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The TROPOspheric Monitoring Instrument (TROPOMI) is used to derive top-down NO X emissions for two large power plants and three megacities in North America. We first re-process the vertical column NO 2 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 NO X emissions agree to within 10% of the emissions reported by the power plants. We then derive top-down NO X emissions rates for New York City, Chicago, and Toronto, and compare them to projected bottom-up emissions inventories. In this analysis of 2018 NO X 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 NO X 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 NO X 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 NO X emissions from relatively small sources and for sub-seasonal timeframes.

The global and U.S. domestic effort to develop a clean energy economy and curb environmental pollution incentivizes the use of hydrogen as a transportation fuel, owing to its zero tailpipe pollutant emissions and high fuel efficiency in fuel cell electric vehicles (FCEVs). However, the hydrogen production process is not emissions free. Conventional hydrogen production via steam methane reforming (SMR) is energy intensive, coproduces carbon dioxide, and emits air pollutants. Thus, it is necessary to quantify the environmental impacts of SMR hydrogen production alongside the use-phase of FCEVs. This study fills the information gap, analyzing the greenhouse gas (GHG) and criteria air pollutant (CAP) emissions associated with hydrogen production in U.S. SMR facilities by compiling and matching the facility-reported GHG and CAP emissions data with facilities' hydrogen production data. The actual amounts of hydrogen produced at U.S. SMR facilities are often confidential. Thus, we have developed four approaches to estimate the hydrogen production amounts. The resultant GHG and CAP emissions per MJ of hydrogen produced in individual facilities were aggregated to develop emission values for both a national median and a California state median. This study also investigates the breakdown of facility emissions into combustion emissions and noncombustion emissions.

In Part II of this work we present the results of the downscaled offline Weather Research and Forecasting/Community Multiscale Air Quality (WRF/CMAQ) model, included in the "Technology Driver Model" (TDM) approach to future U.S. air quality projections (2046-2050) compared to a current-year period (2001-2005), and the interplay between future emission and climate changes. By 2046-2050, there are widespread decreases in future concentrations of carbon monoxide (CO), nitrogen oxides (NO x  = NO + NO 2 ), volatile organic compounds (VOCs), ammonia (NH 3 ), sulfur dioxide (SO 2 ), and particulate matter with an aerodynamic diameter ≤ 2.5 μm (PM 2.5 ) due mainly to decreasing on-road vehicle (ORV) emissions near urban centers as well as decreases in other transportation modes that include non-road engines (NRE). However, there are widespread increases in daily maximum 8-hr ozone (O 3 ) across the U.S., which are due to enhanced greenhouse gases (GHG) including methane (CH 4 ) and carbon dioxide (CO 2 ) under the Intergovernmental Panel on Climate Change (IPCC) A1B scenario, and isolated areas of larger reduction in transportation emissions of NO x compared to that of VOCs over regions with VOC-limited O 3 chemistry. Other notable future changes are reduced haze and improved visibility, increased primary organic to elemental carbon ratio, decreases in PM 2.5 and its species, decreases and increases in dry deposition of SO 2 and O 3 , respectively, and decreases in total nitrogen (TN) deposition. There is a tendency for transportation emission and CH 4 changes to dominate the increases in O 3 , while climate change may either enhance or mitigate these increases in the west or east U.S., respectively. Climate change also decreases PM 2.5 in the future. Other variable changes exhibit stronger susceptibility to either emission (e.g., CO, NO x , and TN deposition) or climate changes (e.g., VOC, NH 3 , SO 2 , and total sulfate deposition), which also have a strong dependence on season and specific U.S. regions., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Emissions from the transportation sector are rapidly changing worldwide; however, the interplay of such emission changes in the face of climate change are not as well understood. This two-part study examines the impact of projected emissions from the U.S. transportation sector (Part I) on ambient air quality in the face of climate change (Part II). In Part I of this study, we describe the methodology and results of a novel Technology Driver Model (see graphical abstract) that includes 1) transportation emission projections (including on-road vehicles, non-road engines, aircraft, rail, and ship) derived from a dynamic technology model that accounts for various technology and policy options under an IPCC emission scenario, and 2) the configuration/evaluation of a dynamically downscaled Weather Research and Forecasting/Community Multiscale Air Quality modeling system. By 2046-2050, the annual domain-average transportation emissions of carbon monoxide (CO), nitrogen oxides (NO x ), volatile organic compounds (VOCs), ammonia (NH 3 ), and sulfur dioxide (SO 2 ) are projected to decrease over the continental U.S. The decreases in gaseous emissions are mainly due to reduced emissions from on-road vehicles and non-road engines, which exhibit spatial and seasonal variations across the U.S. Although particulate matter (PM) emissions widely decrease, some areas in the U.S. experience relatively large increases due to increases in ship emissions. The on-road vehicle emissions dominate the emission changes for CO, NO x , VOC, and NH 3 , while emissions from both the on-road and non-road modes have strong contributions to PM and SO 2 emission changes. The evaluation of the baseline 2005 WRF simulation indicates that annual biases are close to or within the acceptable criteria for meteorological performance in the literature, and there is an overall good agreement in the 2005 CMAQ simulations of chemical variables against both surface and satellite observations., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

We estimate that a cumulative total of 1540 (1060-2800) Gg (gigagrams, 10 9 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.

