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On-line chemical characterization of atmospheric particulate matter (PM) with soft ionization technique and ultrahigh-resolution Mass Spectrometry (UHRMS) provides molecular information of organic constituents in real time. Here we describe the development and application of an automatic measurement system that incorporates PM 2.5 sampling, thermal desorption, atmospheric pressure photoionization, and UHRMS analysis. Molecular formulas of detected organic compounds were deducted from the accurate (±10 ppm) molecular weights obtained at a mass resolution of 100,000, allowing the identification of small organic compounds in PM 2.5 . Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 pg. As a proof of principle, PM 2.5 samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the system. The automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 hr. The detected organic compounds comprised mainly CHON and CHN compounds below 350 m/z. Pronounced seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in winter. This result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in summer. Diurnal variation in signal intensity of each formula provides crucial information to reveal its source and formation pathway. In summary, the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM 2.5 ., 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.)

In recent years, many cities have taken measures to reduce volatile organic compounds (VOCs), an important precursor of ozone (O 3 ), to alleviate O 3 pollution in China. 116 VOC species were measured by online and offline methods in the urban area of Jiaozuo from May to October in 2021 to analyze the compositional characteristics. VOC sources were analyzed by a positive matrix factorization (PMF) model, and the sensitivity of ozone generation was determined by ozone isopleth plotting research (OZIPR) simulation. The results showed that the average volume concentration of total VOCs was 30.54 ppbv and showed a bimodal feature due to the rush-hour traffic in the morning and at nightfall. The most dominant VOC groups were oxygenated VOCs (OVOCs, 29.3%) and alkanes (26.7%), and the most abundant VOC species were acetone and acetylene. However, based on the maximum incremental reactivity (MIR) method, the major VOC groups in terms of ozone formation potential (OFP) contribution were OVOCs (68.09 µg/m 3 , 31.5%), aromatics (62.90 µg/m 3 , 29.1%) and alkene/alkynes (54.90 µg/m 3 , 25.4%). This indicates that the control of OVOCs, aromatics and alkene/alkynes should take priority. Five sources of VOCs were quantified by PMF, including fixed sources of fossil fuel combustion (27.8%), industrial processes (25.9%), vehicle exhaust (19.7%), natural and secondary formation (13.9%) and solvent usage (12.7%). The empirical kinetic modeling approach (EKMA) curve obtained by OZIPR on O 3 exceedance days indicated that the O 3 sensitivity varied in different months. The results provide theoretical support for O 3 pollution prevention and control in Jiaozuo., 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.)

Black carbon (BC) aerosols in the atmosphere play a significant role in climate systems due to their strong ability to absorb solar radiation. The lifetime of BC depends on atmospheric transport, aging and consequently on wet scavenging processes (in-cloud and below-cloud scavenging). In this study, sequential rainwater samples in eight rainfall events collected in 2 mm interval were measured by a tandem system including a single particle soot photometer (SP2) and a nebulizer. The results showed that the volume-weighted average (VWA) mass concentrations of refractory black carbon (rBC) in each rainfall event varied, ranging from 10.8 to 78.9 µg/L. The highest rBC concentrations in the rainwater samples typically occurred in the first fraction from individual rainfall events. The geometric mean median mass-equivalent diameter (MMD) decreased under precipitation, indicating that rBC with larger sizes was relatively aged and preferentially removed by wet scavenging. A positive correlation (R 2  = 0.73) between the VWA mass concentrations of rBC in rainwater and that in ambient air suggested the important contribution of scavenging process. Additionally, the contributions of in-cloud and below-cloud scavenging were distinguished and accounted for 74% and 26% to wet scavenging, respectively. The scavenging ratio of rBC particles was estimated to be 0.06 on average. This study provides helpful information for better understanding the mechanism of rBC wet scavenging and reducing the uncertainty of numerical simulations of the climate effects of rBC., (Copyright © 2022. Published by Elsevier B.V.)

