emissions also capture intraseasonal variability, such as the weekday versus weekend effect (emissions are +45% larger on weekdays versus weekends in Chicago). Finally, we demonstrate the enhanced capabilities of TROPOMI, which allow us to derive a NOX emissions rate for Chicago using a single overpass on July 7, 2018. The large signal-to-noise ratio of TROPOMI is well-suited for estimating NOX emissions from relatively small sources and for sub-seasonal timeframes.

Total Mercury Released to the Environment by Human Activities.

We estimate that a cumulative total of 1540 (1060-2800) Gg (gigagrams, 109 grams or thousand tonnes) of mercury (Hg) have been released by human activities up to 2010, 73% of which was released after 1850. Of this liberated Hg, 470 Gg were emitted directly into the atmosphere, and 74% of the air emissions were elemental Hg. Cumulatively, about 1070 Gg were released to land and water bodies. Though annual releases of Hg have been relatively stable since 1880 at 8 ± 2 Gg, except for wartime, the distributions of those releases among source types, world regions, and environmental media have changed dramatically. Production of Hg accounts for 27% of cumulative Hg releases to the environment, followed by silver production (24%) and chemicals manufacturing (12%). North America (30%), Europe (27%), and Asia (16%) have experienced the largest releases. Biogeochemical modeling shows a 3.2-fold increase in the atmospheric burden relative to 1850 and a contemporary atmospheric reservoir of 4.57 Gg, both of which agree well with observational constraints. We find that approximately 40% (390 Gg) of the Hg discarded to land and water must be sequestered at contaminated sites to maintain consistency with recent declines in atmospheric Hg concentrations.

China's international trade and air pollution in the United States.

China is the world's largest emitter of anthropogenic air pollutants, and measurable amounts of Chinese pollution are transported via the atmosphere to other countries, including the United States. However, a large fraction of Chinese emissions is due to manufacture of goods for foreign consumption. Here, we analyze the impacts of trade-related Chinese air pollutant emissions on the global atmospheric environment, linking an economic-emission analysis and atmospheric chemical transport modeling. We find that in 2006, 36% of anthropogenic sulfur dioxide, 27% of nitrogen oxides, 22% of carbon monoxide, and 17% of black carbon emitted in China were associated with production of goods for export. For each of these pollutants, about 21% of export-related Chinese emissions were attributed to China-to-US export. Atmospheric modeling shows that transport of the export-related Chinese pollution contributed 3-10% of annual mean surface sulfate concentrations and 0.5-1.5% of ozone over the western United States in 2006. This Chinese pollution also resulted in one extra day or more of noncompliance with the US ozone standard in 2006 over the Los Angeles area and many regions in the eastern United States. On a daily basis, the export-related Chinese pollution contributed, at a maximum, 12-24% of sulfate concentrations over the western United States. As the United States outsourced manufacturing to China, sulfate pollution in 2006 increased in the western United States but decreased in the eastern United States, reflecting the competing effect between enhanced transport of Chinese pollution and reduced US emissions. Our findings are relevant to international efforts to reduce transboundary air pollution.

Impacts of the Minamata convention on mercury emissions and global deposition from coal-fired power generation in Asia.

We explore implications of the United Nations Minamata Convention on Mercury for emissions from Asian coal-fired power generation, and resulting changes to deposition worldwide by 2050. We use engineering analysis, document analysis, and interviews to construct plausible technology scenarios consistent with the Convention. We translate these scenarios into emissions projections for 2050, and use the GEOS-Chem model to calculate global mercury deposition. Where technology requirements in the Convention are flexibly defined, under a global energy and development scenario that relies heavily on coal, we project ∼90 and 150 Mg·y(-1) of avoided power sector emissions for China and India, respectively, in 2050, compared to a scenario in which only current technologies are used. Benefits of this avoided emissions growth are primarily captured regionally, with projected changes in annual average gross deposition over China and India ∼2 and 13 µg·m(-2) lower, respectively, than the current technology case. Stricter, but technologically feasible, mercury control requirements in both countries could lead to a combined additional 170 Mg·y(-1) avoided emissions. Assuming only current technologies but a global transition away from coal avoids 6% and 36% more emissions than this strict technology scenario under heavy coal use for China and India, respectively.

