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Nitrous acid (HONO) serves as the primary source of OH radicals in the atmosphere, exerting significant impacts on atmospheric secondary pollution. The heterogeneous reactions of NO 2 on surfaces and photolysis of particulate nitrate or adsorbed nitric acid are important sources of atmospheric HONO, yet the corresponding kinetic parameters based on laboratory investigations and field observations exhibit considerable variations. In this study, we developed an explainable machine learning model to analyze the HONO budget using two years of summer urban supersite observations. By integrating chemical mechanisms and feature engineering into our machine learning model, we assessed the contributions of different sources to HONO and inferred the kinetic parameters for the primary HONO formation pathways, thereby partially addressing the limitations associated with predetermined rate coefficients. Our findings revealed that the primary source of daytime HONO in the summer was the photolysis of nitric acid adsorbed on both aerosol and ground surfaces, accounting for over 40% of its unknown sources. This was followed by the photoenhanced heterogeneous conversion of NO 2 and the photolysis of particulate nitrate. Additionally, we derived the corresponding kinetic parameters, analyzed their influencing factors, and confirmed that machine learning methods hold great potential for the study of the HONO budget.

The health impact of heavy metals in atmospheric PM 2.5 has garnered increasingly widespread attention. We have collected PM 2.5 samples in a typical city (Kaifeng) within the Central Plains Urban Agglomeration in China during winter and measured the mass concentration of PM 2.5 -bound heavy metals. The pollution of As and Cr in the urban atmosphere requires significant attention. As PM 2.5 concentrations increased, the enrichment factors (EFs) of Mn, Cu, Zn, As, and Pb also rose, suggesting a growing contribution from anthropogenic emissions. The analysis showed that the hazard quotient (HQ) for the non-heating and heating periods (HQ < 1) did not result in a cumulative non-carcinogenic health risk to humans. Regarding carcinogenic effects, As and Cr exhibit significant carcinogenic impacts on both children and adults (ELCR>1 × 10 -6 ), indicating that the carcinogenic risks posed by As and Cr under PM 2.5 exposure in Kaifeng could not be overlooked. It was found that industrial and biomass combustion are the primary sources of carcinogenic risk in Kaifeng city. From the non-heating to the heating period, the industrial carcinogenic risk increased from 37.12 % to 43.39 %, while the contribution of biomass burning remained at 25 %. This result was strongly correlated with the high proportions of heavy metal elements such as As, Mn, Pb, and Ni from the metal refinery industry. The results of this study revealed the equally important source of heavy metals, compared to coal combustion in North China Plain. In addition to residential coal combustion, industrial emissions are a major source of PM 2.5 -bound heavy metals in Kaifeng, contributing significantly to overall air pollution and providing a useful reference to mitigating human health risks in the area., 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 Elsevier B.V. All rights reserved.)

Air quality models (AQMs) are pivotal in forecasting air quality and shaping pollution control strategies. Nonetheless, the effectiveness of AQMs is often compromised in many cities due to the absence of accurate local emission inventories. To address this gap, this study presents a novel AQM-ready emission inventory generation technique with iterative optimization ability for city-scale applications in China. An efficient emission processing tool was introduced in this study, which utilizes the High-Resolution Multi-resolution Emission Inventory for China (HR-MEIC) as input. Using environmental observations and a region map, the tool can justify emissions of different regions iteratively. With the iterative optimization method, the model performance can be notably improved even without local emissions. The optimization was realized by splitting model-ready emissions into different regions and adjusting the emissions using scale factors calculated with the modeling results and the observations of each region. This methodology was applied to the Eight Cities in the Chengdu Plain (CP8C), located in the western margin of Sichuan Basin with complex topography and meteorological conditions, southwestern China, monthly throughout 2023. Air quality modeling was carried out using Weather Forecast and Research Model (WRF) and the Community Multiscale Air Quality Model (CMAQ). The results showed that the optimization acquired a good performance after five cycles for PM 2.5 and NO 2 , with correlation coefficients (R values) surging from 0.62 and 0.37 to 0.77 and 0.73, respectively, while their normalized mean bias (NMB) substantially decreased from 22.8 % and 100.4 % to 3.6 % and 3.3 %. The underestimation on O 3 concentration was also improved by the optimization, although enhancements in O 3 modeling remained modest. This technique provides an easy-to-copy method to generate reasonable AQM-ready emission files with open emission data and observation data, which would be beneficial for the cities' air quality forecast in cities without local emission inventories., 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.)

Emissions of nitrogen oxides (NOx) are a dominant contributor to ambient nitrogen dioxide (NO 2 ) concentrations, but the quantitative relationship between them at an intracity scale remains elusive. The Chengdu 2021 FISU World University Games (July 22 to August 10, 2023) was the first world-class multisport event in China after the COVID-19 pandemic which led to a substantial decline in NOx emissions in Chengdu. This study evaluated the impact of variations in NOx emissions on NO 2 concentrations at a fine spatiotemporal scale by leveraging this event-driven experiment. Based on ground-based and satellite observations, we developed a data-driven approach to estimate full-coverage hourly NO 2 concentrations at 1 km resolution. Then, a random-forest-based meteorological normalization method was applied to decouple the impact of meteorological conditions on NO 2 concentrations for every grid cell, the resulting data were then compared with the timely bottom-up NOx emissions. The SHapley-Additive-exPlanation (SHAP) method was employed to delineate the individual contributions of meteorological factors and various emission sources to the changes in NO 2 concentrations. According to the full-coverage meteorologically normalized NO 2 concentrations, a decrease in NOx emissions and favorable meteorological conditions accounted for 80 % and 20 % of the NO 2 reduction, respectively, across Chengdu city during the control period. Within the strict control zone, a 30 % decrease in the meteorologically normalized NO 2 concentrations was observed during the control period. The normalized NO 2 concentrations demonstrated a strong correlation with NOx emissions (R = 0.96). Based on the SHAP analysis, traffic emissions accounted for 73 % of the reduction in NO 2 concentrations, underscoring the significance of traffic control measures in improving air quality in urban areas. This study provides insights into the relationship between NO 2 concentrations and NOx emissions using real-world data, which implies the substantial benefits of vehicle electrification for sustainable urban development., 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 Elsevier B.V. All rights reserved.)

To mitigate the societal impact of the COVID-19 pandemic, China implemented long-term restrictive measures. The sudden liberalization at the end of 2022 disrupted residents' daily routines, making it scientifically intriguing to explore its effect on air quality. Taking Chongqing City in Southwest China as an example, we examined the impact of restriction liberalization on air quality, identified potential sources of pollutants, simulated the effects of abrupt anthropogenic control relaxation using a Random Forest Model, and applied an optimized model to predict the post-liberalization pollutant concentrations. The results showed increases in PM 2.5 (72.3%), PM 10 (67.7%), and NO 2 (21.9%) concentrations, while O 3 concentration decreased by 20.5%. Although potential pollution source areas contracted, pollution levels intensified with northeastern Sichuan, interior Chongqing, and northern Guizhou being major contributors to pollutant emissions. Anthropogenic emissions accounted for 26.7 ~ 33% changes in PM 2.5 and PM 10 concentrations while meteorological conditions contributed to 40.2 ~ 43.3% variations observed during the period. The optimized model demonstrated a correlation between predicted and observed values with R 2 ranging from 0.70 to 0.89, enabling accurate prediction of post-liberalization pollutant concentrations. This study can enhance our understanding regarding the impact of sudden social lockdown relaxation events on air quality while providing support for urban air pollution prevention., (© 2024. The Author(s), under exclusive licence to Springer Nature Switzerland AG.)

Top-down estimates of fossil fuel CO 2 (FFCO 2 ) emissions are crucial for tracking emissions and evaluating mitigation strategies. However, their practical application is hindered by limited data coverage and overreliance on NOx-to-CO 2 emission ratios from emission inventories. We developed the Machine Learning-Driven Mapping Satellite-based XCO 2en (ML-MSXE) model using the column-averaged dry-air mole fraction of CO 2 enhancement (XCO 2en ) derived from OCO-2 and OCO-3 measurements to reconstruct the XCO 2en distribution for monitoring FFCO 2 emissions. Compared to the previous Machine Learning-Driven Deriving XCO 2en from Mapped XCO 2 (ML-DXEMX) model, ML-MSXE enhances the utilization of TROPOMI NO 2 measurements, increasing their relative contribution from 4.3 to 21.7%, thereby improving XCO 2en reconstruction accuracy and enhancing the ability to track emissions. Despite the COVID-19 lockdown, XCO 2en levels in China rose from 1.33 ± 1.06 in 2019 to 1.39 ± 1.01 ppm in 2021. In February 2020, while the national average rate of XCO 2en decline (16.3%) aligned with the reduction in FFCO 2 emissions estimated by inventories, XCO 2en further revealed varying rates of decline between cities. Furthermore, the spatial distribution of XCO 2en identified hotspots where FFCO 2 emissions might be underestimated by inventories. This study presents a space-based approach for monitoring FFCO 2 emissions, offering valuable insights for assessing carbon neutrality progress and informing policy.