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 (PM 2.5 ) 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 PM 2.5 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, PM 2.5 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 PM 2.5 pollution associated with international trade are greater than those associated with long-distance atmospheric pollutant transport.

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.

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.

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.

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.

High levels of sulfur dioxide (SO2) due to human activities pose a serious air pollution issue in China, especially in urban agglomerations. However, limited research has investigated the impact of anthropogenic emissions on higher SO2 concentrations in urban regions compared to rural areas in China. Here, we analyzed the trends in SO2 concentrations from 1980 to 2021 in China using the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) dataset. SO2 column concentrations from the Copernicus Atmosphere Monitoring Service (CAMS) and the Ozone Monitoring Instrument (OMI) during the years 2007–2021 were also examined for validation and comparison purposes. Eight representative areas, including four urban regions (Pearl River Delta [PRD], Beijing-Tianjin-Hebei [BTH], Yangtze River Delta [YRD], and Sichuan Basin [SCB]) and four rural regions (Northeast Region [NER], Mongolian Region [MR], West Region [WR], and Tibetan Plateau Region [TR]) were selected for the analysis. Overall, a significant but fluctuating increase in SO2 concentrations over China was observed during 1980–2021. During 1980–1997 and 2000–2010, there was an increase in SO2 concentration, while during 1997–2000 and 2010–2021, a decreasing trend was observed. The average increase in SO2 concentration was approximately 16 times higher in urban regions than in the rural background. We also found that SO2 dynamics were highly associated with expansion of urban areas, population density, and gross domestic product. Nonetheless, since 2007, SO2 concentrations have exhibited a downward trend, which is mainly attributed to the air pollution policies implemented by the Chinese government. Our findings highlight the need for further studies on the impact of SO2 on regional climate change in China. [ABSTRACT FROM AUTHOR]

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 (R2 = 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. Plain Language Summary: Nitrogen oxides are a group of air pollutants released after fossil fuel combustion. A constituent of nitrogen oxides, nitrogen dioxide (NO2), can be observed by satellite instruments due to its chemical properties. In this project, we average together images of NO2 pollution gathered by the Tropospheric Monitoring Instrument satellite instrument over the United States in order to better determine the spatial distribution of NO2 air pollution. We find that this newest satellite instrument can observe air pollution with unprecedented clarity, similar to how HDTV is an advancement over regular TV. For example, we quantify pollution near individual airports, shipping areas, and major interstates; previous satellite instruments were unable to quantify air pollution with this type of precision. We also average the satellite data over different intervals to better determine cycles of air pollution. We find that NO2 air pollution is 16% lower on Saturdays and 24% lower on Sundays. Additionally, we find that NO2 pollution is larger on the hottest summer days as compared to typical summer days. These developments demonstrate how this new satellite instrument can advantageous for policymakers and health officials, who request information at high spatial resolution and short timescales, in order to assess, devise, and evaluate regulations Key Points: The high instrument sensitivity of Tropospheric Monitoring Instrument (TROPOMI) can measure NO2 pollution with unprecedented clarity compared to predecessor instrumentsWe can now quantify pollution hotspots within cities such as those related to airport/shipping operations and high traffic areasAnnual column NO2 observed by TROPOMI has good correlation (R2 = 0.66) with EPA surface observations without any surface‐to‐column conversion [ABSTRACT FROM AUTHOR]

Taking CO 2 as tracer gas, and using numerical simulation, the law of indoor air pollutant concentration with the change of ventilation time was obtained. Using the standard κ-ε model and component transport model can simulate the ventilation process of diluting contaminants in a chamber. Through analyzing the results, it is found that the up-supply down-return ventilation does well in ventilation. [ABSTRACT FROM AUTHOR]

Light-duty battery electric vehicles (BEVs) can reduce both greenhouse gas (GHG) and criteria air pollutant (CAPs) emissions, when compared to gasoline vehicles. However, research has found that while today's BEVs typically reduce GHGs, they can increase certain CAPs, though with significant regional variability based on the electric grid mix. In addition, the environmental performance of electric and gasoline vehicles is not static, as key factors driving emissions have undergone significant changes recently and are expected to continue to evolve. In this study, we perform a cradle-to-grave life cycle analysis using state-level generation mix and vehicle operation emission data. We generated state-level emission factors using a projection from 2020 to 2050 for three light-duty vehicle types. We found that BEVs currently provide GHG benefits in nearly every state, with the median state's benefit being between approximately 50% to 60% lower than gasoline counterparts. However, gasoline vehicles currently have lower total NOx, urban NOx, total PM2.5, and urban PM2.5 in 33%; 15%; 70%; and 10% of states, respectively. BEV emissions will decrease in 2050 due to a cleaner grid, but the relative benefits when compared to gasoline vehicles do not change significantly, as gasoline vehicles are also improving over this time. [ABSTRACT FROM AUTHOR]