To understand the source, formation, and seasonality of biogenic secondary organic aerosol (BSOA), a nine-stage cascade impactor was utilized to collect size-segregated particulate samples from April 2017 to January 2018 in Beijing, China. BSOA tracers derived from isoprene, monoterpene, and sesquiterpene were measured with gas chromatography-mass spectrometry. Isoprene and monoterpene SOA tracers exhibited significant seasonal variations, with a summer maximum and a winter minimum. Dominance of 2-methyltetrols (isoprene SOA tracers) with a good correlation with levoglucosan (a biomass burning tracer), which was combined with the detection of methyltartaric acids (possible indicators for aged isoprene) in summer, implies possible biomass burning and long-range transport. In contrast, sesquiterpene SOA tracer (β-caryophyllinic acid) was dominant in winter and was probably associated with the local burning of biomass. Bimodal size distributions were observed for most isoprene SOA tracers, consistent with previous laboratory experiments and field studies showing that they can be formed not only in the aerosol phase but also in the gas phase. Monoterpene SOA tracers cis-pinonic acid and pinic acid showed a coarse-mode peak (5.8-9.0 μm) in four seasons due to their volatile nature. Sesquiterpene SOA tracer β-caryophyllinic acid showed a unimodal pattern with a major fine-mode peak (1.1-2.1 μm), which is linked to local biomass burning. The tracer-yield method was used to quantify the contributions of isoprene, monoterpene, and sesquiterpene to secondary organic carbon (SOC) and SOA. The highest isoprene SOC and SOA concentrations occurred in summer (2.00 μgC m -3 and 4.93 μg m -3 , respectively), contributing to 1.61% of OC and 5.22% of PM 2.5 , respectively. These results suggest that BSOA tracers are promising tracers for understanding the source, formation, and seasonality of BSOA., 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.)

Strict emission controls were implemented in Beijing and the surrounding regions in the North China Plain to guarantee good air quality during the 2014 Asia-Pacific Economic Cooperation (APEC) summit. Thus, the APEC period provides a good opportunity to study the sources and formation processes of atmospheric organic aerosol. Here, fine particles (PM 2.5 , particulate matter with a diameter of 2.5 μm or less) collected in urban Beijing before and during the APEC period were analyzed for molecular tracers of primary and secondary organic aerosol (SOA). The primary organic carbon (POC) and secondary organic carbon (SOC) were also reconstructed using a tracer-based method. The concentrations of biogenic SOA tracers ranged from 1.09 to 34.5 ng m -3 (mean 10.3 ± 8.51 ng m -3 ). Monoterpene oxidation products were the largest contributor to biogenic SOA, followed by isoprene- and sesquiterpene-derived SOA. The concentrations of biogenic SOA tracers decreased by 50 % during the APEC, which was largely attributed to the implementation of emission controls by the Chinese government. The increasing mass fractions of biogenic SOA tracers from isoprene and sesquiterpene during the pollution episodes implied that their photooxidation processes contributed to the poor air quality in urban Beijing. The reconstructed biogenic and anthropogenic SOC and POC concentrations were 89.6 ± 96.8 ng m -3 , 570 ± 611 ng m -3 , and 2.49 ± 2.08 μg m -3 , respectively, accounting for 21.9 ± 11.4 % of OC in total. Biomass-burning derived OC was the largest contributor to carbonaceous aerosol over the North China Plain. By comparing the results before and during the APEC, the emission controls effectively mitigated about 34 % of the estimated OC and were more effective at reducing SOC than POC. This suggests that the reduction of the primary organic aerosol loading is harder than SOA over the North China Plain., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