The 31st FISU Summer World University Games (SWUG) was held in Chengdu, southwestern China, from July 22 to August 8, 2023. A series of control measures were carried out to ensure good air quality during the SWUG, providing an opportunity to investigate the atmospheric behaviors of light-absorbing aerosols under such a substantial disturbance caused by the control measures. To assess the impacts of emission controls on primary pollutants, a field campaign was conducted at a rural site in Chengdu to investigate the characterization of equivalent black carbon (eBC). The changes of eBC concentrations before, during, and after the SWUG were characterized. The sources of eBC were resolved, and the impacts of atmospheric processes on the absorption capacity were also investigated. During the SWUG, the eBC concentration decreased by 12.1 % and 25.3 % compared with those before and after the SWUG. A fossil fuel combustion (eBC ff ) and a biomass burning (eBC bb ) originated eBC were resolved using the aethalometer model. Both eBC ff and eBC bb decreased during the SWUG, indicating the effectiveness of control measures. After the SWUG, the influence of biomass burning emissions became more and more significant, and the contribution of brown carbon (BrC) to light absorption at 370-660 nm increased by 52, 19, 7, 6, and 17 % compared to those during the SWUG. As the biomass burning emitted aerosols aged, the absorption Ångström exponent and b abs (BrC 370nm ) decreased gradually, which was mainly due to the photobleaching of the chromophores during the daytime. eBC ff was mainly affected by strong wind, while high eBC bb concentration was mainly attributed to the gradual accumulation of biomass-burning emissions near the observation site. The results show the significant reduction of eBC with the implementation of the air pollution mitigation campaign, and provide insights on the impacts of atmospheric processes on BC optical properties during summertime., 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 Elsevier Ltd. All rights reserved.)

The complex air pollution driven by both Ozone (O 3 ) and fine particulate matter (PM 2.5 ) significantly influences the air quality in the Sichuan Basin (SCB). Understanding the O 3 formation during autumn and winter is necessary to understand the atmospheric oxidative capacity. Therefore, continuous in-site field observations were carried out during the late summer, early autumn and winter of 2020 in a rural area of Chongqing. The total volatile organic compounds (VOCs) concentration reported by a Proton-Transfer-Reaction Time-of-Flight Mass Spectrometry (PTR-ToF-MS) were 13.66 ± 9.75 ppb, 5.50 ± 2.64 ppb, and 9.41 ± 5.11 ppb in late summer, early autumn and winter, respectively. The anthropogenic VOCs (AVOCs) and biogenic VOCs (BVOCs) were 8.48 ± 7.92 ppb and 5.18 ± 2.99 ppb in late summer, 3.31 ± 1.89 ppb and 2.19 ± 0.93 ppb in autumn, and 6.22 ± 3.99 ppb and 3.20 ± 1.27 ppb in winter. A zero-dimensional atmospheric box model was employed to investigate the sensitivity of O 3 -precursors by relative incremental reactivity (RIR). The RIR values of AVOCs, BVOCs, carbon monoxide (CO), and nitrogen oxides (NO x ) were 0.31, 0.71, 0.09, and -0.36 for late summer, 0.24, 0.59, 0.22, and -0.38 for early autumn, and 0.30, 0.64, 0.33 and -0.70 for winter, and the results showed that the O 3 formation of sampling area was in the VOC-limited region, and O 3 was most sensitive to BVOCs (with highest RIR values, > 0.6). This study can be helpful in understanding O 3 formation and interpreting the secondary formation of aerosols in the winter., 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 © 2023. Published by Elsevier B.V.)

Severe air pollution tends to occur under stagnant weather conditions. This study focused on the occurrence and formation of PM 2.5 -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/m 3 versus 12.3-39.9 ng/m 3 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 O 3 concentration at T < 22 °C but sustained at a high level despite the fluctuation of temperature and O 3 concentration at T > 22 °C. Elevated NO 2 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 NO 2 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 NO 2 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., 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 Elsevier B.V. All rights reserved.)

Surface NO 2 pollution can result in serious health consequences such as cardiovascular disease, asthma, and premature mortality. Due to the extensive spatial variation in surface NO 2 , the spatial resolution of a NO 2 dataset has a significant impact on the exposure and health impact assessment. There is currently no long-term, high-resolution, and publicly available NO 2 dataset for China. To fill this gap, this study generated a NO 2 dataset named RBE-DS-NO2 for China during 2005-2020 at 1 km and daily resolution. We employed the robust back-extrapolation via a data augmentation approach (RBE-DA) to ensure the predictive accuracy in back-extrapolation before 2013, and utilized an improved spatial downscaling technique (DS) to refine the spatial resolution from 10 km to 1 km. Back-extrapolation validation based on 2005-2012 observations from sites in Taiwan province yielded an R 2 of 0.72 and RMSE of 10.7 μg/m 3 , while cross-validation across China during 2013-2020 showed an R 2 of 0.73 and RMSE of 9.6 μg/m 3 . RBE-DS-NO2 better captured spatiotemporal variation of surface NO 2 in China compared to the existing publicly available datasets. Exposure assessment using RBE-DS-NO2 show that the population living in non-attainment areas (NO 2  ≥ 30 μg/m 3 ) grew from 376 million in 2005 to 612 million in 2012, then declined to 404 million by 2020. Unlike this national trend, exposure levels in several major cities (e.g., Shanghai and Chengdu) continued to increase during 2012-2020, driven by population growth and urban migration. Furthermore, this study revealed that low-resolution dataset (i.e., the 10 km intermediate dataset before the downscaling) overestimated NO 2 levels, due to the limited specificity of the low-resolution model in simulating the relationship between NO 2 and the predictor variables. Such limited specificity likely biased previous long-term NO 2 exposure and health impact studies employing low-resolution datasets. The RBE-DS-NO2 dataset enables robust long-term assessments of NO 2 exposure and health impacts in China., 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 Elsevier Inc. All rights reserved.)

The ozone (O 3 ) pollution in China drew lots of attention in recent years, and the Sichuan Basin (SCB) was one of the regions confronting worsening O 3 pollution problem. Many previous studies have shown that regional transport is an important contributor to O 3 pollution. However, very few features of the O 3 profile during transport have been reported, especially in the border regions between different administrative divisions. In this study, we conducted tethered balloon soundings in SCB during the summer of 2020 and captured a nocturnal O 3 transport event during the campaign. Vertically, the O 3 transport occurred in the bottom of the residual layer, between 200 and 500 m above ground level. Horizontally, the transport pathway was directed from southeast to northwest based on the analysis of the wind field and air mass trajectories. The effect of transport in the residual layer on the surface O 3 concentration was related to the spatial distribution of O 3 . For cities with high O 3 concentrations in the upwind region, the transport process would bring clean air masses and abate pollution. For downwind lightly polluted cities, the transport process would slow down the decreasing or even increase the surface O 3 concentration during the night. We provided observational facts on the profile features of a transboundary O 3 transport event between two provincial administrative divisions, which implicated the importance of joint prevention and control measures. However, the sounding parameters were limited and the quantitative analysis was preliminary, more integrated, and thorough studies of this topic were called for in the future., 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 © 2023. Published by Elsevier B.V.)

The chemical composition of acid rain and its impact on lake water chemistry in Chongqing, China, from 2000 to 2020 were studied in this study. The regional acid rain intensity is affected jointly by the acid gas emissions and the neutralization of alkaline substances. The pH of precipitation experienced three stages of fluctuating decline, continuous improvement, and a slight correction. Precipitation pH showed inflection points in 2010, mainly due to the total control actions of SO 2 and NO x implemented in 2011. The total ion concentrations in rural areas and urban areas were 489.08 µeq/L and 618.57 µeq/L, respectively. The top four ions were SO 4 2- , Ca 2+ , NH 4 + and NO 3 - , which accounted for more than 90% of the total ion concentration, indicating the anthropogenic effects. Before 2010, SO 4 2- fluctuated greatly while NO 3 - continued to rise; however, after 2010, both SO 4 2- and NO 3 - began to decline rapidly, with the rates of -12.03 µeq/(L·year) and -4.11 µeq/(L·year). Because the decline rate of SO 4 2- was 2.91 times that of NO 3 - , the regional acid rain has changed from sulfuric acid rain to mixed sulfuric and nitric acid rain. The lake water is weakly acidic, with an average pH of 5.86, and the acidification frequency is 30.00%. Acidification of lake water is jointly affected by acid deposition and acid neutralization capacity of lake water. Acid deposition has a profound impact on water acidification, and nitrogen (N) deposition, especially reduced N deposition, should be the focus of future research., 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 © 2023. Published by Elsevier B.V.)

Carbonaceous aerosols play a vital role in global climate patterns due to their potent light absorption capabilities. However, the light absorption enhancement effect (E abs ) of black carbon (BC) is still subject to great uncertainties due to factors such as the mixing state, coating material, and particle size distribution. In this study, fine particulate matter (PM 2.5 ) samples were collected in Chengdu, a megacity in the Sichuan Basin, during the winter of 2020 and 2021. The chemical components of PM 2.5 and the light absorption properties of BC were investigated. The results revealed that secondary inorganic aerosols and carbonaceous aerosols were the dominant components in PM 2.5 . Additionally, the aerosol filter filtration-dissolution (AFD) treatment could improve the accuracy of measuring elemental carbon (EC) through thermal/optical analysis. During winter in Chengdu, the absorption enhancement values of BC ranged between 1.56 and 2.27, depending on the absorption wavelength and the mixing state of BC and non-BC materials. The presence of internally mixed BC and non-BC materials significantly contributed to E abs , accounting for an average of 68 % at 405 nm and 100 % at 635 nm. The thickness of the BC coating influenced E abs , displaying an increasing-then-decreasing trend. This trend was primarily attributed to the hygroscopic growth and dehydration shrinkage of particulate matter. Nitrate, as the major component of BC coating, played a crucial role in the lensing effect and exhibited fast growth during variation in E abs . By combining the results from PMF, we identified the secondary formation and vehicle emission as the primary contributors to E abs . Consequently, this study can provide valuable insights into the optical parameters, which are essential for assessing the environmental quality, improving regional atmospheric conditions, and formulating effective air pollution control strategies., 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 Elsevier B.V. All rights reserved.)

