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Formaldehyde (HCHO) is an important source for driving tropospheric ozone (O 3 ) formation. This study investigated the combined effects of anthropogenic and biogenic emission on O 3 formation in the Guanzhong Basin (GZB), Central China, providing useful information into the mechanisms of O 3 formation due to the interaction between anthropogenic and biogenic volatile organic compounds (VOCs). A severe O 3 pollution episode in summer of 2017 was simulated using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to examine the impacts of ambient HCHO on ground-level O 3 . Results showed secondary HCHO dominated ambient levels, peaking in the afternoon (up to 86 %), while primary emissions contributed 14 % on average. This enhanced O 3 production by 7.7 % during the morning rush hour and 24.3 % in the afternoon. In addition, HCHO concentration peaked before that of O 3 , suggesting it plays significant role in O 3 formation. Biogenic emission oxidation contributed 3.1 μg m -3 (53.1 %) of HCHO and 5.2 pptv (40.1 %) of hydroperoxyl radicals (HO 2 ) in average urban areas, where the downwind regions of the forests had high nitrogen oxides (NO x ) levels and favorable conditions for O 3 production (17.3 μg m -3 , 20.5 %). In forested regions, sustained isoprene oxidation led to elevated oxidized VOCs including HCHO and acetaldehyde downwind, which practiced further photolysis of O 3 formation with anthropogenic NO x in urban areas. Sensitivity experiments recommend controlling industrial and traffic NO x emissions, with regional joint prevention and regulation, which are essential to reduce O 3 pollution., 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 © 2024. Published by Elsevier B.V.)

The secondary formation and diffusion processes of aerosol are extraordinarily complex and significantly impact the environment and human health. Therefore, exploring the process of aerosol formation and diffusion based on independent new tracer has always been a concern. The 7 Be and 10 Be, which are generated only by the action of cosmic rays, are chemically stable and adsorbed on aerosol for transmission, so they have the potential characteristics of aerosol tracers. Here, we obtained the daily resolution atmospheric 7 Be, 10 Be, and 10 Be/ 7 Be without dust interference in Xi'an autumn and winter (heavy pollution period in a typical polluted area) by accelerator mass spectrometry. It is found that during the rapid formation of secondary aerosols (SA) under the stable 10 Be/ 7 Be ratio, which indicates the stable atmospheric vertical structure, the concentration of 7 Be and 10 Be is significantly negatively correlated (R 2 > 0.9) with the aerosol concentration. Therefore, SA relative content in aerosols can be estimated by the dilution amount of 7 Be and 10 Be to reveal the secondary-formation process of aerosol (33% average contribution to aerosols during the winter heavy air pollution period). Furthermore, we also revealed the physical removal process of aerosols based on 7 Be, 10 Be, and 10 Be/ 7 Be, including precipitation removal and diffusion of vertical atmospheric movement caused by stratospheric air intrusion. In summary, meteoric cosmogenic 7 Be and 10 Be will provide a new way to study the secondary chemical formation and physical removal of aerosols., 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.)

In this study, 30 elements in fine particulate matter (PM 2.5 ) were measured in 18 Chinese cities in 2013. Elemental pollution in northern, southwest, and central China were severe, attributing to excessive coal and biomass combustion in these regions. The concentrations of S, Cl, and K in these areas were 8.21 ± 3.90, 4.03 ± 1.96, and 1.59 ± 0.613 μg/m 3 , respectively, which were 1.6-2.7 times higher than those in other regions of China. In addition, the industrial emissions in northeast and north China were large, leading to the elevated heavy metal concentration of 1.32 ± 1.17 μg/m 3 , especially Zn, Pb, Cr, Cd, and Br. Soil dust was the highest in northwest China among the five regions with the concentration of crustal elements of 6.37 ± 4.51 μg/m 3 . Moreover, although the levels of elemental concentration in east and southeast China were relatively acceptable, regulators must pay attention to elevated level of V (0.009 ± 0.006 μg/m 3 ) in these areas. Compared with 2003, several elements have deteriorated in some cities. For example, As increased by 70%, 18%, and 155% in Changchun, Beijing, and Jinchang, respectively. However, ~ 77% measured elements, e.g., Ti, Fe, and Pb markedly reduced in 2013, with reduction rates of 13-81%. These indicate that the government's policies related to particle-bound elements have shown certain positive environmental effects. For the health risks from the heavy metals in 2013, the non-cancer risks of As and Cd must not be neglected. The cancer risks of As and Pb were much higher than the international safety limit (10 -4 ). More prominent health risks were found in southwest, central, and northwest China. Therefore, the government should accelerate the shift to cleaner energy in underdeveloped areas of China to obtain more environmental and health benefits., (© 2021. The Author(s), under exclusive licence to Springer Nature B.V.)

