Abstract. As a major alkaline gas in the atmosphere, NH3 significantly impacts atmospheric chemistry, ecological environment, and biodiversity. Gridded NH3 emission inventories can significantly affect the accuracy of model concentrations and play a crucial role in the refinement of mitigation strategies. However, several uncertainties are still associated with existing NH3 emission inventories in China. Therefore, in this study, we focused on improving fertilizer-application-related NH3 emission inventories. We comprehensively evaluated the dates and times of fertilizer application to the major crops that are cultivated in China, improved the spatial allocation methods for NH3 emissions from croplands with different rice types, and established a gridded NH3 emission inventory for mainland China with a resolution of 5 min × 5 min in 2016. The results showed that the atmospheric NH3 emissions in mainland China amounted to 12.11 Tg, with livestock waste (44.8 %) and fertilizer application (38.6 %) being the two main NH3 emission sources in China. Obvious spatial variability in NH3 emissions was also identified, and high emissions were predominantly concentrated in North China. Further, NH3 emissions tended to be high in summer and low in winter, and the ratio for the July–January period was 3.08. Furthermore, maize and rice fertilization in summer was primarily responsible for the increase in NH3 emissions in China, and the evaluation of the spatial and temporal accuracy of the NH3 emission inventory established in this study using the WRF-Chem and ground-station- and satellite-based observations showed that it was more accurate than other inventories.

We developed a regional atmospheric transport model for microplastics (MPs, 10 μm to 5 mm in size) over Asia and the adjacent Pacific and Indian oceans, accounting for MPs’ size- and shape-dependent aerodynamics. The model was driven by tuned atmospheric emissions of MPs from the land and the ocean, and the simulations were evaluated against coastal ( n = 19) and marine ( n = 56) observations. Our tuned atmospheric emissions of MPs from Asia and the adjacent oceans were 310 Gg y –1 (1 Gg = 1 kton) and 60 Gg y –1 , respectively. MP lines and fragments may be transported in the atmosphere >1000 km; MP pellets in our model mostly deposited near-source. We estimated that 1.4% of the MP mass emitted into the Asian atmosphere deposited into the oceans via atmospheric transport; the rest deposited over land. The resulting net atmospheric transported MP flux from Asia into the oceans was 3.9 Gg y –1 , twice as large as a previous estimate for the riverine-transported MP flux from Asia into the oceans. The uncertainty of our simulated atmospheric MP budget was between factors of 3 and 7. Our work highlighted the impacts of the size and morphology on the aerodynamics of MPs and the importance of atmospheric transport in the source-to-sink relationship of global MP pollution.

Abstract. Last spring, super dust storms reappeared in East Asia after being absent for one and a half decades. The event caused enormous losses in both Mongolia and China. Accurate simulation of such super sandstorms is valuable for the quantification of health damage, aviation risks, and profound impacts on the Earth system, but also to reveal the climatic driving force and the process of desertification. However, accurate simulation of dust life cycles is challenging, mainly due to imperfect knowledge of emissions. In this study, the emissions that lead to the 2021 spring dust storms are estimated through assimilation of MODIS AOD and ground-based PM10 concentration data simultaneously. With this, the dust concentrations during these super storms could be reproduced and validated with concentration observations. The multi-observation assimilation is also compared against emission inversion that assimilates AOD or PM10 concentration measurements alone, and the added values are analyzed. The emission inversion results reveal that wind-blown dust emissions originated from both China and Mongolia during spring 2021. Specifically, 19.9×106 and 37.5×106 t of particles were released in the Chinese and Mongolian Gobi, respectively, during these severe dust events. By source apportionment it was revealed that the Mongolian Gobi poses more severe threats to the densely populated regions of the Fenwei Plain (FWP) and the North China Plain (NCP) located in northern China than does the Chinese Gobi. It was estimated that 63 % of the dust deposited in FWP was due to transnational transport from Mongolia. For NCP, the long-distance transport dust from Mongolia contributes about 69 % to the dust deposition.

Abstract. A large population in China has been exposed to both severe ozone (O3) pollution and extreme heat under global warming. Here, the spatiotemporal characteristics of coupled extremes in surface O3 and heat (OPCs) over China are investigated using surface observations, a process-based chemical transport model (GEOS-Chem), and multi-model simulations from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). North China Plain (NCP; 37–41∘ N; 114–120∘ E) is identified as a hot spot of OPCs, where more than half of the O3 pollution days are accompanied by high temperature extremes. OPCs over NCP exceeded 40 d during 2014–2019, exhibiting an increasing trend. Both O3 concentrations and temperatures are elevated during OPCs compared with O3 pollution days occurring individually (OPIs). Therefore, OPCs impose more severe health impacts to humans than OPIs, but the stronger health effects are mainly driven by the higher temperatures. GEOS-Chem simulations further reveal that enhanced chemical production resulting from hot and stable atmospheric conditions under anomalous weather patterns primarily contributes to the exacerbated O3 levels during OPCs. In the future, CMIP6 projections suggest increased occurrences of OPCs over NCP in the middle of this century, but by the end of this century, OPCs may decrease or increase depending on the pollutant emission scenarios. However, for all future scenarios, extreme high temperatures will play an increasingly important role in modulating O3 pollution in a warming climate.

Abstract. The co-polluted days by ozone (O3) and PM2.5 (particulate matter with an aerodynamic equivalent diameter of 2.5 µm or less) (O3–PM2.5PDs) were frequently observed in the Beijing–Tianjin–Hebei (BTH) region in warm seasons (April–October) of 2013–2020. We applied the 3-D global chemical transport model (GEOS-Chem) to investigate the chemical and physical characteristics of O3–PM2.5PDs by composited analyses of such days that were captured by both the observations and the model. Model results showed that, when O3–PM2.5PDs occurred, the concentrations of hydroxyl radical and total oxidant, sulfur oxidation ratio, and nitrogen oxidation ratio were all high, and the concentrations of sulfate at the surface were the highest among all pollution types. We also found unique features in vertical distributions of aerosols during O3–PM2.5PDs; concentrations of PM2.5 decreased with altitude near the surface but remained stable at 975–819 hPa. Process analyses showed that secondary aerosols (nitrate, ammonium, and sulfate) had strong chemical productions at 913–819 hPa, which were then transported downward, resulting in the quite uniform vertical profiles at 975–819 hPa on O3–PM2.5PDs. The weather patterns for O3–PM2.5PDs were characterized by anomalous high-pressure system at 500 hPa as well as strong southerlies and high RH at 850 hPa. The latter resulted in the strong chemical productions around 850 hPa on O3–PM2.5PDs. The physical and chemical characteristics of O3–PM2.5PDs are quite different from those of polluted days by either O3 alone or PM2.5 alone and have important implications for air quality management.