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1. Long-term trends of impacts of global gasoline and diesel emissions on ambient PM _2.5 and O ₃ pollution and the related health burden for 2000–2015

   https://doi.org/10.1088/1748-9326/ac9422  

   Xiong, Ying; Partha, Debatosh; Prime, Noah; Smith, Steven J.; Mariscal, Noribeth; Salah, Halima; Huang, Yaoxian (October 2022, Environmental Research Letters)

   Abstract Global economic development and urbanization during the past two decades have driven the increases in demand of personal and commercial vehicle fleets, especially in developing countries, which has likely resulted in changes in year-to-year vehicle tailpipe emissions associated with aerosols and trace gases. However, long-term trends of impacts of global gasoline and diesel emissions on air quality and human health are not clear. In this study, we employ the Community Earth System Model in conjunction with the newly developed Community Emissions Data System as anthropogenic emission inventory to quantify the long-term trends of impacts of global gasoline and diesel emissions on ambient air quality and human health for the period of 2000–2015. Global gasoline and diesel emissions contributed to regional increases in annual mean surface PM_2.5(particulate matter with aerodynamic diameters ⩽2.5μm) concentrations by up to 17.5 and 13.7µg m⁻³, and surface ozone (O₃) concentrations by up to 7.1 and 7.2 ppbv, respectively, for 2000–2015. However, we also found substantial declines of surface PM_2.5and O₃concentrations over Europe, the US, Canada, and China for the same period, which suggested the co-benefits of air quality and human health from improving gasoline and diesel fuel quality and tightening vehicle emissions standards. Globally, we estimate the mean annual total PM_2.5- and O₃-induced premature deaths are 139 700–170 700 for gasoline and 205 200–309 300 for diesel, with the corresponding years of life lost of 2.74–3.47 and 4.56–6.52 million years, respectively. Diesel and gasoline emissions create health-effect disparities between the developed and developing countries, which are likely to aggravate afterwards. 

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2. Secondary Organic Aerosol Formation via Multiphase Reaction of Hydrocarbons in Urban Atmosphere Using the CAMx Model Integrated with the UNIPAR model

   https://doi.org/10.5194/acp-2021-1002  

   Yu, Z.; Jang, M.; Kim, S.; Son, K.; Madhu, A.; Han, S.; Park, J. (January 2022, Atmospheric chemistry and physics)

   The prediction of Secondary Organic Aerosol (SOA) in regional scales is traditionally performed by using gas-particle partitioning models. In the presence of inorganic salted wet aerosols, aqueous reactions of semivolatile organic compounds can also significantly contribute to SOA formation. The UNIfied Partitioning-Aerosol phase Reaction (UNIPAR) model utilizes the explicit gas mechanism to better predict SOA formation from multiphase reactions of hydrocarbons. In this work, the UNIPAR model was incorporated with the Comprehensive Air Quality Model with Extensions (CAMx) to predict the ambient concentration of organic matter (OM) in urban atmospheres during the Korean-United States Air Quality (2016 KORUS-AQ) campaign. The SOA mass predicted with the CAMx-UNIPAR model changed with varying levels of humidity and emissions and in turn, has the potential to improve the accuracy of OM simulations. The CAMx-UNIPAR model significantly improved the simulation of SOA formation under the wet condition, which often occurred during the KORUS-AQ campaign, through the consideration of aqueous reactions of reactive organic species and gas-aqueous partitioning. The contribution of aromatic SOA to total OM was significant during the low-level transport/haze period (24-31 May 2016) because aromatic oxygenated products are hydrophilic and reactive in aqueous aerosols. The OM mass predicted with the CAMx-UNIPAR model was compared with that predicted with the CAMx model integrated with the conventional two product model (SOAP). Based on estimated statistical parameters to predict OM mass, the performance of CAMx-UNIPAR was noticeably better than the conventional CAMx model although both SOA models underestimated OM compared to observed values, possibly due to missing precursor hydrocarbons such as sesquiterpenes, alkanes, and intermediate VOCs. The CAMx-UNIPAR model simulation suggested that in the urban areas of South Korea, terpene and anthropogenic emissions significantly contribute to SOA formation while isoprene SOA minimally impacts SOA formation. 

