Relaxation of Spring Festival Firework Regulations Leads to a Deterioration in Air Quality.

The relaxation of restrictions on Chinese Spring Festival (SF) firework displays in certain regions has raised concerns due to intensive emissions exacerbating air quality deterioration. To evaluate the impacts of fireworks on air quality, a comparative investigation was conducted in a city between 2022 (restricted fireworks) and 2023 SF (unrestricted), utilizing high time-resolution field observations of particle chemical components and air quality model simulations. We observed two severe PM2.5 pollution episodes primarily triggered by firework emissions and exacerbated by static meteorology (contributing approximately 30%) during 2023 SF, contrasting with its absence in 2022. During firework displays, freshly emitted particles containing more primary inorganics (such as chloride and metals like Al, Mg, and Ba), elemental carbon, and organic compounds (including polycyclic aromatic hydrocarbons) were predominant; subsequently, aged particles with more secondary components became prevalent and continued to worsen air quality. The primary emissions from fireworks constituted 54% of the observed high PM2.5 during the displays, contributing a peak hourly PM2.5 concentration of 188 µg/m3 and representing over 70% of the ambient PM2.5. This study underscores that caution should be exercised when igniting substantial fireworks under stable meteorological conditions, considering both the primary and potential secondary effects.

Abundance and sources of particulate polycyclic aromatic hydrocarbons and aromatic acids at an urban site in central China.

We conducted a simultaneous field study of PM2.5-bound particulate polycyclic aromatic hydrocarbons (PAHs) and aromatic acids (AAs) in a polluted city Zhengzhou to explore the concentration, sources and potential conversion pathways between PAHs and AAs in different seasons. The average concentrations of PM2.5, 28PAHs and 8AAs during the sampling period were 77 µg/m3, 75 ng/m3, and 283 ng/m3, respectively. The concentration of both 28PAHs and 8AAs were highest in winter and lowest in summer with ratios of 6.3 and 2.3, respectively. PAHs with 5-7 rings were the main components of PAHs (52%), followed by 4 rings PAHs (30%) and 2-3 rings PAHs (18%). According to the source appointment results obtained by positive matrix factorization, the main sources of PAHs were combustion and vehicle emissions, which account for 37% and 34%, respectively. 8AAs were divided into three groups, including four benzene dicarboxylic acids (B2CAs), three benzene tricarboxylic acids (B3CAs) and one benzene tetracarboxylic acid (B4CA). And interspecies correlation analysis with PM2.5 source markers were used to investigate potential sources. Phthalic acid (o-Ph) was the most abundant specie of 8AAs (157 ng/m3, 55% of 8AAs), which was well correlated with sulfate. Meanwhile, B3CAs and B4CA were highly correlated with sulfate and weakly correlated with levoglucosan, suggesting that secondary formation was their main source. As logical oxidation products of PAHs, o-Ph and B3CAs showed good correlations with a number of PAHs, indicating possible photochemical oxidation pathway by PAHs. In addition, O3, NO2, temperature and relative humidity have positive effects on the secondary formation of B3CAs.

Mixing states and secondary formation processes of organic nitrogen-containing single particles in Guangzhou, China.

Organic nitrogen (ON) compounds play a significant role in the light absorption of brown carbon and the formation of organic aerosols, however, the mixing state, secondary formation processes, and influencing factors of ON compounds are still unclear. This paper reports on the mixing state of ON-containing particles based on measurements obtained using a high-performance single particle aerosol mass spectrometer in January 2020 in Guangzhou. The ON-containing particles accounted for 21% of the total detected single particles, and the particle count and number fraction of the ON-containing particles were two times higher at night than during the day. The prominent increase in the content of ON-containing particles with the enhancement of NOx mainly occurred at night, and accompanied by high relative humidity and nitrate, which were associated with heterogeneous reactions between organics and gaseous NOx and/or NO3 radical. The synchronous decreases in ON-containing particles and the mass absorption coefficient of water-soluble extracts at 365 nm in the afternoon may be associated with photo-bleaching of the ON species in the particles. In addition, the positive matrix factorization analysis found five factors dominated the formation processes of ON particles, and the nitrate factor (33%) mainly contributed to the production of ON particles at night. The results of this study provide unique insights into the mixing states and secondary formation processes of the ON-containing particles.

