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Air quality in China has continuously improved during the Three-Year Action Plan (2018-2020); however, the changes in aerosol composition, properties, and sources in Beijing summer remain poorly understood. Here, we conducted real-time measurements of aerosol composition in five summers from 2018 to 2022 along with WRF-Community Multiscale Air Quality simulations to characterize the changes in aerosol chemistry and the roles of meteorology and emission reductions. Largely different from winter, secondary inorganic aerosol and photochemical-related secondary organic aerosol (SOA) showed significant decreases by 55-67% in summer, and the most decreases occurred in 2021. Comparatively, the decreases in the primary aerosol species and gaseous precursors were comparably small. While decreased atmospheric oxidation capacity as indicated by ozone changes played an important role in changing SOA composition, the large decrease in aerosol liquid water and small increase in particle acidity were critical for nitrate changes by decreasing gas-particle partitioning substantially (∼28%). Analysis of meteorological influences demonstrated clear and similar transitions in aerosol composition and formation mechanisms at a relative humidity of 50-60% in five summers. Model simulations revealed that emission controls played the decisive role in reducing sulfate, primary OA, and anthropogenic SOA during the Three-Year Action Plan, while meteorology affected more nitrate and biogenic SOA.

Hydroxymethanesulfonate (HMS), a key marker species of aqueous-phase processing, plays a significant role in sulfur budget in atmosphere. Here we have a comprehensive characterization of HMS at urban and rural sites in North China Plain (NCP) by using the real-time measurements from a high-resolution aerosol mass spectrometer (AMS) and a single-particle AMS together with offline filter analysis. Our results showed much higher winter concentration of HMS at the rural site (average±1σ: 2.58 ± 2.56 μg m -3 ) than that (1.70 ± 2.68 μg m -3 ) in Beijing due to the more frequent fog events, low particle acidity and high concentration of precursors. The HMS on average contributed 6.3% and 5.2% to organic aerosol (OA), and 16% and 12% to the total particulate sulfur, at the rural and urban sites, respectively. HMS was highly correlated with aqueous-phase secondary OA and sulfate, and its contribution to the total particulate sulfur increased significantly as a function of relative humidity demonstrating the effective HMS production from aqueous-phase processing. Single-particle analysis showed that HMS-containing particles were mainly mixed with amine-related compounds. In addition, we found that organosulfur compounds (OS) estimated from sulfur-containing fragments of AMS correlated well with HMS at both urban and rural sites. While OS at the rural site was dominated by HMS, other types of OS were also important in urban area. The high HMS also affected the estimation of particle acidity using the AMS measured and predicted ammonium, particularly during severe haze episodes. Overall, our results demonstrated the importance of HMS in winter in NCP, and it could be more important in total particulate sulfur budget as the continuous decrease in sulfate in the future., (Copyright © 2022 Elsevier Inc. All rights reserved.)