With the implementation of clean coal policy in China, the chunk coal has been gradually replaced by honeycomb briquette in domestic energies. In this study, the molecular composition of fine particles (PM 2.5 ) from chunk coal and honeycomb briquette combustion is characterized using the Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS). More than 6000 molecular formulae were detected in each PM 2.5 sample. A remarkable decrease in unsaturation and aromatic compounds was found from chunk coal to honeycomb briquette derived aerosols. Around 73.6% of the unique CHON compounds in chunk coal are considered to have aromatic structures, while it decreased to 7.3% in honeycomb briquette. Most of these nitroaromatics detected only in chunk coal are highly carcinogenic and mutagenic with 4-6 rings. Moreover, the aromatic compounds in sulfur-containing compounds also showed a significant decrease. Meanwhile, because of the perforated shape and the additives added during the production of honeycomb briquettes, there are more heteroatoms-containing molecules released from honeycomb briquette combustion, which are highly functional compounds with high molecular weight, high degree of oxidation, and low volatility. Our results provide molecular level evidence that the transformation from chunk coal to honeycomb briquette can effectively reduce the emission of aromatic compounds, which is beneficial to assessing and reducing the impacts to climate change as well as human 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 © 2022. Published by Elsevier B.V.)

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

Online detection of bioaerosols based on the light-induced fluorescence (LIF) technique is still challenging due to the complexity of bioaerosols and the external/internal mixing with nonbiological fluorescent compositions. Although many lab studies have measured the fluorescence properties of the biological and nonbiological materials, there is still a scarcity of knowledge of the sources of fluorescent aerosol particles (FAP) in the ambient atmosphere. Here, we fill this gap by combining the online measurement of an LIF-based instrument (wideband integrated bioaerosol sensor, WIBS, 0.8-20 μm) with the measurements of typical biological matter and the compositions related to major nonbiological FAP from May to July in the megacity Beijing. We find that fungal spores and pollen are widely observed in all types of FAP using a WIBS. Bacteria are suggested to be associated with the fine mode FAP (excitation/emission: 280 nm/310-400 nm; 0.8-3 μm). The FL-B and -BC particles (emission in 420-650 nm) contributing the most to FAP are strongly associated with humic-like substances, dust, burning and combustion emissions, and secondary organic aerosols (SOA). This study provides a guide for interpreting individual FAP measured by LIF instruments and points to the applicability of online LIF instruments to characterize nonbiological compositions including SOA.

Secondary inorganic aerosols (SIA) account for 20-60% of the total fine particulates in the Beijing-Tianjin-Hebei (BTH) region of China, indicating an urgent need to clarify the relationship among such compounds. The purpose of this study was to quantify the relationship between emissions of NH 3 , NOx, SO 2 , VOCs and SIA concentrations during a severe winter haze episode using an air quality model and a meteorology-based redistributed NH 3 emission inventory within the BTH region. The results showed that the model performance regarding the NH 3 simulations in January by the four emission inventories improved after the redistribution of daily NH 3 emissions, with an increase of 0.02-0.13 in R, a 9-56% decrease in NMB, and a 7-51% decrease in NME. The updated simulations reproduced the daily observations of SIA, SO 2 , and NO 2 well. A total of 125 sets of sensitivity simulations showed that a synergistic reduction in NH 3 and VOCs was more efficient in terms of SIA control than simply reducing SO 2 or NOx in the BTH region. If only NOx emissions were reduced, the SIA concentration would first increase and then decrease, and it could decline by another 0.86-8.03% in parallel with an equal NH 3 emission cut. SIA could be reduced by approximately 22.68% with the most stringent inorganic precursors' control. Moreover, VOCs emission reductions could lead to a decrease in SIA, and the impact of VOCs on SIA was similar to that of NH 3 . The collaborative control of both inorganic precursors and VOCs was more effective than single-factor control measures for decreasing SIA, and the decline rate was approximately 29.26% under minimum emission conditions. This improved effectiveness was obtained because VOCs mitigation effectively decreases the ozone concentration, which in turn influences SIA formation. Finally, on the premise of a 60% SO 2 cut, the reduction scheme NH 3 :VOCs:NOx = 4:4:1 was suggested for SIA control., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Cross-boundary transport of air pollution is a difficult issue in pollution control for the North China Plain. In this study, an industrial district (Shahe City) with a large glass manufacturing sector was investigated to clarify the relative contribution of fine particulate matter (PM 2.5 ) to the city's high levels of pollution. The Nest Air Quality Prediction Model System (NAQPMS), paired with Weather Research and Forecasting (WRF), was adopted and applied with a spatial resolution of 5 km. During the study period, the mean mass concentrations of PM 2.5 , SO 2 , and NO 2 were observed to be 132.0, 76.1, and 55.5 μg/m 3 , respectively. The model reproduced the variations in pollutant concentrations in Shahe at an acceptable level. The simulation of online source-tagging revealed that pollutants emitted within a 50-km radius of downtown Shahe contributed 63.4% of the city's total PM 2.5 concentration. This contribution increased to 73.9±21.2% when unfavorable meteorological conditions (high relative humidity, weak wind, and low planetary boundary layer height) were present; such conditions are more frequently associated with severe pollution (PM 2.5 ≥ 250 μg/m 3 ). The contribution from Shahe was 52.3±21.6%. The source apportionment results showed that industry (47%), transportation (10%), power (17%), and residential (26%) sectors were the most important sources of PM 2.5 in Shahe. The glass factories (where chimney stack heights were normally < 70 m) in Shahe contributed 32.1% of the total PM 2.5 concentration in Shahe. With an increase in PM 2.5 concentration, the emissions from glass factories accumulated vertically and narrowed horizontally. At times when pollution levels were severe, the horizontally influenced area mainly covered Shahe. Furthermore, sensitivity tests indicated that reducing emissions by 20%, 40%, and 60% could lead to a decrease in the mass concentration of PM 2.5 of of 12.0%, 23.8%, and 35.5%, respectively., (Copyright © 2021. Published by Elsevier B.V.)