Characteristics of wintertime carbonaceous aerosols in two typical cities in Beijing-Tianjin-Hebei region, China: Insights from multiyear measurements.

In order to investigate the impact of "Blue Sky War" implemented during 2018-2020 on carbonaceous aerosols in Beijing-Tianjin-Hebei (BTH) region, China, fine particulate matter (PM2.5) samples were collected simultaneously in Tianjin and Handan in three consecutive winters from 2018 to 2020. Organic carbon (OC) and elemental carbon (EC) in PM2.5 were measured with the same thermal-optical methods and analysis protocols. Significant reductions in primary organic carbon (POC) and EC concentrations were observed both in Tianjin and Handan, with decreasing rates of 0.65 and 2.95 µg m-3 yr-1 for POC and 0.13 and 0.64 µg m-3 yr-1 for EC, respectively. The measured absorption coefficients of EC (babs, EC) also decreased year by year, with a decreasing rate of 1.82 and 6.16 Mm-1 yr-1 in Tianjin and Handan, respectively. The estimated secondary organic carbon (SOC) concentrations decreased first and then increased in both Tianjin and Handan, accounting for more than half of the total OC in winter of 2020-2021 and with increasing contributions especially in highly polluted days. SOC was recognized as one of key factors influencing EC light absorption. EC in the two cities was relatively more related to coal combustion and industrial sources. The reductions of primary carbonaceous components may be attributed to the air quality regulations targeting coal combustion and industrial sources emissions in BTH area. Potential source contribution function (PSCF) analysis results indicated that the major source areas of OC and EC in Tianjin were the southwest region of the sampling site, while the southeast areas for Handan. These findings demonstrated the effectiveness of air quality regulation in primary emissions in typical polluted cities in BTH region and highlighted the needs for further control and in-depth investigation of SOC formation along with implementation of air pollution control act in the future.

Variabilities of δ13C and carbonaceous components in ambient PM2.5 in Northeast India: Insights into sources and atmospheric processes.

A year-long sampling campaign of ambient PM2.5 (particulate matter with aerodynamic diameter ≤2.5 mm) at a regional station in the North-Eastern Region (NER) of India was performed to understand the sources and formation of carbonaceous aerosols. Mass concentration, carbon fractions (organic and elemental carbon), and stable carbon isotope ratio (δ13C) of PM2.5 were measured and studied along with cluster analysis and Potential Source Contribution Function (PSCF) modelling. PM2.5 mass concentration was observed to be highest during winter and post-monsoon seasons when the meteorological conditions were relatively stable compared to other seasons. Organic carbon (OC) concentration was more than two times higher in the post-monsoon and winter seasons than in the pre-monsoon and monsoon seasons. Air mass back trajectory cluster analysis showed the dominance of local and regional air masses during winter and post-monsoon periods. In contrast, long-range transported air masses influenced the background site in pre-monsoon and monsoon. Air mass data and PSCF analysis indicated that aerosols during winter and post-monsoon are dominated by freshly generated emissions from local sources along with the influence from regional transport of polluted aerosols. On the contrary, the long-range transported air masses containing aged aerosols were dominant during pre-monsoon. No significant variability was observed in the range of δ13C values (-28.2‰ to -26.4‰) during the sampled seasons. The δ13C of aerosols indicates major sources to be combustion of biomass/biofuels (C3 plant origin), biogenic aerosols, and secondary aerosols. The δ13C variability and cluster/PSCF modelling suggest that aged aerosols (along with enhanced photo-oxidation derived secondary aerosols) influenced the final δ13C during the pre-monsoon. On the other hand, lower δ13C in winter and post-monsoon is attributed to the freshly emitted aerosols from biomass/biofuels.