Forty-six percent of the world's population resides in rural areas, the majority of whom belong to vulnerable groups. They mainly use cheap solid fuels for cooking and heating, which release a large amount of PM 2.5 and cause adverse effects to human health. PM 2.5 exhibits urban-rural differences in its health risk to the respiratory system. However, the majority of research on this issue has focused on respiratory diseases induced by atmospheric PM 2.5 in urban areas, while rural areas have been ignored for a long time, especially the pathogenesis of respiratory diseases. This is not helpful for promoting environmental equity to aid vulnerable groups under PM 2.5 pollution. Thus, this study focuses on rural atmospheric PM 2.5 in terms of its chemical components, toxicological effects, respiratory disease types, and pathogenesis, represented by PM 2.5 from rural areas in the Sichuan Basin, China (Rural SC-PM 2.5 ). In this study, organic carbon is the most significant component of Rural SC-PM 2.5 . Rural SC-PM 2.5 significantly induces cytotoxicity, oxidative stress, and inflammatory response. Based on multiomics, bioinformatics, and molecular biology, Rural SC-PM 2.5 inhibits ribonucleotide reductase regulatory subunit M2 (RRM2) to disrupt the cell cycle, impede DNA replication, and ultimately inhibit lung cell proliferation. Furthermore, this study supplements and supports the epidemic investigation. Through an analysis of the transcriptome and human disease database, it is found that Rural SC-PM 2.5 may mainly involve pulmonary hypertension, sarcoidosis, and interstitial lung diseases; in particular, congenital diseases may be ignored by epidemiological surveys in rural areas, including tracheoesophageal fistula, submucous cleft of the hard palate, and congenital hypoplasia of the lung. This study contributes to a greater scientific understanding of the health risks posed by rural PM 2.5 , elucidates the pathogenesis of respiratory diseases, clarifies the types of respiratory diseases, and promotes environmental equity., Competing Interests: Declaration of competing interest The authors confirm that they have no known competing financial interests or personal relationships which might have influenced the work presented in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Remote sensing data from the Ozone Monitoring Instrument (OMI) and the TROPOspheric Monitoring Instrument (TROPOMI) play important roles in estimating surface nitrogen dioxide (NO 2 ), but few studies have compared their differences for application in surface NO 2 reconstruction. This study aims to explore the effectiveness of incorporating the tropospheric NO 2 vertical column density (VCD) from OMI and TROPOMI (hereafter referred to as OMI and TROPOMI, respectively, for conciseness) for deriving surface NO 2 and to apply the resulting data to revisit the spatiotemporal variations in surface NO 2 for Beijing over the 2005-2020 period during which there were significant reductions in nitrogen oxide emissions. In the OMI versus TROPOMI performance comparison, the cross-validation R 2 values were 0.73 and 0.72, respectively, at 1 km resolution and 0.69 for both at 100 m resolution. The comparisons between satellite data sources indicate that even though TROPOMI has a finer resolution it does not improve upon OMI for deriving surface NO 2 at 1 km resolution, especially for analyzing long-term trends. In light of the comparison results, we used a hybrid approach based on machine learning to derive the spatiotemporal distribution of surface NO 2 during 2005-2020 based on OMI. We had novel, independent passive sampling data collected weekly from July to September of 2008 for hindcasting validation and found a spatiotemporal R 2 of 0.46 (RMSE = 7.0 ppb). Regarding the long-term trend of surface NO 2 , the level in 2008 was obviously lower than that in 2007 and 2009, as expected, which was attributed to pollution restrictions during the Olympic Games. The NO 2 level started to steadily decline from 2015 and fell below 2008's level after 2017. Based on OMI, a long-term and fine-resolution surface NO 2 dataset was developed for Beijing to support future environmental management questions and epidemiological research., 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 © 2023 Elsevier B.V. All rights reserved.)

Nitrous acid (HONO) is an established precursor of hydroxyl (OH) radical and has significant impacts on the formation of PM 2.5 and O 3 . Despite extensive research on HONO observation in recent years, knowledge regarding its sources and sinks in urban areas remains inadequate. In this study, we monitored the atmospheric concentrations of HONO and related pollutants, including gaseous nitric acid and particulate nitrate, simultaneously at a supersite in downtown Chengdu, a megacity in southwestern China during spring, when was chosen due to its tolerance for both PM 2.5 and O 3 pollution. Furthermore, we employed the random forest model to fill the missing data of HONO, which exhibited good predictive performance (R 2  = 0.96, RMSE = 0.36 ppbv). During this campaign, the average mixing ratio of HONO was measured to be 1.0 ± 0.7 ppbv. Notably, during periods of high O 3 and PM 2.5 concentrations, the mixing ratio of HONO was >50 % higher compared to the clean period. We developed a comprehensive parameterization scheme for the HONO budget, and it performed well in simulating diurnal variations of HONO. Based on the HONO budget analysis, we identified different mechanisms that dominate HONO formation at different times of the day. Vehicle emissions and NO 2 heterogeneous conversions were found to be the primary sources of HONO during nighttime (21.0 %, 30.2 %, respectively, from 18:00 to 7:00 the next day). In the morning (7:00-12:00), NO 2 heterogeneous conversions and the reaction of NO with OH became the main sources (35.0 %, 32.2 %, respectively). However, in the afternoon (12:00-18:00), the heterogeneous photolysis of HNO 3 on PM 2.5 was identified as the most substantial source of HONO (contributing 52.5 %). This study highlights the significant variations in primary HONO sources throughout the day., 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 © 2023. Published by Elsevier B.V.)

Terrain effect is challenging for understanding atmospheric environment changes under complex topography. This study targets the Sichuan Basin (SCB), a deep basin isolated by plateaus and mountains in Southwest China, by employing WRF-Chem with integrated process rates (IPR) analysis to characterize the terrain-driven seasonal variations of tropospheric ozone (O 3 ) with atmospheric physical and chemical processes. Results show that the basin terrain exerts reversed impacts on regional air quality changes by aggravating summertime and alleviating wintertime near-surface O 3 with the relative contributions oscillating seasonally between -40% and 40% in SCB. Similarly, a seasonal shift of vertical O 3 structures is dominated by summertime positive and wintertime negative changes in the lower troposphere induced by basin terrain. The key contributions of atmospheric process to near-surface O 3 are identified with vertical and horizontal transport, which is dominated by basin terrain with intensifying seasonal and diurnal variations. With the existence of basin, the daytime O 3 productions at the near-surface layer are elevated in months of warm seasons (April and July) but inhibited in the cold seasons (October and January), presenting a seasonal transition of primary factor from meteorology to aerosol-radiation forcing on photochemical reactions. Driven by plateau-basin thermodynamic forcing, horizontal O 3 transport between the SCB and eastern TP is enhanced by mountain-plains solenoid (MPS), and even nocturnal O 3 -rich layers contribute to the impacts of vertical exchange on near-surface O 3 levels. The terrain effects of deep basin under the interaction of Asian monsoons and westerlies could jointly change atmospheric physical and chemical processes to construct the seasonal and diurnal O 3 evolution patterns over the SCB region., 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 © 2023. Published by Elsevier Ltd.)

Volatile organic compounds (VOCs) are significant precursors to photochemical pollution. However, reactive VOC species are easily oxidized during transportation, resulting in a systematic underestimate of the measured concentrations. To address this, we applied an improved calculation method to correct the measured VOC concentrations into photochemical initial concentrations (PICs) in Chengdu, a megacity in the Sichuan Basin, China, which is highly vulnerable to complex pollution. In this study, 56 VOC species on the Photochemical Assessment Monitor Station (PAMS) target list were quantitatively monitored throughout all four seasons. Comparing to directly measured values, photochemically initialized total mixing ratios of VOCs increased by 18.6 % in general. The photochemical loss percentages of alkenes and aromatics were prominent in summer (68.6 %, 28.7 %) and spring (65.9 %, 24.7 %), respectively. Furthermore, we examined contributions of VOCs to atmospheric oxidation capacity (AOC) depending on PICs and found that maximum daily total AOC showed a surge in spring and summer. Besides hydroxyl radicals, daytime O 3 in spring and late-afternoon nitrate radicals in summer were essential for AOC with PICs. As expected, alkenes and aromatics dominated PIC-based ozone formation potentials (OFPs). Furthermore, contribution of alkenes to secondary organic aerosol formation potentials reached 15.5 % and 7.6 % in spring and summer, respectively. Using positive matrix factorization model, we identified five VOC sources including vehicular exhaust, industrial emissions, solvent usage, biogenic sources, and liquefied petroleum gas/natural gas use. Based on PICs, biogenic sources were significantly underestimated in spring and summer. Meanwhile, m,p-xylene from solvent usage and isoprene from biogenic sources were the primary contributors to OFPs. Consequently, these results emphasize the significance of photochemically oxidized VOC concentrations, especially for reactive species in typical seasons., 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 © 2023 Elsevier B.V. All rights reserved.)

Maternal PM 2.5 exposure has been identified as a potential risk factor for preterm birth, yet the inconsistent findings on the susceptible exposure windows may be partially due to the influence of gaseous pollutants. This study aims to examine the association between PM 2.5 exposure and preterm birth during different susceptible exposure windows after adjusting for exposure to gaseous pollutants. We collected 2,294,188 records of singleton live births from 30 provinces of China from 2013 to 2019, and the gridded daily concentrations of air pollutants (including PM 2.5 , O 3 , NO 2 , SO 2 , and CO) were derived by using machine learning models for assessing individual exposure. We employed logistic regression to develop single-pollutant models (including PM 2.5 only) and co-pollutant models (including PM 2.5 and a gaseous pollutant) to estimate the odds ratio for preterm birth and its subtypes, with adjustment for maternal age, neonatal sex, parity, meteorological conditions, and other potential confounders. In the single-pollutant models, PM 2.5 exposure in each trimester was significantly associated with preterm birth, and the third trimester exposure showed a stronger association with very preterm birth than that with moderate to late preterm birth. The co-pollutant models revealed that preterm birth might be significantly associated only with maternal exposure to PM 2.5 in the third trimester, and not with exposure in the first or second trimester. The observed significant associations between preterm birth and maternal PM 2.5 exposure in the first and second trimesters in single-pollutant models might primarily be influenced by exposure to gaseous pollutants. Our study provides evidence that the third trimester may be the susceptible window for maternal PM 2.5 exposure and preterm birth. The association between PM 2.5 exposure and preterm birth could be influenced by gaseous pollutants, which should be taken into consideration when evaluating the impact of PM 2.5 exposure on maternal and fetal health., 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 © 2023 Elsevier B.V. All rights reserved.)