Spatiotemporal variations of ozone (O 3 ) taken from the Copernicus Atmosphere Monitoring Service (CAMS) and the second Modern-Era Retrospective Analysis for Research and Applications (MERRA-2) were intercompared and evaluated with ground and ozone-sonde observations over China in 2018 and 2019. Intercomparison of the surface ozone from CAMS and MERRA-2 reanalysis showed significant negative bias (CAMS minus MERRA-2, same below) at Tibetan Plateau of up to 80 µg/m 3 , and the average R 2 was about 0.6 across China. Evaluated with the ground observations from China National Environmental Monitoring Center (CNEMC), we found that CAMS and MERRA-2 reanalysis were capable of capturing the key patterns of monthly and diurnal variations of surface ozone over China except for the western region, and MERRA-2 overestimated the observations compared to CAMS. Vertically, the CAMS profiles overestimated the ozone-sonde from the World Ozone and Ultraviolet Radiation Data Center (WOUDC) above 200 hPa with the magnitude reaching up to 150 µg/m 3 , while little bias was found between the reanalysis and observations below 200 hPa. Intercomparison drawn from the vertical distribution between CAMS and MERRA-2 reanalysis showed that the negative bias appeared throughout the troposphere over China, while the positive bias emerged in the upper troposphere and lower stratosphere (UTLS) with high order of magnitude exceeding 100 µg/m 3 , indicating large uncertainties at higher altitudes. In summary, we concluded that CAMS reanalysis showed better agreement with the observations in contrast to MERRA-2, and the large discrepancy especially at higher altitudes between these two reanalysis datasets could not be ignored., (Copyright © 2022. Published by Elsevier B.V.)

It is very important for air pollution prevention and control to accurately quantify atmospheric environment capacity (AEC) in the planetary boundary layer (PBL). This study developed a high temporal-resolution dynamic multi-box algorithm to estimate PM 2.5 AEC with a PBL ceilometer and Doppler wind profile lidar in Beijing City. Compared with the traditional A-value method, two primary improvements are introducing the time coefficient and vertical multi-box assumption into the original box model. The algorithm can accurately calculate the PM 2.5 AEC under different circulation patterns and predict the short-time dynamic change of AEC. The results show that the time coefficient effectively reduced the estimation errors when the initial PM 2.5 concentration, horizontal wind speed and PBL heights change greatly with time, such situation is consistent with most circulation patterns. And the improvement of multi-box model is much more remarkable when the PM 2.5 concentration and horizontal wind change greatly in the vertical direction, such as A, NE and W type circulations. The ideal AEC under polluted circulation patterns won't increase infinitely with wind speed and PBL height, generally less than 30 t/h. The horizontal advection has a much greater effect on expanding the capacity of PM 2.5 than the vertical diffusion under clean circulation patterns, and the maximum value of ideal AEC can reach 50 t/h. The positive residual AEC under clean circulations indicates surplus capacity for PM 2.5 because of vigorous turbulences, while weak diffusion and ventilation conditions under polluted circulations lead to negative residual AEC and insufficient capacity of atmosphere., 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 © 2021 Elsevier B.V. All rights reserved.)