Evolution of aerosol chemistry in Beijing under strong influence of anthropogenic pollutants: Composition, sources, and secondary formation of fine particulate nitrated aromatic compounds.

Nitrated aromatic compounds (NACs) constitute a key segment of brown carbon (BrC), thereby contributing to the light-absorbing characteristics of aerosols in the atmosphere. However, until recently, there is a scarcity of research on their generation in the urban environment. The current study is based upon an extensive field study of NACs from fine particle samples obtained at an urban location in Beijing in the spring and summer of 2017, which was characterized by both high anthropogenic volatile organic compounds (VOCs) and high-NOx dominated conditions. The mean total concentration of the nine NACs was 8.58 ng m-3 in spring and 8.54 ng m-3 in summer. In the spring, the most abundant NACs were 4-nitrophenol (33.7%) and 4-nitrocatechol (19.3%), while in the summer, the most abundant NACs were 4-nitroguaiacol (34.9%) and 2, 4-dinitrophenol (23%). Atmospheric NACs were primarily produced from coal combustion (52%) and biomass burning (32%) in spring, and originated from the secondary formation (37%) and traffic (35%) in summer. NO2 could promote the formation of NACs with a significant effect on their compositions, especially for nitrophenols and nitrocatechols. It can also affect the formation of nitrated aerosols and their existing form. Inorganic nitrates were increased to conversion in the daytime when NO2 concentrations were higher than 30 ppb, but the corresponding oxidation products shifted to primarily organic ones at night. The transition was VOC-sensitive regimes for NAC formation, and nitration of toluene was a more important pathway during the campaign in Beijing.

Year-round observation of atmospheric inorganic aerosols in urban Beijing: Size distribution, source analysis, and reduction mechanism.

To investigate particle characteristics and find an effective measure to control severe particle pollution, year-round observation of size-segregated inorganic aerosols was conducted in Beijing from January to December, 2016. The sampled atmospheric particles all presented bimodal size distribution at four pollution levels (clear, slight pollution, moderate pollution and severe pollution), and peak values appeared at the size range of 0.7-2.1 µm and >9.0 µm, respectively. As dominant particle compositions, NO3-, SO42-, and NH4+ in four pollution levels all showed significant peaks in fine mode, especially at the size range of 1.1-2.1 µm. Secondary inorganic aerosols accounted for about 67.6% (36.3% (secondary sulfates) + 31.3% (secondary nitrates)) of the total sources of fine particles in urban Beijing. Severe pollution of fine particles was mainly caused by the air masses transported from nearby western and southern areas, which are industrial and densely populated region, respectively. Sensitivity tests further revealed that the control measures focusing on ammonium emission reduction was the most effective for particle pollution mitigation, and fine particles all showed nonlinear responses after reducing ammonium, nitrate, and sulfate concentrations, with the fitting curves of y = -120.8x - 306.1x2 + 290.2x3, y = -43.5x - 67.8x2, and y = -25.8x - 110.4x2 + 7.6x3, respectively (y and x present fine particle mass variation (µg/m3) and concentration reduction ratio (CRR)/100 (dimensionless)). Overall, our study presents useful information for understanding the characteristics of atmospheric inorganic aerosols in urban Beijing, as well as offers policy makers with effective measure for mitigating particle pollution.

Insights into measurements of water-soluble ions in PM2.5 and their gaseous precursors in Beijing.