PM 2.5 seriously endangers human health, and its mutagenicity is considered an important pathogenic mechanism. However, the mutagenicity of PM 2.5 is mainly determined by traditional bioassays, which are limited in the large-scale identification of mutation sites. Single nucleoside polymorphisms (SNPs) can be used for the large-scale analysis of DNA mutation sites but have not yet been used on the mutagenicity of PM 2.5 . The Chengdu-Chongqing Economic Circle is one of China's four major economic circles and five major urban agglomerations, and the relationship between the mutagenicity of PM 2.5 and ethnic susceptibility in this circle remains unclear. In this study, the representative samples are PM 2.5 from Chengdu in summer (CDSUM), Chengdu in winter (CDWIN), Chongqing in summer (CQSUM) and Chongqing in winter (CQWIN) respectively. PM 2.5 from CDWIN, CDSUM and CQSUM induce the highest levels of mutation in the regions of exon/5'Utr, upstream/splice site and downstream/3'Utr respectively. PM 2.5 from CQWIN, CDWIN and CDSUM induce the highest ratio of missense, nonsense and synonymous mutation respectively. PM 2.5 from CQWIN and CDWIN induce the highest transition and transversion mutations respectively. The ability of PM 2.5 from the four groups to induce disruptive mutation effects is similar. For ethnic susceptibility, PM 2.5 in this economic circle is more likely to induce DNA mutation in Chinese Dai from Xishuangbanna among Chinese ethnic groups. PM 2.5 from CDSUM, CDWIN, CQSUM and CQWIN may particularly tend to induce Southern Han Chinese, Dai in Xishuangbanna, Dai in Xishuangbanna and Southern Han Chinese respectively. These findings may assist in the development of a new method for analyzing the mutagenicity of PM 2.5 . Moreover, this study not only promotes attention to ethnic susceptibility to PM 2.5 , but also introduces public protection policies for the susceptible population., 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 © 2023 Elsevier B.V. All rights reserved.)

In recent years, the annual mean concentration of PM 2.5 has decreased in Chengdu, China; however, atmospheric visibility has not improved accordingly. Low-visibility events occurred even when the PM 2.5 mass concentrations were below the national ambient air quality secondary standard (daily mean concentration, 75 μg/m 3 ). In this study, the non-linear relationship between PM 2.5 and visibility was analyzed under different NO 3 - mass fractions in PM 2.5 based on 2-year field observation data. The results indicated that NO 3 - formation contributed to particulate pollution events and reduced atmospheric visibility. Multiple linear regression was used to propose a localized reconstruction equation for the light-scattering coefficient. According to the maximum likelihood estimation method and log-transformed residuals, the mass scattering coefficients (MSEs) of organic matter (OM), NH 4 NO 3 , and (NH 4 ) 2 SO 4 in Chengdu were 7.42, 3.83, and 3.80, respectively. OM and NH 4 NO 3 contributed to more than 50% of the light-extinction coefficient (b ext ). NH 4 NO 3 was the main pollutant causing the substantial increase in b ext . Chengdu has a high relative humidity (annual mean 70%), and under such conditions, the contribution of NH 4 NO 3 to b ext was considerably enhanced through hygroscopic growth and heterogeneous reactions. This study estimated the localized MSEs of OM, NH 4 NO 3 , and (NH 4 ) 2 SO 4 in Chengdu and emphasized that effective control measures to reduce nitrate and its precursors could simultaneously ameliorate air quality and visibility in humid regions with poor atmospheric visibility., 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 © 2023 Elsevier Ltd. All rights reserved.)

Air pollutants suspended in the atmosphere have a large impact on air quality, climate, and human health. As one of the important populated and industrialized regions in China, the Sichuan Basin (SCB) has confronted severe air pollution in recent years. Previous studies have shown that regional transport played a significant role in the formation of regional pollution in the SCB, particularly in the southern basin. Using Yibin and Zigong as representative receptor cities, we further identified the transport channels affecting the southern basin by conducting gridded dispersion simulations. A total of seven channels were identified, including three for cyclonic transport, three through the mountainous areas between the Longquan Mountain and the Huaying Mountain, and one along the Yangtze River. Varying seasonal distributions of their occurrence frequencies were observed. Furthermore, observational evidence for several universal channels was presented during a typical transport case. The transport pathways identified in this study can guide the planning of regional distribution of emission sources and the measures for regional joint prevention and control of air pollution.

Nowadays, the fine particle pollution is still severe in some megacities of China, especially in the Sichuan Basin, southwestern China. In order to understand the causes, sources, and impacts of fine particles, we collected PM 2.5 samples and analyzed their chemical composition in typical months from July 2018 to May 2019 at an urban and a suburban (background) site of Chengdu, a megacity in this region. The daily average concentrations of PM 2.5 ranged from 5.6-102.3 µg/m 3 and 4.3-110.4 µg/m 3 at each site. Secondary inorganics and organic matters were the major components in PM 2.5 at both sites. The proportion of nitrate in PM 2.5 has exceeded sulfate and become the primary inorganic component. SO 2 was easier to transform into sulfate in urban areas because of Mn-catalytic heterogeneous reactions. In contrast, NO 2 was easily converted in suburbs with high aerosol water content. Furthermore, organic carbon in urban was much greater than that in rural, other than elemental carbon. Element Cr and As were the key cancer risk drivers. The main sources of PM 2.5 in urban and suburban areas were all secondary aerosols (42.9%, 32.1%), combustion (16.0%, 25.2%) and vehicle emission (15.2%, 19.2%). From clean period to pollution period, the contributions from combustion and secondary aerosols increased markedly. In addition to tightening vehicle controls, urban areas need to restrict emissions from steel smelters, and suburbs need to minimize coal and biomass combustion in autumn and winter., (Copyright © 2022. Published by Elsevier B.V.)

To study the emission characteristics of typical construction machinery in Chengdu, 12 construction machinery (excavators, bulldozers, loaders, and forklifts) under idling mode, moving mode, and working mode, were tested using a portable emission measurement system (PEMS). Under three operating modes, the typical construction machinery in the working mode was higher in the fuel-based average emission factors of PM 2.5 and NO x, while the fuel-based average emission factors of HC and CO were higher in idling mode. Integrated the results of investigation on ownership and activity levels of construction machinery, an exhaust emission inventory of typical construction machinery of Chengdu in 2018 was established according to the recommendation method. The annual emission of PM 2.5 , NO x , HC, and CO were 1.67 × 10 6 , 1.61 × 10 8 , 3.83 × 10 6 , and 1.26 × 10 7  kg, respectively, and the excavator contributed the maximum emissions, accounting for an average proportion of 43.95%. The emission of construction machinery in Chengdu exhibited a clear monthly trend, with the highest from April to October and the lowest from November to March. In addition, the exhaust emissions presented an obvious spot-like characteristics, and the high-value areas were mainly concentrated in the surrounding suburban counties such as Shuangliu Wenjiang etc. To reduce pollution from construction machinery and improve the quality of the atmospheric environment, more effective measures on housing construction and municipal construction should be taken in those districts in Chengdu., (Copyright © 2022. Published by Elsevier B.V.)

Carbonaceous aerosols pose significant climatic impact, however, their sources and respective contribution to light absorption vary and remain poorly understood. In this work, filter-based PM 2.5 samples were collected in winter of 2021 at three urban sites in Yibin, a fast-growing city in the south of Sichuan Basin, China. The composition characteristics of PM 2.5 , light absorption and source of carbonaceous aerosol were analyzed. The city-wide average concentration of PM 2.5 was 87.4 ± 31.0 μg/m 3 in winter. Carbonaceous aerosol was the most abundant species, accounting for 42.5% of the total PM 2.5 . Source apportionment results showed that vehicular emission was the main source of PM 2.5 during winter, contributing 34.6% to PM 2.5 . The light absorption of black carbon (BC) and brown carbon (BrC) were derived from a simplified two-component model. We apportioned the light absorption of carbonaceous aerosols to BC and BrC using the Least Squares Linear Regression with optimal angstrom absorption exponent of BC (AAE BC ). The average absorption of BC and BrC at 405 nm were 51.6 ± 21.5 Mm -1 and 17.7 ± 8.0 Mm -1 , respectively, with mean AAE BC  = 0.82 ± 0.02. The contribution of BrC to the absorption of carbonaceous reached 26.1% at 405 nm. Based on the PM 2.5 source apportionment and the mass absorption cross-section (MAC) value of BrC at 405 nm, vehicle emission was found to be the dominant source of BrC in winter, contributing up to 56.4%. Therefore, vehicle emissions mitigation should be the primary and an effective way to improve atmospheric visibility in this fast-developing city., 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 Ltd. All rights reserved.)