Light absorption properties and radiative effects of primary organic aerosol emissions.

Organic aerosols (OAs) in the atmosphere affect Earth's energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called "brown carbon" (BrC) component. However, the absorptivities of OAs are not represented or are poorly represented in current climate and chemical transport models. In this study, we provide a method to constrain the BrC absorptivity at the emission inventory level using recent laboratory and field observations. We review available measurements of the light-absorbing primary OA (POA), and quantify the wavelength-dependent imaginary refractive indices (kOA, the fundamental optical parameter determining the particle's absorptivity) and their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the kOA of biomass/biofuel combustion sources as a function of the black carbon (BC)-to-OA ratio, indicating that the absorptive properties of POA depend strongly on burning conditions. The derived fuel-type-based kOA profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated kOA values of sectoral and total POA emissions are presented. Results of a simple radiative transfer model show that the POA absorptivity warms the atmosphere significantly and leads to ∼27% reduction in the amount of the net global average POA cooling compared to results from the nonabsorbing assumption.

Effectiveness of mitigation measures in reducing future primary particulate matter emissions from on-road vehicle exhaust.

This work evaluates the effectiveness of on-road primary particulate matter emission reductions that can be achieved by long-term vehicle scrappage and retrofit measures on regional and global levels. Scenario analysis shows that scrappage can provide significant emission reductions as soon as the measures begin, whereas retrofit provides greater emission reductions in later years, when more advanced technologies become available in most regions. Reductions are compared with a baseline that already accounts for implementation of clean vehicle standards. The greatest global emission reductions from a scrappage program occur 5 to 10 years after its introduction and can reach as much as 70%. The greatest reductions with retrofit occur around 2030 and range from 16-31%. Monte Carlo simulations are used to evaluate how uncertainties in the composition of the vehicle fleet affect predicted reductions. Scrappage and retrofit reduce global emissions by 22-60% and 15-31%, respectively, within 95% confidence intervals, under a midrange scenario in the year 2030. The simulations provide guidance about which strategies are most effective for specific regions. Retrofit is preferable for high-income regions. For regions where early emission standards are in place, scrappage is suggested, followed by retrofit after more advanced emission standards are introduced. The early implementation of advanced emission standards is recommended for Western and Eastern Africa.

Historical Mercury releases from commercial products: global environmental implications.

The intentional use of mercury (Hg) in products and processes ("commercial Hg") has contributed a large and previously unquantified anthropogenic source of Hg to the global environment over the industrial era, with major implications for Hg accumulation in environmental reservoirs. We present a global inventory of commercial Hg uses and releases to the atmosphere, water, soil, and landfills from 1850 to 2010. Previous inventories of anthropogenic Hg releases have focused almost exclusively on atmospheric emissions from "byproduct" sectors (e.g., fossil fuel combustion). Cumulative anthropogenic atmospheric Hg emissions since 1850 have recently been estimated at 215 Gg (only including commercial Hg releases from chlor-alkali production, waste incineration, and mining). We find that other commercial Hg uses and nonatmospheric releases from chlor-alkali and mining result in an additional 540 Gg of Hg released to the global environment since 1850 (air: 20%; water: 30%; soil: 30%; landfills: 20%). Some of this release has been sequestered in landfills and benthic sediments, but 310 Gg actively cycles among geochemical reservoirs and contributes to elevated present-day environmental Hg concentrations. Commercial Hg use peaked in 1970 and has declined sharply since. We use our inventory of historical environmental releases to force a global biogeochemical model that includes new estimates of the global burial in ocean margin sediments. Accounting for commercial Hg releases improves model consistency with observed atmospheric concentrations and associated historical trends.

Mercury stable isotope signatures of world coal deposits and historical coal combustion emissions.