To better understand the characteristics and transformation mechanisms of secondary inorganic aerosols, hourly mass concentrations of water-soluble inorganic ions (WSIIs) in PM2.5 and their gaseous precursors were measured online from 2016 to 2018 at an urban site in Beijing. Seasonal and diurnal variations in water-soluble ions and gaseous precursors were discussed and their gas-particle conversion and partitioning were also examined, some related parameters were characterized. The (TNH3) Rich was also defined to describe the variations of the excess NH3 in different seasons. In addition, a sensitivity test was carried out by using ISORROPIA II to outline the driving factors of gas-particle partitioning. In Beijing, the relative contribution of nitrate to PM2.5 has increased markedly in recent years, especially under polluted conditions. In the four seasons, only a small portion of NO2 in the atmosphere was converted into total nitrate (TNO3), and more than 80% of TNO3 occurred in the form of nitrate due to the abundant ammonia. The concentration of total ammonia (TNH3) was much higher than that required to neutralize acid gases, and most of the TNH3 occurred as gaseous NH3. The nitrous acid (HONO) concentration was highly correlated with NH3 concentration and had increased significantly in Beijing compared with previous studies. The total chloride (TCl) was the highest in winter, and ε(Cl-) was more sensitive to variations in the ambient temperature (T) and relative humidity (RH) than ε(NO3-).

Characterizing oxygenated volatile organic compounds and their sources in rural atmospheres in China.

Oxygenated volatile organic compounds (OVOCs) are important precursors and products of atmospheric secondary pollution. The sources of OVOCs, however, are still quite uncertain, especially in the atmosphere with much pollution in China. To study the sources of OVOCs in rural atmospheres, a proton transfer reaction mass spectrometry (PTR-MS) was deployed at a northern rural site (WD) and a southern rural site (YMK) in China during the summer of 2014 and 2016, respectively. The continuous observation showed that the mean concentration of TVOCs (totally 17 VOCs) measured at WD (52.4 ppbv) was far higher than that at YMK (11.1 ppbv), and the OVOCs were the most abundant at both the two sites. The diurnal variations showed that local sources of OVOCs were still prominent at WD, while regional transport influenced YMK much. The photochemical age-based parameterization method was then used to quantitatively apportion the sources of ambient OVOCs. The anthropogenic primary sources at WD and YMK contributed less (2%-16%) to each OVOC species. At both the sites, the atmospheric background had a dominant contribution (~50%) to acetone and formic acid, while the anthropogenic secondary formation was the main source (~40%) of methanol and MEK. For acetaldehyde and acetic acid, the biogenic sources were their largest source (~40%) at WD, while the background (39%) and anthropogenic secondary formation (42%) were their largest sources at YMK, respectively. This study reveals the complexity of sources of OVOCs in China, which urgently needs explored further.

Effects of relative humidity and PM2.5 chemical compositions on visibility impairment in Chengdu, China.

To better understand the potential causes of visibility impairment in autumn and winter in Chengdu, relative humidity (RH), visibility, the concentrations of PM2.5 and its chemical components were on-line measured continuously in Chengdu from Nov. 2016 to Jan. 2017. Six obvious haze episodes occurred in Chengdu, with the total time of haze episodes accounted for more than 90% of the total observation period, and higher NO2 concentrations and RH were related to the high particle concentrations in haze episodes. The visibility decreased in a non-linear tendency under different RH conditions with the increase of PM2.5 concentrations, which was more sensitive to RH under lower PM2.5 concentrations. The threshold concentration of PM2.5 got more smaller with the increase of RH. During the entire observation period, organic matter (OM) was the largest contributor (31.12% to extinction coefficient (bext)), followed by NH4NO3 and (NH4)2SO4 with 28.03% and 23.01%, respectively. However, with the visibility impairment from Type I (visibility > 10 km) to Type IV (visibility ≤2 km), the contribution of OM to bext decreased from 38.12% to 26.77%, while the contribution of NH4NO3 and (NH4)2SO4 to bext increased from 19.09% and 20.20% to 34.29% and 24.35%, respectively, and NH4NO3 became the largest contributor to bext at Type IV. The results showed that OM and NH4NO3 were the key components of PM2.5 for visibility impairment in Chengdu, indicating that the control of precursors emissions of carbonaceous species and NH4NO3 could effectively improve the visibility in Chengdu.

