Abstract. Anthropogenic secondary organic aerosol (ASOA), formed from anthropogenic emissions of organic compounds, constitutes a substantial fraction of the mass of submicron aerosol in populated areas around the world and contributes to poor air quality and premature mortality. However, the precursor sources of ASOA are poorly understood, and there are large uncertainties in the health benefits that might accrue from reducing anthropogenic organic emissions. We show that the production of ASOA in 11 urban areas on three continents is strongly correlated with the reactivity of specific anthropogenic volatile organic compounds. The differences in ASOA production across different cities can be explained by differences in the emissions of aromatics and intermediate- and semi-volatile organic compounds, indicating the importance of controlling these ASOA precursors. With an improved model representation of ASOA driven by the observations, we attribute 340 000 PM2.5-related premature deaths per year to ASOA, which is over an order of magnitude higher than prior studies. A sensitivity case with a more recently proposed model for attributing mortality to PM2.5 (the Global Exposure Mortality Model) results in up to 900 000 deaths. A limitation of this study is the extrapolation from cities with detailed studies and regions where detailed emission inventories are available to other regions where uncertainties in emissions are larger. In addition to further development of institutional air quality management infrastructure, comprehensive air quality campaigns in the countries in South and Central America, Africa, South Asia, and the Middle East are needed for further progress in this area.
The objective of this study was to assess experimentally the potential impact of anthropogenic pH perturbation (ApHP) on concentrations of dimethyl sulfide (DMS) and dimethylsulfoniopropionate (DMSP), as well as processes governing the microbial cycling of sulfur compounds. A summer planktonic community from surface waters of the Lower St. Lawrence Estuary was monitored in microcosms over 12 days under three pCO2 targets: 1 × pCO2 (775 µatm), 2 × pCO2 (1,850 µatm), and 3 × pCO2 (2,700 µatm). A mixed phytoplankton bloom comprised of diatoms and unidentified flagellates developed over the course of the experiment. The magnitude and timing of biomass buildup, measured by chlorophyll a concentration, changed in the 3 × pCO2 treatment, reaching about half the peak chlorophyll a concentration measured in the 1 × pCO2 treatment, with a 2-day lag. Doubling and tripling the pCO2 resulted in a 15% and 40% decline in average concentrations of DMS compared to the control. Results from 35S-DMSPd uptake assays indicated that neither concentrations nor microbial scavenging efficiency of dissolved DMSP was affected by increased pCO2. However, our results show a reduction of the mean microbial yield of DMS by 34% and 61% in the 2 × pCO2 and 3 × pCO2 treatments, respectively. DMS concentrations correlated positively with microbial yields of DMS (Spearman’s ρ = 0.65; P < 0.001), suggesting that the impact of ApHP on concentrations of DMS in diatom-dominated systems may be strongly linked with alterations of the microbial breakdown of dissolved DMSP. Findings from this study provide further empirical evidence of the sensitivity of the microbial DMSP switch under ApHP. Because even small modifications in microbial regulatory mechanisms of DMSP can elicit changes in atmospheric chemistry via dampened efflux of DMS, results from this study may contribute to a better comprehension of Earth’s future climate.
Amazonian deforestation from slash‐and‐burn practices is a significant contributor to biomass burning within Brazil. Fires emit carbonaceous aerosols that negatively impact human health by increasing fine particulate matter (PM2.5) exposure. These negative effects on health compound the already detrimental climatological and ecological impacts. Despite high biomass burning emissions in Brazil and the international attention drawn by the relaxation of Amazon protections in 2019, little is known about the health impacts from PM2.5 exposure attributable to these fires. We estimate PM2.5‐related premature deaths in Brazil associated with biomass burning, focusing on temporal, interannual, and spatial trends. We find that during the fire season of 2019, 4,966 (2,427, 8,340) premature deaths were attributable to fire emissions making up 10% (5, 17) of all PM2.5‐related premature deaths in Brazil. Between the 2019 and 2018 seasons, fire emissions increased by 1.37 Tg (1.00, 2.18) or 115% (60, 201), which was responsible for an increase in health impacts of 2,109 (965, 3,623) premature deaths or 74% (54, 98). Biomass burning emissions throughout Brazil contribute significantly to premature deaths, with the largest burning events occurring in northwestern Brazil. The impact of fires on PM2.5‐related premature deaths is highest in heavily populated regions despite their fires being 1 to 2 orders of magnitude smaller than the largest burning events. Results from this study characterize the extent to which elevated PM2.5 exposure levels owing to fires affect public health in Brazil and present an additional, public health‐focused, support for increased Amazon protections.
In situ measurements have suggested vehicle emissions may dominate agricultural sources of NH 3 in many cities, which is alarming given the potential for urban NH 3 to significantly increase human exposure to ambient particulate matter. However, confirmation of the prevalence of vehicle NH 3 throughout a city has been challenging because of mixing with agricultural sources, and the latter are thus routinely assumed to dominate.Here we report vehicle NH 3 emissions based on TROPOMI NO 2 and CrIS NH 3 (0.152 kg s −1 ) that are consistent with a model-based estimate (0.178 kg s −1 ) and show that COVID-19 lockdowns provide a unique opportunity for making the first satellite-based constraints on vehicle NH 3 emissions for an entire urban region (western Los Angeles), which we find make up 60−95% of total NH 3 emissions, substantially higher than the values of 13−22% in state and national inventories. This provides a new means of constraining a component of transportation emissions whose impacts may rival those of NO x yet which has been largely under-recognized and uncontrolled.
Exposure to air pollution is a leading risk factor for premature death globally; however, the complexity of its formation and the diversity of its sources can make it difficult to address. The Group of Twenty (G20) countries are a collection of the world's largest and most influential economies and are uniquely poised to take action to reduce the global health burden associated with air pollution. We present a framework capable of simultaneously identifying regional and sectoral sources of the health impacts associated with two air pollutants, fine particulate matter (PM 2.5 ) and ozone (O 3 ) in G20 countries; this framework is also used to assess the health impacts associated with emission reductions. This approach combines GEOS‐Chem adjoint sensitivities, satellite‐derived data, and a new framework designed to better characterize the non‐linear relationship between O 3 exposures and nitrogen oxides emissions. From this approach, we estimate that a 50% reduction of land transportation emissions by 2040 would result in 251 thousand premature deaths avoided in G20 countries. These premature deaths would be attributable equally to reductions in PM 2.5 and O 3 exposure which make up 51% and 49% of the potential benefits, respectively. In our second application, we estimate that the energy generation related co‐benefits associated with G20 countries staying on pace with their net‐zero carbon dioxide targets would be 290 thousand premature deaths avoided in 2040; action by India (47%) would result in the most benefits of any country and a majority of these avoided deaths would be attributable to reductions in PM 2.5 exposure (68%).
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