The Fenwei Plain (FWP) continues to be one of the most polluted regions in China despite the improvement of air quality in recent years. However, our understanding of aerosol optical properties (AOP) and its relationship with aerosol composition particularly in cold season is far from complete. Here we conducted three-month measurements of AOP from November 2020 to January 2021 in the FWP along with fine particle composition and water-soluble organic aerosol (WSOA) measurements. Our results showed rapid transitions in AOP from November to January due to the enhanced primary emissions and the decreased aqueous-phase processing. The single scattering albedo (SSA) decreased from 0.85 to 0.78, while the absorption Ångstrӧm exponent (AAE) increased from 1.41 to 1.60, demonstrating the increasing role of absorbing aerosol and brown carbon in cold season. Further analysis showed that SSA increased significantly with the fraction of secondary inorganic aerosol, while AAE was highly correlated with the fraction of primary OA (POA), highlighting the different impacts of primary and secondary aerosol on AOP. Chemical apportionment showed the dominant contributions of ammonium nitrate (29%) and ammonium sulfate (27%) to particle extinction before heating season, while that of POA increased to 27% during heating season. Although the pollution level showed a clear increase during the heating season, the changes in visibility were small due to the decreased mass extinction efficiency from 3.48 to 2.91 m 2 g -1 . Positive matrix factorization illustrated a clear transition in WSOA composition from the dominance of secondary OA (SOA) in November to POA in heating season. Compared with the large decrease in water-soluble aqueous-phase SOA, the consistently high concentration of photochemical-related SOA elucidated the presence of strong photochemical processing in cold season. Overall, our results demonstrate the significant transition in primary emissions and secondary formation in cold season, and such changes have affected AOP substantially., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Air quality in Beijing has been improved significantly in recent years; however, our knowledge of the vertically resolved aerosol chemistry in summer remains poor. Here, we carried out comprehensive measurements of aerosol composition, gaseous species, and aerosol optical properties on a meteorological tower in Beijing in summer and compared with those measured in winter. Our results showed that aerosol liquid water (ALW) contributing approximately 50% of the total mass with higher values aloft played a crucial role in aerosol formation. Particularly, the higher nitrate concentration in city aloft than at the ground level during daytime was mainly due to the enhanced gas-particle partitioning driven by ALW and particle acidity. The vertical profiles of organic aerosol (OA) factors varied more differently in the urban boundary layer. Although the ubiquitous decreases in primary OA with the increase in height were mainly due to the influences of local emissions and vertical convection, the vertical differences in oxygenated OA between summer and winter may be related to the photochemical processing of different biogenic and anthropogenic volatile organic compounds. The single-scattering albedo, brown carbon, and absorption Ångstrom exponent of aerosol particles also presented different vertical profiles between day and night due to the vertical changes in aerosol chemistry.

Most of human exposure to atmospheric pollutants occurs indoors, and the components of outdoor aerosols may have been changed in the way before reaching indoor spaces. Here we conducted real-time online measurements of mass concentrations and chemical composition of black carbon and the non-refractory species in PM 2.5 in an occupied office for approximately one month. The open-close windows and controlled dampness experiments were also performed. Our results show that indoor aerosol species primarily originate from outdoors with indoor/outdoor ratio of these species typically less than unity except for certain organic aerosol (OA) factors. All aerosol species went through filtration upon transport indoors. Ammonium nitrate and fossil fuel OA underwent evaporation or particle-to-gas partitioning, while less oxidized secondary OA (SOA) underwent secondary formation and cooking OA might have indoor sources. With higher particulate matter (PM) mass concentration outdoors than in the office, elevated natural ventilation increased PM exposure indoors and this increased exposure was prolonged when outdoor PM was scavenged. We found that increasing humidity in the office led to higher indoor PM mass concentration particularly more oxidized SOA. Overall, our results highlight that indoor exposure of occupants is substantially different from outdoor in terms of mass concentrations and chemical species., (© 2021 John Wiley & Sons A/S. Published by John Wiley & Sons Ltd.)

Extensive studies on aerosol chemistry have been carried out in megacities in China, however, aerosol characterization in Central China Plain (CCP) is limited. Here we conducted real-time measurements of fine particle composition with a time-of-flight aerosol chemical speciation monitor in Kaifeng, Henan province in October 2019. Our results showed that nitrate and organics constituted the major fraction of non-refractory PM 2.5 for the entire study, on average accounting for 34% and 33%, respectively. However, aerosol composition was substantially different among four periods due to different meteorological conditions and chemical processing. For instance, nitrate presented the lowest contribution during the first period due to evaporative loss associated with high temperature (T), and then rapidly increased during polluted periods as a function of relative humidity (RH). Positive matrix factorization analysis showed the dominance of secondary organic aerosol (SOA) in OA, and also the changes in OA composition under different T and RH levels. In addition, this study is unique with two periods of local emission controls. Back trajectory and coefficient of divergence analysis showed that air pollution in CCP was overall homogeneously distributed. As a result, the effectiveness of local emission controls in this region was strongly affected by meteorological conditions and regional transport. We found that one of the periods with emission control even showed the highest concentrations for the entire study. Our results point towards the limited effect of local emission controls in mitigating air pollution in CCP, and highlight the importance of joint emission controls under unfavorable meteorological conditions., (Copyright © 2020. Published by Elsevier B.V.)