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3. Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO₂ emission controls

   https://doi.org/10.5194/acp-16-1603-2016  

   Marais, E. A.; Jacob, D. J.; Jimenez, J. L.; Campuzano-Jost, P.; Day, D. A.; Hu, W.; Krechmer, J.; Zhu, L.; Kim, P. S.; Miller, C. C.; et al (January 2016, Atmospheric Chemistry and Physics)

   Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA), but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (γ) for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC⁴RS) and ground-based (SOAS) observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NO_x  ≡  NO + NO₂) over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO₂) react significantly with both NO (high-NO_x pathway) and HO₂ (low-NO_x pathway), leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA) and formaldehyde (a product of isoprene oxidation). Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58 % of isoprene SOA) from the low-NO_x pathway and glyoxal (28 %) from both low- and high-NO_x pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC⁴RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NO_x emissions decrease (favoring the low-NO_x pathway for isoprene oxidation), but decrease more strongly as SO₂ emissions decrease (due to the effect of sulfate on aerosol acidity and volume). The US Environmental Protection Agency (EPA) projects 2013–2025 decreases in anthropogenic emissions of 34 % for NO_x (leading to a 7 % increase in isoprene SOA) and 48 % for SO₂ (35 % decrease in isoprene SOA). Reducing SO₂ emissions decreases sulfate and isoprene SOA by a similar magnitude, representing a factor of 2 co-benefit for PM_2.5 from SO₂ emission controls. 

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4. Heterogeneous Nitrate Production Mechanisms in Intense Haze Events in the North China Plain

   https://doi.org/10.1029/2021JD034688  

   Chan, Yuk‐Chun; Evans, Mathew J.; He, Pengzhen; Holmes, Christopher D.; Jaeglé, Lyatt; Kasibhatla, Prasad; Liu, Xue‐Yan; Sherwen, Tomás; Thornton, Joel A.; Wang, Xuan; et al (May 2021, Journal of Geophysical Research: Atmospheres)

   Abstract Studies of wintertime air quality in the North China Plain (NCP) show that particulate‐nitrate pollution persists despite rapid reduction in NO_xemissions. This intriguing NO_x‐nitrate relationship may originate from non‐linear nitrate‐formation chemistry, but it is unclear which feedback mechanisms dominate in NCP. In this study, we re‐interpret the wintertime observations of¹⁷O excess of nitrate (∆¹⁷O(NO₃⁻)) in Beijing using the GEOS‐Chem (GC) chemical transport model to estimate the importance of various nitrate‐production pathways and how their contributions change with the intensity of haze events. We also analyze the relationships between other metrics of NO_ychemistry and [PM_2.5] in observations and model simulations. We find that the model on average has a negative bias of −0.9‰ and −36% for ∆¹⁷O(NO₃⁻) and [O_x,major] (≡ [O₃] + [NO₂] + [p‐NO₃⁻]), respectively, while overestimating the nitrogen oxidation ratio ([NO₃⁻]/([NO₃⁻] + [NO₂])) by +0.12 in intense haze. The discrepancies become larger in more intense haze. We attribute the model biases to an overestimate of NO₂‐uptake on aerosols and an underestimate in wintertime O₃concentrations. Our findings highlight a need to address uncertainties related to heterogeneous chemistry of NO₂in air‐quality models. The combined assessment of observations and model results suggest that N₂O₅uptake in aerosols and clouds is the dominant nitrate‐production pathway in wintertime Beijing, but its rate is limited by ozone under high‐NO_x‐high‐PM_2.5conditions. Nitrate production rates may continue to increase as long as [O₃] increases despite reduction in [NO_x], creating a negative feedback that reduces the effectiveness of air pollution mitigation. 

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5. Disproportionately large impacts of wildland-urban interface fire emissions on global air quality and human health

   https://doi.org/10.1126/sciadv.adr2616  

   Tang, Wenfu; Emmons, Louisa K; Wiedinmyer, Christine; Partha, Debatosh B; Huang, Yaoxian; He, Cenlin; Zhang, Junzhe; Barsanti, Kelley C; Gaubert, Benjamin; Jo, Duseong S; et al (March 2025, Science Advances)

   Fires in the wildland-urban interface (WUI) are a global issue with growing importance. However, the impact of WUI fires on air quality and health is less understood compared to that of fires in wildland. We analyze WUI fire impacts on air quality and health at the global scale using a multi-scale atmospheric chemistry model—the Multi-Scale Infrastructure for Chemistry and Aerosols model (MUSICA). WUI fires have notable impacts on key air pollutants [e.g., carbon monoxide (CO), nitrogen dioxide (NO₂), fine particulate matter (PM_2.5), and ozone (O₃)]. The health impact of WUI fire emission is disproportionately large compared to wildland fires primarily because WUI fires are closer to human settlement. Globally, the fraction of WUI fire–caused annual premature deaths (APDs) to all fire–caused APDs is about three times of the fraction of WUI fire emissions to all fire emissions. The developed model framework can be applied to address critical needs in understanding and mitigating WUI fires and their impacts. 

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