An intensive measurement campaign was conducted in Xi'an, China from December 2012-January 2013 to investigate the chemical composition, formation, and optical properties of PM 1 . The PM 1 mass concentration (average = 138.8 ± 83.2 μg m -3 ) accounted for ∼50% of the PM 2.5 mass. Organic aerosols (OA) and secondary inorganic aerosols (SIA) were the most abundant PM 1 components, contributing 53.0% and 35.0% to the mass, respectively. Both primary emissions and aqueous-phase oxidation of secondary aerosols played roles in the pollution episodes. The average light scattering and absorption coefficients during the campaign were 805 ± 581 Mm -1 and 123 ± 96 Mm -1 , respectively. Both the mass scattering and mass absorption efficiencies for PM 1 were higher than that for PM 2.5-1 , indicating stronger ability of light extinction for the smaller particles at visible wavelengths compared with the larger ones. The contributions of aerosol species to light extinction coefficients under two visibility conditions were estimated based on multiple linear regression models, and the OA was found to be the largest contributor to light extinction in both cases. A larger contribution of SIA to light extinction for visibility <5 km demonstrated its greater impacts on visibility during heavy pollution conditions. These findings provide insights into the importance of submicron particles for pollution and visibility degradation in northwestern China., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

To investigate the chemical composition, size distribution, and mixing state of aerosol particles on heavy pollution days, single-particle aerosol mass spectrometry was conducted during 9-26 October 2015 in Xi'an, China. The measured particles were classified into six major categories: biomass burning (BB) particles, K-secondary particles, elemental carbon (EC)-related particles, metal-containing particles, dust, and organic carbon (OC) particles. BB and EC-related particles were the dominant types during the study period and mainly originated from biomass burning, vehicle emissions, and coal combustion. According to the ambient air quality index, two typical episodes were defined: clean days (CDs) and polluted days (PDs). Accumulation of BB particles and EC-related particles was the main reason for the pollution in Xi'an. Most types of particle size were larger on PDs than CDs. Each particle type was mixed with secondary species to different degrees on CDs and PDs, indicating that atmospheric aging occurred. The mixing state results demonstrated that the primary tracers were oxidized or vanished and that the amount of secondary species was increased on PDs. This study provides valuable information and a dataset to help control air pollution in the urban areas of Xi'an. Graphical abstract.

An intensive sampling campaign of airborne fine particles (PM 2.5 ) was conducted at Sanya, a coastal city in Southern China, from January to February 2012. Chemical analyses and mass reconstruction were used identify potential pollution sources and investigate atmospheric reaction mechanisms. A thermodynamic model indicated that low ammonia and high relative humidity caused the aerosols be acidic and that drove heterogeneous reactions which led to the formation of secondary inorganic aerosol. Relationships among neutralization ratios, free acidity, and air-mass trajectories suggest that the atmosphere at Sanya was impacted by both local and regional emissions. Three major transport pathways were identified, and flow from the northeast (from South China) typically brought the most polluted air to Sanya. A case study confirmed strong impact from South China (e.g., Pearl River Delta region) (contributed 76.8% to EC, and then this result can be extended to primary pollutants) when the northeast winds were dominant. The Weather Research Forecasting Black carbon model and trace organic markers were used to apportion local pollution versus regional contributions. Results of the study offer new insights into the atmospheric conditions and air pollution at this coastal city.

PM2.5 samples were collected in Sanya, China in summer and winter in 2012/2013. Organic carbon (OC), elemental carbon (EC), and non-polar organic compounds including n-alkanes (n-C14-n-C40) and polycyclic aromatic hydrocarbons (PAHs) were quantified. The concentrations of these carbonaceous matters were generally higher in winter than summer. The estimated secondary organic carbon (OCsec) accounted for 38% and 54% of the total organic carbon (TOC) in winter and summer, respectively. The higher value of OCsec in addition to the presences of photochemically-produced PAHs in summer supports that photochemical conversions of organics are much active at the higher air temperatures and with stronger intense solar radiation. Carbon preference index (CPI) and percent contribution of wax n-alkanes suggest that anthropogenic sources were more dominant than derivation from terrestrial plants in Sanya. Diagnostic ratios of atmospheric PAHs further indicate that there was a wide mix of pollution sources in winter while fossil fuel combustion was the most dominant in summer. Positive Matrix Factorization (PMF) analysis with 18 PAHs in the winter samples found that motor vehicle emissions and biomass burning were the two main pollution sources, contributing 37.5% and 24.6% of the total quantified PAHs, respectively., (Copyright © 2015 Elsevier B.V. All rights reserved.)