Severe haze episodes in cold season in Beijing have been mitigated greatly during the last decade. However, the changes in aerosol chemistry as responses to the large reductions in gaseous precursors during the two phases of clean air action, i.e., phase Ⅰ (2013-2017) and phase Ⅱ (2018-2020), are less understood. Here we characterized such changes in cold season (January-March) by using five-year real-time aerosol particle composition measurements. Our results showed consistently large reductions for all chemical species from 2013 to 2020 with the largest decreases being chloride (95%) and organics (74%) followed by sulfate (69%), while the decreases in nitrate were comparatively small (44%). However, the contributions of sulfate were fairly stable despite the increased nitrate contributions from 18% in 2013 to 30% in 2020. Organic aerosol (OA) composition also changed significantly since 2018 with large increases in the contributions of secondary OA and corresponding decreases in primary OA from fossil fuel combustion and cooking emissions. The changes in aerosol chemistry were closely related to the different reductions in gaseous precursors, e.g., SO 2 vs. NO 2 , and the enhanced secondary processes, e.g., the increases in O 3 , sulfur and nitrogen oxidation efficiency. Further, we found that the changes in aerosol chemistry in cold season during the phase Ⅱ of clean air action (2018-2020) started to slow down with relatively small changes in PM 2.5 and secondary inorganic species. Our results point towards a future challenge in mitigating air pollution in cold season, and the need of more stringent and scientific strategies to control secondary aerosol pollution in an environment with enhanced oxidation capacity and high precursors., Competing Interests: Declaration of competing interest The authors declare that they have no conflict of interest., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

The rapidly spread coronavirus disease (COVID-19) has limited people's outdoor activities and hence caused substantial reductions in anthropogenic emissions around the world. However, the air quality in some megacities has not been improved as expected due to the complex responses of aerosol chemistry to the changes in precursors and meteorology. Here we demonstrate the responses of primary and secondary aerosol species to the changes in anthropogenic emissions during the COVID-19 outbreak in Beijing, China along with the Chinese New Year (CNY) holiday effects on air pollution by using six-year aerosol particle composition measurements. Our results showed large reductions in primary aerosol species associated with traffic, cooking and coal combustion emissions by 30-50% on average during the CNY, while the decreases in secondary aerosol species were much small (5-12%). These results point towards a future challenge in mitigating secondary air pollution because the reduced gaseous precursors may not suppress secondary aerosol formation efficiently under stagnant meteorological conditions. By analyzing the long-term measurements from 2012 to 2020, we found considerable increases in the ratios of nitrate to sulfate, secondary to primary OA, and sulfur and nitrogen oxidation capacity despite the overall decreasing trends in mass concentrations of most aerosol species, suggesting that the decreases in anthropogenic emissions have facilitated secondary formation processes during the last decade. Therefore, a better understanding of the mechanisms driving the chemical responses of secondary aerosol to the changes in anthropogenic emissions under complex meteorological environment is essential for future mitigation of air pollution in China., Competing Interests: Declaration of competing interest The authors declare no competing financial interest., (Copyright © 2020 Elsevier B.V. All rights reserved.)