Chengdu-Chongqing Economic Circle (CD-CQ Economic Circle) is one of China's four major economic circles and five major urban agglomerations located in Southwest China's Sichuan Basin. The CD-CQ Economic Circle, with its strong economic development and dense population, suffers from severe PM 2.5 pollution, which is known to cause chronic and acute respiratory ailments. This study examined the lung disease-related hub genes, functions, and pathways that are affected by PM 2.5 in summer and winter in the two central megacities of Chengdu and Chongqing. PM 2.5 frequently activates lung disease-associated hub genes, most notably the transcription factor TP53. TP53 interacts with the majority of lung disease-related genes and regulates important and commonly occurring biological functions and pathways, including gland development, aging, reactive oxygen species metabolic process, the response to oxygen levels, and fluid shear stress, among others. Thus, PM 2.5 has been shown to target TP53 for regulating lung disease genes/functions/pathways, thereby influencing the occurrence and progression of lung illnesses. Notably, PM 2.5 may be associated with small cell carcinoma of the lung due to the high number of lung disease genes, hub genes, critical functions, and pathways enriched in this kind of cancer. These findings shed fresh light on the molecular pathophysiology of PM 2.5 pollution on the respiratory system in the CD-CQ Economic Circle and aid in the development of novel techniques for mitigating PM 2.5 pollution-associated respiratory illness., (Copyright © 2022. Published by Elsevier Ltd.)

Until recently, Northern China was one of the most SO 2 polluted regions in the world. The lack of long-term and spatially resolved surface SO 2 data hinders retrospective evaluation of relevant environmental policies and human health effects. This study aims to derive the spatiotemporal distribution of surface SO 2 across Northern China during 2005-2019. As "concept drift" causes substantial estimation bias in back-extrapolation, we propose a new approach named the robust back-extrapolation via data augmentation approach (RBE-DA) to model the long-term surface SO 2 . The results show that the population-weighted regional SO 2 ([SO 2 ] pw ) increased from 2005 to 2007 and decreased steadily afterwards. The [SO 2 ] pw decreased by 80.4% from 74.2 ± 28.4 μg/m 3 in 2007 to 14.6 ± 4.8 μg/m 3 in 2019. The predicted spatial distributions for each year show that the SO 2 pollution was severe (more than 20 μg/m 3 ) in most areas of Northern China until 2017. By using model interpretation methods, we visually reveal the mechanism of estimation bias in the back-extrapolation. Specifically, the training data is severely imbalanced with respect to the satellite-retrieved SO 2 column densities (i.e., it is short on high-value samples), so the benchmark model is unable to extrapolate the effects of this important predictor. This study provides long-term surface SO 2 data for post hoc evaluation and human exposure assessment in Northern China, while demonstrating that the interpretable machine learning approach is critical for model diagnostics and refinement. Leveraging satellite retrievals, the RBE-DA approach can be applied worldwide to back-extrapolate various measures of air quality., Competing Interests: Declaration of competing interest The authors declare no competing interest., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Integral to the urban ecosystem, greening trees provide many ecological benefits, but the active biogenic volatile organic compounds (BVOCs) they release contribute to the production of ozone and secondary organic aerosols, which harm ambient air quality. It is, therefore, necessary to understand the BVOC emission characteristics of dominant greening tree species and their relative contribution to secondary pollutants in various urban contexts. Consequently, this study utilized a dynamic enclosure system to collect BVOC samples of seven dominant greening tree species in urban Chengdu, Southwest China. Gas chromatography/mass spectrometry was used to analyze the BVOC components and standardized BVOC emission rates of each tree species were then calculated to assess their relative potential to form secondary pollutants. We found obvious differences in the composition of BVOCs emitted by each species. Ficus virens displayed a high isoprene emission rate at 31.472 μgC/(gdw (g dry weight)•hr), while Cinnamomum camphora emitted high volumes of D-Limonene at 93.574 μgC/(gdw•hr). In terms of the BVOC emission rates by leaf area, C. camphora had the highest emission rate of total BVOCs at 13,782.59 μgC/(m 2 •hr), followed by Cedrus deodara with 5466.86 μgC/(m 2 •hr). Ginkgo biloba and Osmanthus fragrans mainly emitted oxygenated VOCs with lower overall emission rates. The high BVOC emitters like F. virens, C. camphora, and Magnolia grandiflora have high potential for significantly contributing to environmental secondary pollutants, so should be cautiously considered for future planting. This study provides important implications for improving urban greening efforts for subtropical Chinese urban contexts, like Chengdu., (Copyright © 2021. Published by Elsevier B.V.)

Surface ozone (O 3 ) has become a critical pollutant impeding air quality improvement in many Chinese megacities. Chengdu is a megacity located in Sichuan Basin in southwest China, where O 3 pollution occurs frequently in both spring and summer. In order to understand the elevated O 3 during spring in Chengdu, we conducted sampling campaign at three sites during O 3 pollution episodes in April. Volatile organic compounds (VOCs) compositions at each site were similar, and oxygenated VOCs (OVOCs) concentrations accounted for the highest proportion (35%-45%), followed by alkanes, alkens (including acetylene), halohydrocarbons, and aromatics. The sensitivity of O 3 to its precursors was analyzed using an observation based box model. The relative incremental reactivity of OVOCs was larger than other precursors, suggesting that they also played the dominant role in O 3 formation. Furthermore, the positive matrix factorization model was used to identify the dominant emission sources and to evaluate their contribution to VOCs in the city. The main sources of VOCs in spring were from combustion (27.75%), industrial manufacturing (24.17%), vehicle exhaust (20.35%), and solvent utilization (18.35%). Discussions on VOCs and NO x reduction schemes suggested that Chengdu was typical in the VOC-limited regime, and VOC emission reduction would help to prevent and control O 3 . The analysis of emission reduction scenarios based on VOCs sources showed that the emission reduction ratio of VOCs to NO 2 needs to reach more than 3 in order to achieve O 3 prevention. Emission reduction from vehicular exhaust source and solvent utilization source may be more effective., (Copyright © 2021. Published by Elsevier B.V.)

Particle size distribution of particulate polycyclic aromatic compounds (PACs) is one of the important factors controlling human exposure to PACs in air. In this study, size-segregated airborne particle samples were collected in a megacity in southwest China to analyze PACs concentrations and evaluate related health risks. Annual average concentrations of Σ 19 PAHs (polycyclic aromatic hydrocarbons, 17.4 ng/m 3 ) and Σ 10 OPAHs (oxygenated PAHs, 15.3 ng/m 3 ) were one order of magnitude higher than those of Σ 9 MPAHs (methyl PAHs, 0.97 ng/m 3 ) and Σ 27 NPAHs (nitrated PAHs, 1.54 ng/m 3 ). More than 55% of PACs masses were associated with fine particles (aerodynamic diameter D ae  < 2.1 μm). Inhalation exposure assessment showed that less than 60% of particulate bound PACs could deposit in the respiratory tract, which implies that the traditional model using ambient concentration of PACs would overestimate the inhalation risk. On the other hand, incremental lifetime cancer risks from dermal absorption (ILCR derm ) were comparable to those from inhalation (ILCR inh ) exposure despite the much lower daily dermal absorption dose than the daily inhalation dose, which implies that the health impact might be underestimated if only considering inhalation exposure. Cancer risks from inhalation exposure were mainly attributed to fine particles while those from dermal exposure were mostly associated with coarse particles. Although neither ILCR derm nor ILCR inh exceeded the threshold value of 10 -6 set by USEPA, the total ILCR exceeded this criterion, manifesting potential health risks from exposure to airborne particulate PACs in this region., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Seventy-seven PM2.5 samples were collected at an urban site (Chongqing University Campus A) in October 2015 (autumn), December 2015 (winter), March 2016 (spring), and August 2016 (summer). These samples were analysed for organic carbon (OC), elemental carbon (EC), and their associated char, soot, 16 PAHs, and 28 n-alkanes to trace sources, and atmospheric transport pathways. The annual average of OC, EC, char, soot, ΣPAHs, and Σn-alkanes were 20.75 μg/m 3 , 6.18 μg/m 3 , 5.43 μg/m 3 , 0.75 μg/m 3 , 38.29 ng/m 3 , and 328.69 ng/m 3 , respectively. OC, ΣPAHs, and Σn-alkane concentrations were highest in winter and lowest in summer. EC, char, and soot concentrations were highest in autumn and lowest in winter. Source apportionment via positive matrix factorization (PMF) indicated that coal/biomass combustion-natural gas emissions (23.8%) and motor vehicle exhaust (20.2%) were the two major sources, followed by diesel and petroleum residue (21.1%), natural biogenic sources (17.7%), and evaporative/petrogenic sources (17.2%). The highest source contributor in autumn and winter was evaporative/petrogenic sources (30.6%) and natural biogenic sources (34.5%), respectively, whereas diesel engine emission contributed the most in spring and summer (32.1% and 38.0%, respectively). Potential source contribution function (PSCF) analysis identified southeastern Sichuan and northwestern Chongqing as the major potential sources of these pollutants. These datasets provide critical information for policymakers to establish abatement strategies for the reduction of carbonaceous pollutant emissions and improve air quality in Chongqing and other similar urban centres across China., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Health risks of typical benzene series and halocarbons (BSHs) in a densely populated area near a large-scale chemical industrial park were investigated. Ambient and indoor air and tap water samples were collected in summer and winter; and the concentration characteristics, sources, and exposure risks of typical BSH species, including five benzene series (benzene, toluene, ethylbenzene, o-xylene, m,p-xylene) and five halocarbons (dichloromethane, trichloromethane, trichloroethylene, tetrachloromethane, and tetrachloroethylene), were analysed. The total mean concentrations of BSHs were 53.32 μg m -3 , 36.29 μg m -3 , and 26.88 μg L -1 in indoor air, ambient air, and tap water, respectively. Halocarbons dominated the total BSHs with concentrations relatively higher than those in many other industrial areas. Industrial solvent use, industrial processes, and vehicle exhaust emissions were the principal sources of BSHs in ambient air. The use of household products (e.g., detergents and pesticides) was the principal source of indoor BSHs. Inhalation is the primary human exposure route. Ingestion of drinking water was also an important exposure route but had less impact than inhalation. Lifetime non-cancer risks of individual and cumulative BSHs were below the threshold (HQ = 1), indicating no significant lifetime non-cancer risks in the study area. However, tetrachloromethane, benzene, trichloromethane, ethylbenzene, and trichloroethylene showed potential lifetime cancer risk. The cumulative lifetime cancer risks exceeded the tolerable benchmark (1 × 10 -4 ), indicating a lifetime cancer risk of BSHs to residents near the chemical industry park. This study provides valuable information for the management of public health in chemical industrial parks., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Background: Long-term surface NO 2 data are essential for retrospective policy evaluation and chronic human exposure assessment. In the absence of NO 2 observations for Mainland China before 2013, training a model with 2013-2018 data to make predictions for 2005-2012 (back-extrapolation) could cause substantial estimation bias due to concept drift., Objective: This study aims to correct the estimation bias in order to reconstruct the spatiotemporal distribution of daily surface NO 2 levels across China during 2005-2018., Methods: On the basis of ground- and satellite-based data, we proposed the robust back-extrapolation with a random forest (RBE-RF) to simulate the surface NO 2 through intermediate modeling of the scaling factors. For comparison purposes, we also employed a random forest (Base-RF), as a representative of the commonly used approach, to directly model the surface NO 2 levels., Results: The validation against Taiwan's NO 2 observations during 2005-2012 showed that RBE-RF adequately corrected the substantial underestimation by Base-RF. The RMSE decreased from 10.1 to 8.2 µg/m 3 , 7.1 to 4.3 µg/m 3 , and 6.1 to 2.9 µg/m 3 in predicting daily, monthly, and annual levels, respectively. For North China with the most severe pollution, the population-weighted NO 2 ([NO 2 ] pw ) during 2005-2012 was estimated as 40.2 and 50.9 µg/m 3 by Base-RF and RBE-RF, respectively, i.e., 21.0% difference. While both models predicted that the national annual [NO 2 ] pw increased during 2005-2011 and then decreased, the interannual trends were underestimated by >50.2% by Base-RF relative to RBE-RF. During 2005-2018, the nationwide population that lived in the areas with NO 2  > 40 µg/m 3 were estimated as 259 and 460 million by Base-RF and RBE-RF, respectively., Conclusion: With RBE-RF, we corrected the estimation bias in back-extrapolation and obtained a full-coverage dataset of daily surface NO 2 across China during 2005-2018, which is valuable for environmental management and epidemiological research., (Copyright © 2021 The Author(s). Published by Elsevier Ltd.. All rights reserved.)