Sources of elevated organic acids in the mountainous background atmosphere of southern China.

Formic acid (FA) and acetic acid (AA) are pivotal organic acids in the troposphere, significantly influencing atmospheric chemistry. However, their abundance and sources in the mountainous background atmosphere remain underexplored. We undertook continuous measurements of FA and AA in Nanling mountains, southern China, during autumn 2020 using a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS). Both acids registered higher concentrations than in other global high-altitude or forested locations, averaging at 0.89 (max: 3.91) and 0.95 (max: 3.52) ppbv for FA and AA, respectively. High concentrations of FA and AA in this forested background area arose from secondary formation and biomass burning, collectively contributing 71 % to 89 %. During episodes, FA and AA concentrations surged 2-3 times, owing to the enhanced atmospheric oxidation capacity. The secondary FA production was predominantly due to isoprene oxidation among the VOC precursors studied. However, observed inconsistencies between calculated and actual FA concentrations suggest overlooked precursors or mechanisms warranting further investigation. Our findings can enhance the understanding of organic acid characteristics and the interplay of biogenic and anthropogenic sources in the background atmosphere.

Exploring secondary aerosol formation associated with elemental carbon in the lower free troposphere.

The variability of element carbon (EC) mixed with secondary species significantly complicates the assessment of its environmental impact, reflecting the complexity and diversity of EC-containing particles' composition and morphology during their ascent and regional transport. While the catalytic role of EC in secondary aerosol formation is recognized, the effects of heterogeneous chemistry on secondary species formation within diverse EC particle types are not thoroughly understood, particularly in the troposphere. Alpine sites offer a prime environment to explore EC properties post-transport from the ground to the free troposphere. Consequently, we conducted a comprehensive study on the genesis of secondary aerosols in EC-containing particles at Mt. Hua (altitude: 2069 m) from 1 May to 10 July, using a single particle aerosol mass spectrometer (SPAMS). Our analysis identified six major EC particle types, with EC-K, EC-SN, and EC-NaK particles accounting for 27.6 %, 27.0 %, and 19.6 % of the EC particle population, respectively. The concentration-weighted trajectory (CWT) indicated that the lower free troposphere over Mt. Hua is significantly affected by anthropogenic emissions at ground-level, predominantly from northwestern and eastern China. Atmospheric interactions are crucial in generating high sulfate levels in EC-SN and EC-OC particles (> 70 %) and notable nitrate levels in EC-K, EC-BB, and EC-Fe particles (> 80 %). The observed high chloride content in EC-OC particles (56 ± 32 %) might enhance chlorine's reactivity with organic compounds via heterogeneous reactions within the troposphere. Distinct diurnal cycles for sulfate and nitrate are mainly driven by varying transport dynamics and formation processes, showing minimal dependency on EC particle types. Enhanced nocturnal oxalate conversion in EC-Fe particles is likely due to the aqueous oxidation of precursors, with Fe-catalyzed Fenton reactions enhancing OH radical production. This investigation provides critical insights into EC's role in secondary aerosol development during its transport in the lower free troposphere.

Secondary formation of oxygenated and nitrated polycyclic aromatic compounds under stagnant weather conditions: Drivers and seasonal variation.