Mercury (Hg) emissions from coal combustion contribute approximately half of anthropogenic Hg emissions to the atmosphere. With the implementation of the first legally binding UNEP treaty aimed at reducing anthropogenic Hg emissions, the identification and traceability of Hg emissions from different countries/regions are critically important. Here, we present a comprehensive world coal Hg stable isotope database including 108 new coal samples from major coal-producing deposits in South Africa, China, Europe, India, Indonesia, Mongolia, former USSR, and the U.S. A 4.7‰ range in δ(202)Hg (-3.9 to 0.8‰) and a 1‰ range in Δ(199)Hg (-0.6 to 0.4‰) are observed. Fourteen (p < 0.05) to 17 (p < 0.1) of the 28 pairwise comparisons between eight global regions are statistically distinguishable on the basis of δ(202)Hg, Δ(199)Hg or both, highlighting the potential application of Hg isotope signatures to coal Hg emissions tracing. A revised coal combustion Hg isotope fractionation model is presented, and suggests that gaseous elemental coal Hg emissions are enriched in the heavier Hg isotopes relative to oxidized forms of emitted Hg. The model explains to first order the published δ(202)Hg observations on near-field Hg deposition from a power plant and global scale atmospheric gaseous Hg. Yet, model uncertainties appear too large at present to permit straightforward Hg isotope source identification of atmospheric forms of Hg. Finally, global historical (1850-2008) coal Hg isotope emission curves were modeled and indicate modern-day mean δ(202)Hg and Δ(199)Hg values for bulk coal emissions of -1.2 ± 0.5‰ (1SD) and 0.05 ± 0.06‰ (1SD).

Global chemical composition of ambient fine particulate matter for exposure assessment.

Epidemiologic and health impact studies are inhibited by the paucity of global, long-term measurements of the chemical composition of fine particulate matter. We inferred PM2.5 chemical composition at 0.1° × 0.1° spatial resolution for 2004-2008 by combining aerosol optical depth retrieved from the MODIS and MISR satellite instruments, with coincident profile and composition information from the GEOS-Chem global chemical transport model. Evaluation of the satellite-model PM2.5 composition data set with North American in situ measurements indicated significant spatial agreement for secondary inorganic aerosol, particulate organic mass, black carbon, mineral dust, and sea salt. We found that global population-weighted PM2.5 concentrations were dominated by particulate organic mass (11.9 ± 7.3 µg/m(3)), secondary inorganic aerosol (11.1 ± 5.0 µg/m(3)), and mineral dust (11.1 ± 7.9 µg/m(3)). Secondary inorganic PM2.5 concentrations exceeded 30 µg/m(3) over East China. Sensitivity simulations suggested that population-weighted ambient PM2.5 from biofuel burning (11 µg/m(3)) could be almost as large as from fossil fuel combustion sources (17 µg/m(3)). These estimates offer information about global population exposure to the chemical components and sources of PM2.5.

Ozone monitoring instrument observations of interannual increases in SO2 emissions from Indian coal-fired power plants during 2005-2012.

Due to the rapid growth of electricity demand and the absence of regulations, sulfur dioxide (SO2) emissions from coal-fired power plants in India have increased notably in the past decade. In this study, we present the first interannual comparison of SO2 emissions and the satellite SO2 observations from the Ozone Monitoring Instrument (OMI) for Indian coal-fired power plants during the OMI era of 2005-2012. A detailed unit-based inventory is developed for the Indian coal-fired power sector, and results show that its SO2 emissions increased dramatically by 71% during 2005-2012. Using the oversampling technique, yearly high-resolution OMI maps for the whole domain of India are created, and they reveal a continuous increase in SO2 columns over India. Power plant regions with annual SO2 emissions greater than 50 Gg year(-1) produce statistically significant OMI signals, and a high correlation (R = 0.93) is found between SO2 emissions and OMI-observed SO2 burdens. Contrary to the decreasing trend of national mean SO2 concentrations reported by the Indian Government, both the total OMI-observed SO2 and annual average SO2 concentrations in coal-fired power plant regions increased by >60% during 2005-2012, implying the air quality monitoring network needs to be optimized to reflect the true SO2 situation in India.