Background: The association between maternal exposure to gaseous air pollutants and congenital heart defects (CHD) remains unclear. The concentration-response relationship and the time windows of susceptibility to gaseous pollutants may vary by pollutant species and CHD subtypes., Objective: We aimed to examine the relationship between maternal exposures to four species of gaseous pollutants (NO 2 , O 3 , SO 2 , and CO) and atrial septal defect (ASD), which is a common subtype of CHD, and to determine the critical time windows of susceptibility for each gaseous pollutant., Methods: Among 1,253,633 infants born between October 1, 2013 and December 31, 2016 in China, 1937 newborns were diagnosed with isolated ASD, a prevalence of 1.55‰. Maternal exposures to the gaseous pollutants were estimated by matching the geocoded maternal addresses with the gridded ambient concentrations. The adjusted odds ratios (aOR) between exposures and ASD were quantified by using mixed-effects logistic regression models., Results: We found significantly positive associations between ASD and maternal exposures to NO 2 , O 3 , SO 2 , and CO during entire pregnancy, first-, second-, and third-trimester. However, no statistically significant association was found between maternal exposure to PM 2.5 , PM 2.5-10 and ASD risk (P > 0.05). In the fully adjusted model with respect to average exposure over entire pregnancy, the adjusted odds ratios (aOR) for each 10 μg/m 3 increment of NO 2 , O 3 , SO 2 were 1.33 (95% CI: 1.22-1.45), 1.13 (95% CI: 1.10-1.16), 1.28 (95% CI: 1.20-1.35), respectively; the aOR for each 100 μg/m 3 increment of CO was 1.10 (95% CI: 1.06-1.15). The observed concentration-response relationships varied by exposure periods and pollutants, with the strongest association for NO 2 during the 1st-8th embryology weeks, for O 3 during the third trimester, for SO 2 during the second trimester, and for CO without obvious variation., Conclusions: The findings suggest an increased risk of ASD in association with maternal exposures to four common gaseous pollutants. From the perspective of birth defects prevention and ASD risk mitigation, it is critical to reduce maternal exposure to gaseous pollutants especially during the most susceptible time windows., (Copyright © 2021 Elsevier Inc. All rights reserved.)

Atmospheric fine particulate matter (PM 2.5 ) causes severe haze in China and is regarded as a threat to human health. The health effects of PM 2.5 vary location by location due to the variation in size distribution, chemical composition, and sources. In this study, the cytotoxicity effect, oxidative stress, and gene expression regulation of PM 2.5 in Chengdu and Chongqing, two typical urban areas in southern China, were evaluated. Urban PM 2.5 in summer and winter significantly inhibited cell viability and increased reactive oxygen species (ROS) levels in A549 cells. Notably, PM 2.5 in winter exhibited higher cytotoxicity and ROS level than summer. Moreover, in this study, PM 2.5 commonly induced cancer-related gene expression such as cell adhesion molecule 1 (PECAM1), interleukin 24 (IL24), and cytochrome P450 (CYP1A1); meanwhile, PM 2.5 commonly acted on cancer-related biological functions such as cell-substrate junction, cell-cell junction, and focal adhesion. In particular, PM 2.5 in Chengdu in summer had the highest carcinogenic potential among PM 2.5 at the two sites in summer and winter. Importantly, cancer-related genes were uniquely targeted by PM 2.5 , such as epithelial splicing regulatory protein 1 (ESRP1) and membrane-associated ring-CH-type finger 1 (1-Mar) by Chengdu summer PM 2.5 ; collagen type IX alpha 3 chain (COL9A3) by Chengdu winter PM 2.5 ; SH2 domain-containing 1B (SH2D1B) by Chongqing summer PM 2.5 ; and interleukin 1 receptor-like 1 (IL1RL1) and zinc finger protein 42 (ZNF423) by Chongqing winter PM 2.5 . Meanwhile, important cancer-related biological functions were specially induced by PM 2.5 , such as cell cycle checkpoint by Chengdu summer PM 2.5 ; macromolecule methylation by Chengdu winter PM 2.5 ; endoplasmic reticulum-Golgi intermediate compartment membrane by Chongqing summer PM 2.5 ; and cellular lipid catabolic process by Chongqing winter PM 2.5 . Conclusively, in the typical urban areas of southern China, both summer and winter PM 2.5 illustrated significant gene regulation effects. This study contributes to evaluating the adverse health effects of PM 2.5 in southern China and providing public health suggestions for policymakers., 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 © 2020. Published by Elsevier B.V.)

China has been performing nationwide social lockdown by releasing the Level 1 response to major public health emergencies (RMPHE) to struggle against the COVID-19 (SARS-CoV-2) outbreak since late January 2020. During the Level 1 RMPHE, social production and public transport were maintained at minimal levels, and residents stayed in and worked from home. The universal impact of anthropogenic activities on air pollution can be evaluated by comparing it with air quality under such extreme conditions. We investigated the concentration of both gaseous and particulate pollutants and aerosol light absorption at different levels of (RMPHE) in an urban area of southwestern China. During the lockdown, PM 2.5 , PM 10 , SO 2 , NO x , and BC decreased by 30-50%, compared to the pre-Level 1 RMPHE period. Meanwhile, the decrease of NO x caused the rise of O 3 by up to 2.3 times due to the volatile organic compounds (VOCs) limitation. The aerosol light absorption coefficient at multiple wavelengths decreased by 50%, and AAE decreased by 20% during the Level 1 RMPHE. BrC played essential roles in light absorption after the RMPHE was announced, accounting for 54.0% of the aerosol absorption coefficient at 370 nm. Moreover, the lockdown down-weighted the fraction of fossil fuel in BC concentrations to 0.43 (minima). This study characterizes air pollution at the most basic level and can provide policymakers with references for the "baseline.", 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 © 2020 Elsevier B.V. All rights reserved.)

Post-combustion flue gas desulfurization and denitrification technologies are essential in achieving the full compliance of fine particulate matter (PM 2.5 , aerodynamic diameter less than 2.5 μm) air quality standards by 2030 in China as sulfur dioxide (SO 2 ) and nitrogen oxides (NO X ) are the main precursors of PM 2.5 . Some studies have addressed the performance evaluation of desulfurization technology, but none included the water-soluble ions (sulfate (SO 4 2- ), nitrate (NO 3 - ), etc.) as an indicator nor accounted for uncertainty involved. In this study, we present a multilevel fuzzy method that integrates the analytic hierarchy process with fuzzy theory, defines SO 4 2- concentration as a new environmental indicator, and is supplemented with an uncertainly analysis and apply the method for the techno-economic and environmental evaluation of desulfurization and denitrification technologies in six typical enterprises (including two power plants and three industrial production plants and a waste incineration plant) in Chengdu, China. The evaluation shows that first, the fluctuating desulfurization rate and the dosage leads to changed ranking of the economic and technical secondary evaluation results, with the overall comprehensive evaluation ranks unchanged. Second, from the perspective of environmental protection agency and the public, if the environmental indicators are empowered, the lower the SO 4 2- concentration of an enterprise, the better its evaluation ranking will be and vice versa. Third, if we re-empower from the perspective of the enterprise, under the condition that the technical feasibility is met and the environmental indicators are basically up to standard, the low-cost removing process is more likely to be the tendency of the enterprise. In summary, the findings of the study have led to the conclusions that (1) for the power industry, the integration of desulfurization, denitrification, and dedusting technologies should be promoted rigorously; (2) the non-power industry should continue the end-of-pipe treatment and environmental protection regulatory policies of the power industry; and (3) the energy industry structure should be optimized with enhanced end-of-pipe control technologies to achieve deep reduction of air pollutants.