Sulfate aerosols have profound impacts on the climate, ecosystem, visibility, and public health, but the sulfate formation pathway remains elusive. In the present study, a source-oriented WRF-Chem model is applied to simulate a persistent air pollution episode from 4 to 15 July 2015 in Beijing–Tianjin–Hebei (BTH), China, to study the contributions of four pathways to sulfate formation. When comparing simulations to measurements in BTH, the index of agreement (IOA) of meteorological parameters, air pollutants, and aerosol species generally exceeds 0.6. On average in BTH, the heterogeneous reaction of SO2 involving aerosol water and the SO2 oxidation by OH constitutes the two most important sulfate sources, with a contribution of about 35 %–38 % and 33 %–36 %, respectively. Primary sulfate emissions account for around 22 %–24 % of the total sulfate concentration. SO2 oxidation by stabilized Criegee intermediates (sCIs) also plays an appreciable role in sulfate formation, with a contribution of around 9 % when an upper limit of the reaction rate constant of sCIs with SO2 (κsCI+SO2=3.9×10-11 cm 3 s -1) and a lower limit of the reaction rate constant of sCIs with H2O (κsCI+H2O=1.97×10-18 cm 3 s -1) are used. Sensitivity studies reveal that there are still large uncertainties in the sulfate contribution of SO2 oxidation by sCIs. The sulfate contribution of the reaction is decreased to less than 3 % when κSCI+SO2 is decreased to 6.0×10-13 cm 3 s -1. Furthermore, when κsCI+H2O is increased to 2.38×10-15 cm 3 s -1 based on the reported ratio of κSCI+H2O to κSCI+SO2 (6.1×10-5), the sulfate contribution becomes insignificant at less than 2 %. Further studies need to be conducted to better determine κsCI+SO2 and κsCI+H2O to evaluate the effects of sCI chemistry on sulfate formation. [ABSTRACT FROM AUTHOR]

Although stringent emission mitigation strategies have been carried out since 2013 in Beijing–Tianjin–Hebei (BTH), China, heavy haze with high levels of fine particulate matter (PM 2.5) still frequently engulfs the region during wintertime and the nitrate contribution to PM 2.5 mass has progressively increased. N2O5 heterogeneous hydrolysis is the most important pathway of nitrate formation at nighttime. In the present study, the WRF-Chem model is applied to simulate a heavy haze episode from 10 to 27 February 2014 in BTH to evaluate contributions of N2O5 heterogeneous hydrolysis to nitrate formation and effects of organic coating. The model generally performs reasonably well in simulating meteorological parameters, air pollutants, and aerosol species against observations in BTH. N2O5 heterogeneous hydrolysis with all the secondary organic aerosol assumed to be involved in coating considerably improves the nitrate simulations compared to the measurements in Beijing. On average, organic coating decreases nitrate concentrations by 8.4 % in BTH during an episode, and N2O5 heterogeneous hydrolysis with organic coating contributes about 30.1 % of nitrate concentrations. Additionally, the reaction also plays a considerable role in the heavy haze formation, with a PM 2.5 contribution of about 11.6 % in BTH. Sensitivity studies also reveal that future studies need to be conducted to predict the organic aerosol hygroscopicity for accurately representing the organic coating effect on N2O5 heterogeneous hydrolysis. [ABSTRACT FROM AUTHOR]