Black carbon (BC) exerts a large impact on climate radiative forcing and public health, and such impacts depend strongly on chemical composition and mixing state. Here a single particle aerosol mass spectrometry (SPA-MS) along with an aerosol chemical speciation monitor was employed to characterize the composition and mixing state of BC-containing particles in summer and winter in Beijing. Approximately 2 million BC-containing particles were chemically analyzed, and the particles were classified into nine and eight different types in summer and winter, respectively, according to mass spectral signatures and composition. The BC-containing particles in summer were dominated by the type of nitrate-related BC (BC-N, 56.7%), while in winter the BC mixed with organic carbon (OC) and sulfate (BCOC-S), and OC and nitrate (BCOC-N) were two dominant types accounting for 44.9% and 16.6%, respectively. The number fractions of BC-N in summer, and BCOC-N and BC-SN in winter increased largely during periods with severe air pollution, suggesting the enhanced secondary formation on BC-containing particles. We also found that the primary emissions of the biomass burning and coal combustion can affect BC mixing state substaintially as indicated by the considerable fraction of BC mixed with levoglucosan and polycyclic aromatic hydrocarbons in winter. Bivariate polar plots and back trajectory analysis indicated that the sulfate-associated BC-containing particles were mostly from regional transport while the nitrate-related type was more from local production. The optical parameter of absorbing Ångström exponents (AAE) of BC was 1.2 and 1.5 in summer and winter, respectively, and the AAE dependence of BC mixing state was also different in the two seasons. While higher fractions of BC-N were observed during lower AAE periods in summer, the variations of dominant OC-related BC-containing particles in winter were fairly stable as a function of AAE., Competing Interests: Declaration of competing interest The authors declare that they have no conflict of interest., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Unexpectedly frequent severe haze episodes were observed in Beijing during February–March in 2021 after two phases of clean air action plan (2013–2020), yet the causes remained unclear. Here, we conducted real‐time fine particle (PM2.5) composition measurements during January–March in 2021 using a time‐of‐flight aerosol chemical speciation monitor and an aethalometer and compared with those during the coronavirus disease (COVID‐19) period in 2020. Our results showed ubiquitously elevated concentrations of chloride, black carbon (BC), and primary organic aerosol (POA) in 2021, suggesting increased primary emissions during the post‐COVID‐19 period. By using the machine learning‐based random forest (RF) algorithm, we found largely different responses of aerosol changes to meteorology in different months. After decoupling the effects of meteorology, the PM2.5 changes from 2020 to 2021 were reduced from −35.6% to −29.0% in January, −24.1% to −4.5% in February, and +92.6% to +34.2% in March, respectively. Our results demonstrate the dominant roles of stagnant meteorology and secondary production in the formation of severe haze episodes in March 2021. In particular, we found that the compositions of observed and deweathered PM2.5 were fairly similar between 2020 and 2021, and the ratios of secondary OA to secondary inorganic aerosols were close. Our study indicates that decoupling the influence of meteorological conditions is of great importance for better evaluation of mitigating strategies of air pollution due to the large impact of meteorology on the changes in PM2.5 species particularly in a short period. Key Points: Unexpectedly severely haze episodes were observed in March 2021 in BeijingClear increases in primary emissions during the post‐COVID‐19 period in BeijingLargely different responses of aerosol species to meteorology in different months [ABSTRACT FROM AUTHOR]

Air quality in China has been continuously improved since clean air action in 2013, yet the visibility was not improved simultaneously. Here we employed a new method by integrating highly time-resolved aerosol compositions with particle light extinction (b ext) into positive matrix factorization to quantify the different contributors to visibility degradation during four seasons in Beijing. Our results show that ammonium nitrate-related factor contributed dominantly to b ext during all seasons (31–48%) and played more significant roles during low-visibility periods. Secondary organic aerosol (SOA) was an important contributor of b ext (27–35%) in autumn and spring while primary OA related sources were more important in winter (37%). An increase in aerosol mass extinction efficiency and similarly important roles of ammonium nitrate and SOA in visibility degradation were also observed during the COVID-19 lockdown period. Our results point towards a future challenge in improving visibility in China due to the increased contributions of nitrate and SOA in PM 2.5. Future emission controls with a priority to decrease nitrate would benefit both air quality and visibility. [Display omitted] • A new method to quantify the source contributions to particle light extinction. • Dominant contributions of ammonium nitrate and SOA to light extinction in Beijing. • Increased aerosol mass extinction efficiency during the COVID-19 period. [ABSTRACT FROM AUTHOR]