Benefiting from the pollution controls implemented by the Chinese government, the concentrations of PM 2.5 , SO 2 , NO 2 and CO showed a significant decrease in Beijing during 2013-2017. In this study, an observation-based method was employed to estimate the relative contributions of regional transport (MaxRTC) and local emissions (MinLEC) to air pollutant levels during 2013-2017 in Beijing. The results showed that the MaxRTC to SO 2 and PM 2.5 increased significantly over the five years, while those to CO and NO 2 changed little. Furthermore, the difference in the emissions control efficiency (ΔECE) between Beijing (receptor region) and Shijiazhuang (source region), which refers to the concentration changes corresponding to unit emission changes of a certain air pollutant between the two regions, was introduced to verify the estimated variation in MaxRTC and MinLEC over 2013-2017. The negative value of ΔECE found for PM 2.5 and SO 2 supports the conclusion of an increasing effect of regional transport. This implies that local emissions control alone is not adequate for mitigating Beijing's air pollution, especially with the demand for continuously improving air quality. Joint prevention and control with regard to air quality on a regional scale is more important and urgent in the next Five-Year Plan., (Copyright © 2021 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Dust heterogeneous chemistry plays an important role in tropospheric chemistry, but its parameterization in numerical models is often quite simplified, which hampers accurate prediction of particulate matter and its chemical component. In this study, we investigate the evolution of dust heterogeneous chemical process and its potential impacts on gaseous and aerosol components during a dust pollution episode from March 27 to April 2, 2015 over North China. Based on field measurements, the significant role of relative humidity (RH) in dust heterogeneous chemistry is found and a RH-dependent parameterization for uptake coefficients of HNO 3 and SO 2 is incorporated in GEOS-Chem to reproduce the dust heterogeneous chemical process. During the study period, observed dust sulfate (DSO4) and dust nitrate (DNIT) exhibit maximum concentrations of 9.1 and 22.8 μg m -3 respectively, accompanied by high RH and gaseous precursor concentrations. DSO4 concentrations are positively related to RH. The observed dust sulfate oxidation ratio (DSOR) is elevated evidently with increased RH, especially when RH is higher than ~40%, implying that enhanced RH could promote heterogeneous oxidation of SO 2 to DSO4. Model simulation shows that when incorporating the RH-dependent parameterization, DNIT and DSO4 are generally well captured and the model performance of total sulfate oxidation ratio (TSOR) and total nitrate oxidation ratio (TNOR) are improved. High contribution of DNIT and DSO4 are found to be located over the regions close to source areas (>60%) and downwind regions (>40%), respectively. Sensitivity results show that SO 2 and HNO 3 reduce by 2-24 μg m -3 and 1-18 μg m -3 when considering dust heterogeneous impacts, thus leading to reduction in non-dust sulfate and non-dust nitrate concentrations. As a result, simulated NH 3 increases and ammonium reduces by more than 20%. Our study indicates that the contribution of heterogeneous reactions to sulfate formation is 20-30% over North 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 © 2021 Elsevier B.V. All rights reserved.)