Source forensics of black carbon aerosols from China.

The limited understanding of black carbon (BC) aerosol emissions from incomplete combustion causes a poorly constrained anthropogenic climate warming that globally may be second only to CO2 and regionally, such as over East Asia, the dominant driver of climate change. The relative contribution to atmospheric BC from fossil fuel versus biomass combustion is important to constrain as fossil BC is a stronger climate forcer. The source apportionment is the underpinning for targeted mitigation actions. However, technology-based "bottom-up" emission inventories are inconclusive, largely due to uncertain BC emission factors from small-scale/household combustion and open burning. We use "top-down" radiocarbon measurements of atmospheric BC from five sites including three city sites and two regional sites to determine that fossil fuel combustion produces 80 ± 6% of the BC emitted from China. This source-diagnostic radiocarbon signal in the ambient aerosol over East Asia establishes a much larger role for fossil fuel combustion than suggested by all 15 BC emission inventory models, including one with monthly resolution. Our results suggest that current climate modeling should refine both BC emission strength and consider the stronger radiative absorption associated with fossil-fuel-derived BC. To mitigate near-term climate effects and improve air quality in East Asia, activities such as residential coal combustion and city traffic should be targeted.

Increase in NOx emissions from Indian thermal power plants during 1996-2010: unit-based inventories and multisatellite observations.

Driven by rapid economic development and growing electricity demand, NO(x) emissions (E) from the power sector in India have increased dramatically since the mid-1990s. In this study, we present the NO(x) emissions from Indian public thermal power plants for the period 1996-2010 using a unit-based methodology and compare the emission estimates with the satellite observations of NO(2) tropospheric vertical column densities (TVCDs) from four spaceborne instruments: GOME, SCIAMACHY, OMI, and GOME-2. Results show that NO(x) emissions from Indian power plants increased by at least 70% during 1996-2010. Coal-fired power plants, NO(x) emissions from which are not regulated in India, contribute ∼96% to the total power sector emissions, followed by gas-fired (∼4%) and oil-fired (<1%) ones. A number of isolated NO(2) hot spots are observed over the power plant areas, and good agreement between NO(2) TVCDs and NO(x) emissions is found for areas dominated by power plant emissions. Average NO(2) TVCDs over power plant areas were continuously increasing during the study period. We find that the ratio of ΔE/E to ΔTVCD/TVCD changed from greater than one to less than one around 2005-2008, implying that a transition of the overall NO(x) chemistry occurred over the power plant areas, which may cause significant impact on the atmospheric environment.

Analyzing the spatio-temporal variation of the CO2 emissions from district heating systems with "Coal-to-Gas" transition: Evidence from GTWR model and satellite data in China.

Understanding the spatio-temporal heterogeneous effects of socioeconomic and meteorological factors on CO2 emissions from combinations of different district heating systems with "Coal-to-Gas" transition can contribute to the development of future low-carbon energy systems that are efficient and effective. This work downscales city-level CO2 emissions to a 3 × 3 km2 gridded level in northern China during 2012 to 2018. By employing the Geographically and Temporally Weighted Regression (GTWR) model, nighttime light (NTL) data are adopted as a proxy of the level of urbanization, and the Temperature-Humidity-Wind (THW) Index is used as a proxy of meteorological factors in the downscaling model. The results show that, for more than 85% of the cities, urbanization significantly enhances the CO2 emissions of district heating systems, while the THW Index shows negative impacts on CO2 emissions. Significant spatial and temporal heterogeneity exists. The grids with the highest CO2 emissions from coal-fired boilers (grids with annual variation >0.59 Gg CO2/year) are mainly located in nonurban areas of the two megacities Beijing and Tianjin and also in the capital cities of each province. Urbanization has larger effects on the CO2 emissions of natural gas-fired boilers than of coal-fired boilers and combined heat and power (CHP). The average growth rate of CO2 emissions of gas-fired boilers in the urban areas of the study regions was approximately 4.7 times that of nonurban areas. The spatio-temporal heterogeneous impacts of urbanization on CO2 emissions should therefore be considered in future discussions of clean heating policies and climate response strategies.