Measurements of nitrate nitrogen (NO 3 - -N), ammonia nitrogen (NH 4 + -N), and dissolved organic nitrogen (DON) in precipitation were conducted at six different sites in the hinterland of the Three Gorges Reservoir (TGR) area from January 2016 to December 2017. The characteristics and the sources of nitrogen (N) species were identified. N flux of wet deposition in the hinterland of the TGR area were 13.56 ± 2.95 kg N ha -1  yr -1 , of which the proportions of NO 3 - -N, NH 4 + -N and DON were 60.9%, 25.1% and 14.0%, respectively. N flux in urban area was significantly higher than those in suburban, agricultural, and wetland areas. Industrial activities, biomass burning, and secondary transformation were the main contributors of N in urban area. In agricultural area, biomass burning, crustal, and manure were main sources of N. In suburban area, mixed emissions from industry, agriculture, and crustal sources were primary contributors of N. For wetlands, the major contributions were from industrial sector and biomass burning. Additional, analysis of regional distribution of dissolved N deposition in the TGR area was conducted by combining current study data and previously published data between 2000 and 2017. N flux of wet deposition in the entire TGR area ranged from 12.17 to 51.93 kg N ha -1  yr -1 , with an average of 26.81 kg N ha -1  yr -1 . Regional N distribution was greatest in the tail region, followed by the head region, and then the hinterland in the TGR area. The amount of N entering the TGR directly through atmospheric wet deposition was 2906 t yr -1 , accounting for 2.1% of the total N inputs. N load from wet deposition had exceeded the critical loads from that of the water, forest, and even some farmland ecosystems in the TGR area. Decreasing NH 3 emissions from agricultural activities is the key to alleviate the regional N deposition., 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 © 2020 Elsevier B.V. All rights reserved.)

While accumulating evidence shows that air pollution exposure is an important risk factor to influenza prevalence, their association has been inadequately investigated in mountainous regions with dense populations and high humidity. We aim to estimate the association and exposure-outcome effects between exposure to nitrogen dioxide (NO 2 ) and influenza prevalence in a mountainous region with a dense population and high humidity. We investigated 14,993 patients with confirmed influenza cases from January 2013 to December 2017 in Chongqing, a mountainous city in southwest China. We developed distributed lag non-linear models with quasi-Poisson link to take into account the lag and non-linear effects of NO 2 exposure on influenza prevalence. We estimated that the cumulative effect of a 10 μg/m 3 increase in NO 2 with seven-day lag (i.e., summing all the contributions up to seven days) corresponded to relative risk of 1.24 (95% CI: 1.17-1.31) in daily influenza prevalence. Comparing to annual mean of the World Health Organization air quality guidelines of 40 μg/m 3 for NO 2 , we estimated that 14.01% (95% CI: 10.69-17.08%) of the influenza cases were attributable to excessive NO 2 exposure. Our results suggest that NO 2 exposure could worsen the risk of influenza infection in this mountainous city, filling the gap of relevant researches in densely populated and mountainous cities. Our findings provide evidence for developing influenza surveillance and early warning systems., (Copyright © 2020 Elsevier Inc. All rights reserved.)

Environmentally persistent free radicals (EPFRs) are a novel class of hazardous substances that can exist stably in airborne particles for a period ranging from days to weeks and are potentially toxic to human health. Electron paramagnetic resonance spectroscopy (EPR) was used to characterize particulate EPFRs in Wanzhou in the Three Gorges Reservoir area in 2017. During the whole of 2017, the average concentration of particulate EPFRs was 7.0 × 10 13 ± 1.7 × 10 13 spins/m 3 . The seasonal concentration of EPFRs in PM 2.5 showed a trend of autumn > winter > spring > summer. The maxima and minima of EPFRs occurred in spring with concentrations of 2.1 × 10 14 spins/m 3 and 9.4 × 10 12 spins/m 3 respectively. The EPFRs in PM 2.5 were mainly carbon-centered radicals with adjacent oxygen atoms. Significant positive correlations were found between EPFRs and SO 4 2- , NO 3 - and NH 4 + (r > 0.55, n = 111), indicating that EPFRs are associated with secondary sources. The atmospheric processing of particles from coal combustion, traffic, and agriculture were important sources of EPFRs. They were also particularly well correlated with K + and Cl - in winter, suggesting that EPFRs may also be derived from wintertime biomass burning emissions. The amount of inhalable EPFRs in Wanzhou was equivalent to the range of 2.3-6.8 cigarettes per capita per day. This study provides evidence of the potential health risks of EPFRs in PM 2.5 , and references for air pollution control in the Three Gorges Reservoir area., 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 © 2020 Elsevier Ltd. All rights reserved.)

As important pollution gases and represented precursors of both ozone and second organic aerosol (SOA), the component characteristics, source origins, environmental health and emission control of volatile organic compounds (VOCs), are gaining more and more attention in Chinese megacities. In order to understand the concentration, composition and temporal and spatial distribution characteristics of VOCs in the atmosphere of Chengdu, a megacity located in Sichuan basin in southwest China, the offline sampling measurements of VOCs were carried out at 28 different field sites covering all the districts and counties of Chengdu during special periods from May 2016 to January 2017. Speciated VOCs measurement was performed by the GC-FID/MS, and 99 species were identified. The averaged total VOC mixing ratios of each sampling site were in the range from 35.03 to 180.57 ppbv. Based on these observational data, the distribution characteristics of VOCs in different months and different regions of Chengdu were clarified. The VOCs data were used to estimate the potential amount of ozone, secondary aerosol formation and health risk assessment in Chengdu. Furthermore, the positive matrix factorization (PMF) model was used to identify the dominant emission sources and evaluate their contribution to VOCs in the city. The two main sources of VOCs in Chengdu were motor vehicle exhaust and solvent utilization. These accounted for 43% of all emission sources. In the summertime, due to higher temperatures and stronger sunlight, the contribution of natural sources and secondary emissions were also relatively high, which were supported by the regional emission inventories. Finally, the controlling direction of VOCs and O 3 pollution in Chengdu was discussed, and the VOCs pollution control strategy was proposed for the near future., 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 © 2020 Elsevier Inc. All rights reserved.)

The light absorption of brown carbon (BrC) makes a significant contribution to aerosol light absorption (Abs) and affects the radiative forcing. In this study, we analyzed and evaluated the light absorption and radiative forcing of BrC samples collected from December 2016 to January 2017 in Chongqing and Chengdu in the Sichuan Basin of Southwest China. Based on a two-component model, we estimated that BrC light absorption at 405 nm was 19.9 ± 17.1 Mm -1 and 19.2 ± 12.3 Mm -1 in Chongqing and Chengdu, contributing 19.0 ± 5.0% and 17.8 ± 3.7% to Abs respectively. Higher Abs 405,BrC , MAE 405,BrC , and AAE 405 - 980 values were observed during the pollution period over the clean period in both cities. The major sources of BrC were biomass burning (BB) and secondary organic aerosol in Chongqing, and coal combustion (CC) and secondary organic aerosol in Chengdu. During the pollution period, aged BrC formed from anthropogenic precursors via its aqueous reactions with NH 4 + and NOx had impacts on BrC absorption in both cities. BB led to higher Abs 405,BrC , MAE 405,BrC , and AAE 405 - 980 values in Chongqing than Chengdu during the pollution period. The fractional contribution of radiation absorbed by BrC relative to BC in the wavelengths of 405-445 nm was 60.2 ± 17.0% and 64.2 ± 11.6% in Chongqing and Chengdu, significantly higher than that in the range of 405-980 nm (26.2 ± 6.7% and 27.7 ± 4.6% respectively) (p < 0.001). This study is useful for understanding the characterization, sources, and impacts of BrC in the Sichuan Basin., 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 © 2020 Elsevier B.V. All rights reserved.)

To identify seasonal fluxes and sources of dissolved inorganic nitrogen (DIN) wet deposition, concentrations and δ 15 N signatures of nitrate (NO 3 - ) and ammonium (NH 4 + ) in wet precipitation were measured at four typical land-use types in the Three Gorges reservoir (TGR) area of southwest China for a one-year period. Higher DIN fluxes were recorded in spring and summer and their total fluxes (averaged 7.58 kg N ha -1 ) were similar to the critical loads in aquatic ecosystems. Significant differences of precipitation δ 15 N were observed for NH 4 + -N between town and wetland sites in spring and between urban and rural sites in summer. For NO 3 - -N, significant differences of precipitation δ 15 N were observed between town and rural sites in spring and between urban and town sites in autumn, respectively. Quantitative results of NO 3 - -N sources showed that both biomass burning and coal combustion had higher fluxes at the urban site especially in winter (0.18 ± 0.09 and 0.19 ± 0.08 kg N ha -1 ), which were about three times higher than those at the town site. A similar finding was observed for soil emission and vehicle exhausts in winter. On the whole, DIN wet deposition averaged at 12.13 kg N ha -1 yr -1 with the urban site as the hotspot (17.50 kg N ha -1 yr -1 ) and regional NO 3 - -N fluxes had a seasonal pattern with minimum values in winter. The contribution to NO 3 - -N wet deposition from biomass burning was 26.1 ± 14.1%, which is the second dominant factor lower than coal combustion (26.5 ± 12.6%) in the TGR area during spring and summer. Hence N emission reduction from biomass burning, coal combustion and vehicle exhausts should be strengthened especially in spring and summer to effectively manage DIN pollution for the sustainable development in TGR area., (Copyright © 2020 Elsevier Inc. All rights reserved.)