Severe air pollution tends to occur under stagnant weather conditions. This study focused on the occurrence and formation of PM2.5-bound polycyclic aromatic compounds (PACs) under stagnant weather conditions, in consideration of their adverse human health effect and ecological toxicity. The concentrations of PACs were higher under stagnant weather conditions than in other situations with averaged values of 46.0 ng/m3 versus 12.3-39.9 ng/m3 for total PACs. Secondary formation contributed to over half of the oxygenated and nitrated polycyclic aromatic compounds (OPAHs and NPAHs). Further analyses revealed different formation mechanisms for secondary OPAHs and NPAHs. Secondary production of OPAHs was sensitive to the variations of both temperature (T) and O3 concentration at T < 22 °C but sustained at a high level despite the fluctuation of temperature and O3 concentration at T > 22 °C. Elevated NO2 concentrations favored the formation of inorganic nitrogen-containing products over NPAHs under lower temperature and higher humidity. Stagnant weather events, accompanied by raised PAC levels occurred in all seasons, but their effects on secondary processes differed among seasons. The elevated temperature, lowered humidity, and increased NO2 level facilitated the secondary formation of OPAHs and/or NPAHs during the stagnant weather events in spring and summer. While under the temperature and humidity conditions in autumn and winter, increased NO2 levels during stagnant weather events promoted the production of secondary inorganic nitrogen-containing compounds over organic products. This study raised concern about the toxic organic pollutants in the atmosphere under stagnant weather conditions and revealed different formation mechanisms between secondary oxygenated and nitrated pollutants as well as among different seasons.

Anthropogenic, biogenic, and photochemical influences on surface formaldehyde and its significant decadal (2006-2017) decrease in the Lewiston-Clarkston valley of the northwestern United States.

Formaldehyde (HCHO) is a key carcinogen and plays an important role in atmospheric chemistry. Both field measurements and Positive Matrix Factorization (PMF) modeling have been employed to investigate the concentrations and sources of HCHO in the Lewiston-Clarkston (LC) valley of the mountainous northwestern U.S. Different instruments were deployed to measure surface formaldehyde and other related compounds in July of 2016 and 2017. The measurements reveal that the average HCHO concentrations have significantly decreased to 2-5 ppb in the LC valley in comparison to its levels (10-20 ppb) observed in July 2006. This discovery with surface measurements deserves attention given that satellite retrievals showed an increasing long-term trend from 2005 to 2014 in total vertical column density of HCHO in the region, suggesting that satellite instruments may not adequately resolve small valleys in the mountainous region. Our PMF modeling identified four major sources of HCHO in the valley: (1) emissions from a local paper mill, (2) secondary formation and background, (3) biogenic sources, and (4) traffic. This study reveals that the emissions from the paper mill cause high HCHO spikes (6-19 ppb) in the early morning. It is found that biogenic volatile organic compounds (VOCs) in the area are influenced by national forests surrounding the region (e.g., Nez Perce-Clearwater, Umatilla, Wallowa-Whitman, and Idaho Panhandle National Forests). The results provide useful information for developing strategies to control HCHO levels and have implications for future HCHO studies in atmospheric chemistry, which affects secondary aerosols and ozone formation.

Roles of ambient temperature and relative humidity on the relationship between fine particulate matter and gaseous pollutants in the largest industrial city of Ulsan, South Korea.

Although meteorological conditions play a significant role in air pollution, research on their effects on the relationship between air pollutants is limited. In this study, trends of six criteria air pollutants were investigated from 15 air quality monitoring stations (AQMSs) in Ulsan, a multi-industrial city in South Korea, during 2015-2019. Unlike CO and O3, SO2, NO2, PM10, and PM2.5 showed statistically significant decreasing trends over the period. The companion relationship between PM2.5 and gaseous pollutants was evaluated by their correlations [R (PM2.5-GPs)]. R (PM2.5-NO2) was relatively high at almost all AQMSs, whereas high R (PM2.5-SO2) was observed near the petrochemical industrial complex, suggesting a great influence of local emissions (vehicles and industries). R (PM2.5-CO) and the standardized regression coefficients of CO obtained from the multiple linear regression model were the highest, indicating that combustion processes may significantly contribute to PM2.5. The effect of temperature (T) was more apparent on R (PM2.5-GPs) than that of relative humidity, with significant values under T > 15 °C. Moreover, R (PM2.5-O3) was positive at the T range of 12-18 °C, suggesting that reducing GPs emitted by industrial facilities during May-June may control PM2.5 and O3 in Ulsan. The methodology demonstrated in this study can be further used for a better understanding of the influences of environmental factors on the secondary PM2.5 formation from gaseous precursors and the R (PM2.5-O3).