Global source-receptor relationships for mercury deposition under present-day and 2050 emissions scenarios.

Global policies regulating anthropogenic mercury require an understanding of the relationship between emitted and deposited mercury on intercontinental scales. Here, we examine source-receptor relationships for present-day conditions and four 2050 IPCC scenarios encompassing a range of economic development and environmental regulation projections. We use the GEOS-Chem global model to track mercury from its point of emission through rapid cycling in surface ocean and land reservoirs to its accumulation in longer lived ocean and soil pools. Deposited mercury has a local component (emitted Hg(II), lifetime of 3.7 days against deposition) and a global component (emitted Hg(0), lifetime of 6 months against deposition). Fast recycling of deposited mercury through photoreduction of Hg(II) and re-emission of Hg(0) from surface reservoirs (ice, land, surface ocean) increases the effective lifetime of anthropogenic mercury to 9 months against loss to legacy reservoirs (soil pools and the subsurface ocean). This lifetime is still sufficiently short that source-receptor relationships have a strong hemispheric signature. Asian emissions are the largest source of anthropogenic deposition to all ocean basins, though there is also regional source influence from upwind continents. Current anthropogenic emissions account for only about one-third of mercury deposition to the global ocean with the remainder from natural and legacy sources. However, controls on anthropogenic emissions would have the added benefit of reducing the legacy mercury re-emitted to the atmosphere. Better understanding is needed of the time scales for transfer of mercury from active pools to stable geochemical reservoirs.

All-time releases of mercury to the atmosphere from human activities.

Understanding the biogeochemical cycling of mercury is critical for explaining the presence of mercury in remote regions of the world, such as the Arctic and the Himalayas, as well as local concentrations. While we have good knowledge of present-day fluxes of mercury to the atmosphere, we have little knowledge of what emission levels were like in the past. Here we develop a trend of anthropogenic emissions of mercury to the atmosphere from 1850 to 2008-for which relatively complete data are available-and supplement that trend with an estimate of anthropogenic emissions prior to 1850. Global mercury emissions peaked in 1890 at 2600 Mg yr(-1), fell to 700-800 Mg yr(-1) in the interwar years, then rose steadily after 1950 to present-day levels of 2000 Mg yr(-1). Our estimate for total mercury emissions from human activities over all time is 350 Gg, of which 39% was emitted before 1850 and 61% after 1850. Using an eight-compartment global box-model of mercury biogeochemical cycling, we show that these emission trends successfully reproduce present-day atmospheric enrichment in mercury.

TROPOMI NO2 in the United States: A Detailed Look at the Annual Averages, Weekly Cycles, Effects of Temperature, and Correlation With Surface NO2 Concentrations.

Observing the spatial heterogeneities of NO2 air pollution is an important first step in quantifying NOX emissions and exposures. This study investigates the capabilities of the Tropospheric Monitoring Instrument (TROPOMI) in observing the spatial and temporal patterns of NO2 pollution in the continental United States. The unprecedented sensitivity of the sensor can differentiate the fine-scale spatial heterogeneities in urban areas, such as emissions related to airport/shipping operations and high traffic, and the relatively small emission sources in rural areas, such as power plants and mining operations. We then examine NO2 columns by day-of-the-week and find that Saturday and Sunday concentrations are 16% and 24% lower respectively, than during weekdays. We also analyze the correlation of daily maximum 2-m temperatures and NO2 column amounts and find that NO2 is larger on the hottest days (>32°C) as compared to warm days (26°C-32°C), which is in contrast to a general decrease in NO2 with increasing temperature at moderate temperatures. Finally, we demonstrate that a linear regression fit of 2019 annual TROPOMI NO2 data to annual surface-level concentrations yields relatively strong correlation (R 2 = 0.66). These new developments make TROPOMI NO2 satellite data advantageous for policymakers and public health officials, who request information at high spatial resolution and short timescales, in order to assess, devise, and evaluate regulations.