From 2013 to 2017, with the implementation of the toughest-ever clean air policy in China, significant declines in fine particle (PM 2.5 ) concentrations occurred nationwide. Here we estimate the drivers of the improved PM 2.5 air quality and the associated health benefits in China from 2013 to 2017 based on a measure-specific integrated evaluation approach, which combines a bottom-up emission inventory, a chemical transport model, and epidemiological exposure-response functions. The estimated national population-weighted annual mean PM 2.5 concentrations decreased from 61.8 (95%CI: 53.3-70.0) to 42.0 µg/m 3 (95% CI: 35.7-48.6) in 5 y, with dominant contributions from anthropogenic emission abatements. Although interannual meteorological variations could significantly alter PM 2.5 concentrations, the corresponding effects on the 5-y trends were relatively small. The measure-by-measure evaluation indicated that strengthening industrial emission standards (power plants and emission-intensive industrial sectors), upgrades on industrial boilers, phasing out outdated industrial capacities, and promoting clean fuels in the residential sector were major effective measures in reducing PM 2.5 pollution and health burdens. These measures were estimated to contribute to 6.6- (95% CI: 5.9-7.1), 4.4- (95% CI: 3.8-4.9), 2.8- (95% CI: 2.5-3.0), and 2.2- (95% CI: 2.0-2.5) µg/m 3 declines in the national PM 2.5 concentration in 2017, respectively, and further reduced PM 2.5 -attributable excess deaths by 0.37 million (95% CI: 0.35-0.39), or 92% of the total avoided deaths. Our study confirms the effectiveness of China's recent clean air actions, and the measure-by-measure evaluation provides insights into future clean air policy making in China and in other developing and polluting countries., Competing Interests: The authors declare no competing interest., (Copyright © 2019 the Author(s). Published by PNAS.)

To better understand the potential causes of visibility impairment in autumn and winter in Chengdu, relative humidity (RH), visibility, the concentrations of PM 2.5 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 NO 2 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 PM 2.5 concentrations, which was more sensitive to RH under lower PM 2.5 concentrations. The threshold concentration of PM 2.5 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 (b ext )), followed by NH 4 NO 3 and (NH 4 ) 2 SO 4 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 b ext decreased from 38.12% to 26.77%, while the contribution of NH 4 NO 3 and (NH 4 ) 2 SO 4 to b ext increased from 19.09% and 20.20% to 34.29% and 24.35%, respectively, and NH 4 NO 3 became the largest contributor to b ext at Type IV. The results showed that OM and NH 4 NO 3 were the key components of PM 2.5 for visibility impairment in Chengdu, indicating that the control of precursors emissions of carbonaceous species and NH 4 NO 3 could effectively improve the visibility in Chengdu., (Copyright © 2019. Published by Elsevier B.V.)

Secondary inorganic aerosols, including sulfate, nitrate, and ammonium contribute to a large extent to the severe haze pollution events in China. Understanding their formation mechanisms is critical for designing effective mitigation strategies to control haze pollution, especially as the role of nitrate seemed to become more important recently, especially in some megacities. In the present study, simultaneous observations were conducted in two megacities (Chengdu and Chongqing) in Sichuan Basin of southwest China, one of the regions suffering from severe aerosol pollution. One typical long-lasting pollution event in Chengdu and Chongqing was captured during wintertime from December 25, 2016 to January 5, 2017. The campaign-average of hourly concentrations of PM 2.5 , sulfate, and nitrate, measured by an Aerosol Analyzer (ZSF) were 101 ± 73.8 μg/m 3 , 15.9 ± 11.8 μg/m 3 , and 24.9 ± 20.6 μg/m 3 , respectively, in Chengdu, and were 87.7 ± 53.8 μg/m 3 , 19.7 ± 13.5 μg/m 3 , and 15.1 ± 10.1 μg/m 3 , respectively, in Chongqing. Nitrate contributed substantially to PM 2.5 pollution when PM 2.5 was lower than 150 μg/m 3 , largely due to the strong secondary transformation of NO X to nitrate during the occurrence of the pollution episode. Heterogeneous hydrolysis of N 2 O 5 dominated nitrate formation during nighttime, while photochemical reactions and high-RH enhanced gas- to aqueous-phase dissolution of NH 3 and HNO 3 or cloud processes likely played important roles for nitrate formation during daytime. RH-dependent heterogeneous reactions contributed greatly to the formation of sulfate. NO X is confirmed to play an important role as an oxidant in accelerating the secondary transformation of SO 2 to sulfate at high RH and low O 3 levels under neutralization condition during heavy PM 2.5 pollution episode. Results from this study identified the formation mechanism of nitrate, especially during the daytime, and addressed the importance of heterogeneous inorganic reactions in the formation of heavy aerosol pollution events., (Crown Copyright © 2019. Published by Elsevier Ltd. All rights reserved.)

China has been experiencing fine particle (i.e., aerodynamic diameters ≤ 2.5 µm; PM 2.5 ) pollution and acid rain in recent decades, which exert adverse impacts on human health and the ecosystem. Recently, ammonia (i.e., NH 3 ) emission reduction has been proposed as a strategic option to mitigate haze pollution. However, atmospheric NH 3 is also closely bound to nitrogen deposition and acid rain, and comprehensive impacts of NH 3 emission control are still poorly understood in China. In this study, by integrating a chemical transport model with a high-resolution NH 3 emission inventory, we find that NH 3 emission abatement can mitigate PM 2.5 pollution and nitrogen deposition but would worsen acid rain in China. Quantitatively, a 50% reduction in NH 3 emissions achievable by improving agricultural management, along with a targeted emission reduction (15%) for sulfur dioxide and nitrogen oxides, can alleviate PM 2.5 pollution by 11-17% primarily by suppressing ammonium nitrate formation. Meanwhile, nitrogen deposition is estimated to decrease by 34%, with the area exceeding the critical load shrinking from 17% to 9% of China's terrestrial land. Nevertheless, this NH 3 reduction would significantly aggravate precipitation acidification, with a decrease of as much as 1.0 unit in rainfall pH and a corresponding substantial increase in areas with heavy acid rain. An economic evaluation demonstrates that the worsened acid rain would partly offset the total economic benefit from improved air quality and less nitrogen deposition. After considering the costs of abatement options, we propose a region-specific strategy for multipollutant controls that will benefit human and ecosystem health., Competing Interests: The authors declare no conflict of interest.

Lead (Pb) in individual aerosol particles was measured using a single particle aerosol mass spectrometer at an urban site in Chengdu, a typical basin city of China, for four one-month periods in 2016-2017 - one period for each season. The highest mass concentrations of particulate matter (PM) and gaseous species (CO, NO, NO 2 , and SO 2 ) were observed in winter. Cluster analysis was applied to Pb-containing particles, and eight major classes were identified based on mass spectral features. The contribution of these classes to the total Pb-containing particles varied seasonally - for example, Pb-nitrate (PbNO 3 ) particles showed a higher contribution in spring and winter (47%), while Pb-sulfate (PbSO 4 ) particles exhibited a higher contribution in summer and autumn (14%-19%). The size range of particles also changed with seasons as a result of different sources and formation mechanisms under different climatic conditions. A weighted potential source contribution function (WPSCF) analysis suggested that the potential source areas of Pb-containing particles were mainly located to the northeast, east, southeast, and south of Chengdu, and their contribution intensity and coverage area significantly varied in the four seasons. Although almost all pollutants decreased during the Spring Festival holiday (SF) period, fireworks caused the most serious PM and SO 2 pollution episodes during the whole study period. During the SF period, the contributions of industrial and traffic-related particles (Pb-organic + elemental carbon (PbOE) and PbNO 3 particles) decreased, whereas those of Pb-chloride (PbCl), Pb-metal (PbM), and Pb-sulfate + nitrate (PbSN) particles increased due to fireworks. Results from this study may provide valuable information for a deeper understanding of Pb in particles and evaluation its impacts on atmospheric environment and human health., (Copyright © 2019 Elsevier B.V. All rights reserved.)

PM 2.5 samples were collected in four segregate one-month periods, each representing one season, for analyzing their contents of water soluble inorganic ions (WSIIs) in a small city inside Sichuan Basin. Daily PM 2.5 concentrations ranged from 23.2 to 203.1 μg m -3 with an annual mean of 66.9 ± 33.6 μg m -3 . Annual mean concentrations of WSIIs was 28.8 ± 20.3 μg m -3 , accounting for 43.1% of PM 2.5 . Seasonal mean concentrations of WSIIs ranged from 17.5 ± 9.3 μg m -3 in summer to 46.5 ± 27.6 μg m -3 in winter. Annual mean mass ratio of NO 3 - /SO 4 2- was 0.49, demonstrating predominant stationary sources for secondary inorganic aerosols (SNA, including SO 4 2- , NH 4 + and NO 3 - ); whereas annual mean molar ratio of [NH 4 + ]/[NO 3 - ] was 3.5, suggesting dominant agriculture emissions contributing to the total nitrogen. During a severe and long-lasting (13 days) winter pollution period when mean PM 2.5 concentration reached to 132.5 μg m -3 , PM 2.5 concentration was enhanced by a factor of 2.6 while that of SNA by a factor of 2.9 compared to those before the pollution event, and the fraction of SNA in PM 2.5 only increased slightly (from 46.7% to 50.6%). Thus, local accumulation of pollutants under poor diffusion conditions played a major role causing the extremely high PM 2.5 concentration, besides the contributions from the enhanced SNA formation under specific weather conditions., (Crown Copyright © 2018. Published by Elsevier B.V. All rights reserved.)