Distinct seasonal variability of source-dependent health risks from PM2.5-bound PAHs and related derivatives in a megacity, southwest China: Implications for the significance of secondary formation.

In contrast to polycyclic aromatic hydrocarbons (PAHs) which have been regularly monitored, the source-dependent health risk of their derivatives in ambient environment has not been well understood, especially regarding seasonal variability. In this study, oxygenated and nitrated PAHs (OPAHs and NPAHs) in PM2.5 samples from different seasons in urban Chongqing were analyzed and compared with PAHs from a human health perspective. Benzo[a]pyrene equivalent concentrations (BaPeq) were annually averaged at 6.13 ± 8.97 ng/m3 (n = 118) in the present study, with highest levels in winter followed by spring, autumn, and summer. The BaPeq values of OPAHs were higher than PAHs in spring and summer with seasonal averaged value up to 3.7 times of that for PAHs, manifesting significant underestimation of the health impact if only PAHs were considered. Incremental lifetime cancer risk (ILCR) model results suggested that the potential cancer risks were accumulated mostly from inhalation exposure during infancy and adulthood. Furthermore, in comparison with PAHs, OPAHs, mainly 6H-Benzo[c,d]pyren-6-one, had significant contribution to cancer risks (annually averaged at 58.3 %). Source-dependent cancer risks based on positive matrix factorization model denoted secondary formed PAH derivatives as a critical contributor to cancer risk, particularly in spring and summer (attributed to about 61 % of ILCR). The enhanced secondary formation of PAH derivatives during spring and summer was partially justified by diagnostic ratios and further analysis revealed that higher temperature, higher O3 level, and lower relative humidity besides stronger solar intensity during these two seasons as the most likely causes of this seasonal variation. Results in this study emphasizes that more knowledge on the formation and toxicity of OPAHs is imperative, especially in the context of complex PM2.5-ozone pollution in China.

Pollution characteristics and light-driven evolution of environmentally persistent free radicals in PM2.5 in two typical northern cities of China.

Environmentally persistent free radicals (EPFRs) in PM2.5 can pose significant health risks by generating reactive oxygen species (ROS). In this study, Beijing and Yuncheng were chosen as two representative northern cities of China that mainly relied on natural gas and coal respectively as the energy source for domestic heating in winter. The pollution characteristics and exposure risks of EPFRs in PM2.5 around the heating season of 2020 were investigated and compared between the two cities. Through laboratory simulation experiments, the decay kinetics and secondary formation of EPFRs in PM2.5 collected in both cities were also studied. EPFRs in PM2.5 collected in Yuncheng in the heating period showed longer lifetime and lower reactivity, suggesting that EPFRs originated from coal combustion were more stable in the atmosphere. However, the generation rate of hydroxyl radical (·OH) by the newly formed EPFRs in PM2.5 in Beijing under ambient conditions was 4.4 times of that in Yuncheng, suggesting higher oxidative potential of EPFRs from the atmospheric secondary processes. Accordingly, the control strategies of EPFRs and their health risks were raised for the two cities, which would also have direct implication for the control of EPFRs in other areas of similar atmospheric emission and reaction patterns.

Significant roles of aged dust aerosols on rapid nitrate formation under dry conditions in a semi-arid city.