The region along the Taihang Mountains in the North China Plain (NCP) is characterized by serious fine particle pollution. To clarify the formation mechanism and controlling factors, an observational study was conducted to investigate the physical and chemical properties of the fine particulate matter in Jiaozuo city, China. Mass concentrations of the water-soluble ions (WSIs) in PM 2.5 and gaseous pollutant precursors were measured on an hourly basis from December 1, 2017, to February 27, 2018. The positive matrix factorization (PMF) method and the FLEXible PARTicle (FLEXPART) model were employed to identify the sources of PM 2.5 . The results showed that the average mass concentration of PM 2.5 was 111 μg/m 3 during the observation period. Among the major WSIs, sulfate, nitrate, and ammonium (SNA) constituted 62% of the total PM 2.5 mass, and NO 3 - ranked the highest with an average contribution of 24.6%. NH 4 + was abundant in most cases in Jiaozuo. According to chemical balance analysis, SO 4 2- , NO 3 - , and Cl - might be present in the form of (NH 4 ) 2 SO 4 , NH 4 NO 3 , NH 4 Cl, and KCl. The liquid-phase oxidation of SO 2 and NO 2 was severe during the haze period. The relative humidity and pH were the key factors influencing SO 4 2- formation. We found that NO 3 - mainly stemmed from homogeneous gas-phase reactions in the daytime and originated from the hydrolysis of N 2 O 5 in the nighttime, which was inconsistent with previous studies. The PMF model identified five sources of PM 2.5 : secondary origin (37.8%), vehicular emissions (34.7%), biomass burning (11.5%), coal combustion (9.4%), and crustal dust (6.6%)., (Copyright © 2020. Published by Elsevier B.V.)

Atmospheric aerosols over polar regions have attracted considerable attention for their pivotal effects on climate change. In this study, temporospatial variations in single-particle-based depolarization ratios (δ: s -polarized component divided by the total backward scattering intensity) were studied over the Northwest Pacific and the Arctic Ocean using an optical particle counter with a depolarization module. The δ value of aerosols was 0.06 ± 0.01 for the entire observation period, 61 ± 10% lower than the observations for coastal Japan (0.12 ± 0.02) ( Pan et al. Atmos. Chem. Phys. 2016 , 16 , 9863 - 9873 ) and inland China (0.19 ± 0.02) ( Tian et al. Atmos. Chem. Phys. 2018 , 18 , 18203 - 18217 ) in summer. The volume concentration showed two dominant size modes at 0.9 and 2 μm. The supermicrometer particles were mostly related to sea-salt aerosols with a δ value of 0.09 over marine polar areas, ∼22% larger than in the low-latitude region because of differences in chemical composition and dry air conditions. The δ values for fine particles (<1 μm) were 0.05 ± 0.1, 50% lower than inland anthropogenic pollutants, mainly because of the complex mixtures of submicrometer sea salts. High particle concentrations in the Arctic Ocean could mostly be attributed to the strong marine emission of sea salt associated with deep oceanic cyclones, whereas long-range transport pollutants from the continent were among the primary causes of high particle concentrations in the Northwest Pacific region.