Organic aerosol (OA) concentrations are simulated over the Beijing–Tianjin–Hebei (BTH) region from 9 to 26 January 2014 using the Weather Research and Forecasting model coupled with chemistry (WRF-CHEM), with the goal of examining the impact of heterogeneous HONO sources on SOA formation and SOA formation from different pathways during wintertime haze days. The model generally shows good performance with respect to simulating air pollutants and organic aerosols against measurements in BTH. Model results show that heterogeneous HONO sources substantially enhance near-surface SOA formation, increasing the regional average near-surface SOA concentration by about 46.3 % during the episode. Oxidation and partitioning of primary organic aerosols treated as semi-volatile dominate SOA formation, contributing 58.9 % of the near-surface SOA mass in BTH. Irreversible uptake of glyoxal and methylglyoxal on aerosol surfaces constitutes the second most important SOA formation pathway during the episode, with the SOA contribution increasing from 8.5 % under non-haze conditions to 30.2 % under haze conditions. Additionally, direct emissions of glyoxal and methylglyoxal from residential sources contribute about 25.5 % of the total SOA mass on average in BTH. Our study highlights the importance of heterogeneous HONO sources and primary residential emissions of glyoxal and methylglyoxal to SOA formation over the BTH region in winter. [ABSTRACT FROM AUTHOR]

The roles of anthropogenic emissions and weather conditions in air pollution over eastern China have been widely discussed but still controversial. Here we focus on the impact of the intraseasonal variability of midtropospheric weather circulations on air quality during 2015–2016 winter. We use the European Center for Medium‐Range Weather Forecasts reanalysis data to calculate westerly wind index (WI) and meridionality in the midtroposphere and also calculate the intensity of Siberian High at the surface. The results suggest that there were lower WI, higher meridionality, and strengthened Siberian High in January 2016 compared with the conditions in December 2015. Lower WI and higher meridionality imply for wavier midtropospheric weather circulations and stronger surface northerly winds, thereby causing more southward cold fresh air advection and resulting in the lower PM2.5 concentrations over eastern China in January 2016. Sensitivity experiments conducted by the Weather Research and Forecasting Chemical model show that the intraseasonal weather variability dominantly causes lower PM2.5 concentrations in January 2016. It not only counteracts increments in PM2.5 concentrations induced by the increased emission but also reduces PM2.5 concentrations by an extra 25–100 μg/m3. We also simulate two extreme weather patterns and compare their effects on PM2.5 concentrations. Difference in these two weather patterns induces changes in PM2.5 concentrations by 50–200 μg/m3 over eastern China and the maximal change exceeding 200 μg/m3. These findings suggest that understanding the variability of the dominant midtropospheric circulation is the key to successfully forecasting short‐term air quality over eastern China in winter. Plain Language Summary: The subseasonal variation of PM2.5 concentrations is dominantly induced by the intraseasonal variability of weather circulations during 2015–2016 winter. In the early winter (December 2015), a straight westerly wind prevails at the midtroposphere, confining cold air within the high latitudes and causing the accumulation of PM2.5 concentrations in eastern China, while in the late winter (January 2016), a north‐to‐south oriented airflow at the midtroposphere allows cold air advection to eastern China, reducing PM2.5 concentrations. Consequently, the intraseasonal weather variability leads to the maximal reduction of PM2.5 concentrations by 50–200 μg/m3. These findings suggest that understanding the variability of the midtroposphere circulation patterns is the key to successfully forecasting and improving air quality in winter. Key Points: Monthly emission change in 2015‐2016 winter results in an increment in PM2.5 concentrations by 10‐50 micrograms per cubic meter in eastern ChinaWeather variability not only offsets PM2.5 increments due to emission change but also reduces PM2.5 concentrations by an extra 25‐100 micrograms per meterMidtropospheric westerly wind circulations are the key to understanding subseasonal variations of PM2.5 concentrations [ABSTRACT FROM AUTHOR]

An intensive sampling campaign of airborne fine particles (PM2.5) was conducted at Sanya, a coastal city in Southern China, from January to February 2012. Chemical analyses and mass reconstruction were used identify potential pollution sources and investigate atmospheric reaction mechanisms. A thermodynamic model indicated that low ammonia and high relative humidity caused the aerosols be acidic and that drove heterogeneous reactions which led to the formation of secondary inorganic aerosol. Relationships among neutralization ratios, free acidity, and air-mass trajectories suggest that the atmosphere at Sanya was impacted by both local and regional emissions. Three major transport pathways were identified, and flow from the northeast (from South China) typically brought the most polluted air to Sanya. A case study confirmed strong impact from South China (e.g., Pearl River Delta region) (contributed 76.8% to EC, and then this result can be extended to primary pollutants) when the northeast winds were dominant. The Weather Research Forecasting Black carbon model and trace organic markers were used to apportion local pollution versus regional contributions. Results of the study offer new insights into the atmospheric conditions and air pollution at this coastal city. [ABSTRACT FROM AUTHOR]