Mineral dust can accelerate secondary aerosol formation under humid conditions. However, it is unclear whether it can promote secondary aerosol formation under dry conditions. To investigate this issue, two years of comprehensive observations was conducted at a semi-arid site, near the dust source regions. Three types of episodes were selected: dust, anthropogenic-dominated, and mixed (mixed with dust and anthropogenic aerosols). Compared to anthropogenic-dominated episodes under humid conditions, rapid nitrate formation was still observed in mixed episodes under dry conditions, suggesting that active metallic oxides in dust, such as titanium dioxide, could promote photochemical reactions of nitrogen dioxide. The detailed evolutionary processes are further illustrated by a typical dust-to-mixed episode. After the arrival of the dust, titanium sharply increased ten-fold and rapid nitrate formation was observed, together with a rapid increase in the two most important photochemical pollutants, ozone and peroxyacetyl nitrate. The increased secondary organic carbon further illustrated that the suspended dust particles accelerated the atmospheric oxidative capacity, thereby enhancing secondary aerosol formation and eventually leading to haze pollution. These results differ from those in humid regions and therefore expand the scientific understanding of the impact of dust aerosols on haze pollution under dry conditions.

Environmental factors driving the formation of water-soluble organic aerosols: A comparative study under contrasting atmospheric conditions.

Water-soluble organic carbon (WSOC), as major fractions of atmospheric aerosols, have gained attention due to their light-absorption properties. To illustrate the sources and key environmental factors driving WSOC formation under different atmospheric conditions, a comparative study was conducted by summarizing the results obtained from five field campaigns at inland (urban, suburban or regional) sites and a coastal site during different seasons. Organic carbon concentrations varied from 8.5 µg/m3 at the summer regional site to 17.5 µg/m3 at the winter urban site, with 46 %- 89 % of the mass as WSOC. Based on correlation analysis, primary combustion emissions were more important in winter than in summer, and secondary formation was an important source of WSOC during winter, summer and autumn. Atmospheric oxidants (NO2, O3), aerosol liquid water (ALW) and ambient RH were important factors influencing the WSOC formation, while their roles varied in different atmospheres. We observed a seasonal transition of atmospheric oxidants dominating the WSOC formation from O3 and NO2-driven conditions in summer to NO2-driven conditions in winter. Elevated ALW or ambient RH generally favor the WSOC formation, while the WSOC dependence of ALW varied among different ALW ranges. As the increasing of ALW or ambient RH, a transition of WSOC formation from "RH/ALW-limited regime" under low-ALW conditions, to "RH/ALW and precursor-driven regime" under medium-ALW/RH, and to "precursor-limited (RH/ALW-excess) regime" were observed for the inland atmospheric conditions. Under the high-RH and ALW conditions in coastal areas, ALW or ambient RH was generally not a limiting factor for WSOC formation.

Characteristics of secondary inorganic aerosols and contributions to PM2.5 pollution based on machine learning approach in Shandong Province.

Primary emissions of particulate matter and gaseous pollutants, such as SO2 and NOx have decreased in China following the implementation of a series of policies by the Chinese government to address air pollution. However, controlling secondary inorganic aerosol pollution requires attention. This study examined the characteristics of the secondary conversion of nitrate (NO3-) and sulfate (SO42-) in three coastal cities of Shandong Province, namely Binzhou (BZ), Dongying (DY), and Weifang (WF), and an inland city, Jinan (JN), during December 2021. Furthermore, the Shapley Additive Explanation (SHAP), an interpretable attribution technique, was adopted to accurately calculate the contributions of secondary formations to PM2.5. The nitrogen oxidation rate exhibited a significant dependence on the concentration of O3. High humidity facilitates sulfur oxidation. Compared to BZ, DY, and WF, the secondary conversion of NO3- and SO42- was more intense in JN. The light-gradient boosting model outperformed the random forest and extreme-gradient boosting models, achieving a mean R2 value of 0.92. PM2.5 pollution events in BZ, DY, and WF were primarily attributable to biomass burning, whereas pollution in Jinan was contributed by the secondary formation of NO3- and vehicle emissions. Machine learning and the SHAP interpretable attribution technique offer a precise analysis of the causes of air pollution, showing high potential for addressing environmental concerns.