Organic tracers are useful for investigating the sources of carbonaceous aerosols but there are still no adequate studies in China. To obtain insights into the diurnal variations, properties, and the influence of regional emission controls on carbonaceous aerosols in Beijing, day-/nighttime PM 2.5 samples were collected before (Oct. 15th - Nov. 2nd) and during (Nov. 3rd - Nov. 12th) the 2014 Asia-Pacific Economic Cooperation (APEC) summit. Eleven organic compound classes were analysed using gas chromatography/mass spectrometry (GC/MS). In addition, the stable carbon isotope ratios (δ 13 C TC ) of total carbon (TC) were detected using an elemental analyser/isotope ratio mass spectrometry (EA/irMS). Most of the organic compounds were more abundant during the night than in the daytime, and their concentrations generally decreased during the APEC. These features were associated with the strict regional emission controls and meteorological conditions. The day/night variations of δ 13 C TC were smaller during the APEC than those before the APEC the summit, suggesting that regionally transported aerosols are potentially played an important role in the loading of organic aerosols in Beijing before the APEC summit. The source apportionment based on the organic tracers suggested that biomass burning, plastic and microbial emissions, and fossil fuel combustion were important sources of organic aerosols in Beijing. Furthermore, a similar contribution of biomass burning to OC before and during the APEC suggests biomass burning was a persistent contributor to PM 2.5 in Beijing and its surroundings., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Mass concentrations of chemical compounds in both PM 2.5 (particle aerodynamic diameter, Dp < 2.5 μm) and PM 2.5-10 (2.5 < Dp < 10 μm), and acidity of aerosol particles were measured at an urban site in western Japan using a continuous dichotomous Aerosol Chemical Speciation Analyzer (ACSA-12) throughout 2014. Mass concentrations of both PM 2.5 and sulfate had distinct seasonal variabilities with maxima in spring and winter, mostly due to long-range transport with the prevailing westerly wind. Mass concentration of nitrate in PM 2.5 (fNO 3 ) showed an obvious warm-season-low and cold-season-high pattern as a result of both gas-aerosol phase equilibrium processes under high temperature conditions as well as transport. Nitrate in PM 2.5-10 (cNO 3 ) increased during long-range transport of dust, implying the great importance of heterogeneous processes at the surface of coarse mode particles. In this study, Δ[H + ] (derived from the difference in pH of extract liquid with/without sampling) was used to indicate the acidity of particles. We found that acidity of particles in PM 2.5 (fΔH) was mostly positive with a maximum in August because of the large fraction of nitrate and sulfate. Acidity of particles in PM 2.5-10 (cΔH) was negative in winter and spring due to presence of alkaline matter from crustal sources. This study highlights the great importance of anthropogenic pollutants on the acidity of particles in the western Pacific Ocean and further impact on the marine environment and climate., (Copyright © 2017 The Authors. Published by Elsevier Ltd.. All rights reserved.)

A long-lasting high particulate matter (PM) concentration episode persisted over East Asia from May 24 to June 3, 2014. The Nested Air Quality Prediction Model System (NAQPMS) was used to investigate the mixing of dust and anthropogenic pollutants during this episode. Comparison of observations revealed that the NAQPMS successfully reproduced the time series PM 2.5 and PM 10 concentrations, as well as the nitrate and sulfate concentrations in fine (aerodynamic diameter ≤ 2.5 μm) and coarse mode (2.5 μm < aerodynamic diameter ≤ 10 μm). This episode originated from two dust events that occurred in the inland desert areas of Mongolia and China, and then the long-range transported dust and anthropogenic pollutants were trapped over the downwind region of East Asia for more than one week due to the blocked north Pacific subtropical high-pressure system over the east of Japan. The model results showed that mineral dust accounted for 53-83% of PM 10 , and 39-67% of PM 2.5 over five cities in East Asia during this episode. Sensitivity analysis indicated that the Qingdao and Seoul regions experienced dust and pollution twice, by direct transport from the dust source region and from dust detoured over the Shanghai area. The results of the NAQPMS model confirmed the importance of dust heterogeneous reactions (HRs) over East Asia. Simulated dust NO 3 - concentrations accounted for 75% and 84% of total NO 3 - in fine and coarse mode, respectively, in Fukuoka, Japan. The horizontal distribution of model results revealed that the ratio of dust NO 3 - /dust concentration increased from about 1% over the Chinese land mass to a maximum of 8% and 6% respectively in fine and coarse mode over the ocean to the southeast of Japan, indicating that dust NO 3 - was mainly formed over the Yellow Sea and the East China Sea before reaching Japan., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

Unlabelled: The authors analyze the sensitivities of source regions in East Asia to PM2.5 (particulate matter with an aerodynamic diameter of < or = 2.5 microm) concentration at Fukue Island located in the western part of Japan by using a regional chemical transport model with emission sensitivity simulations for the year 2010. The temporal variations in PM2.5 concentration are generally reproduced, but the absolute concentration is underestimated by the model. Chemical composition of PM2.5 in the model is compared with filter sampling data in spring; simulated sulfate, ammonium, and elemental carbon are consistent with observations, but mass concentration of particulate organic matters is underestimated. The relative contribution from each source region shows the seasonal variation, especially in summer. The contribution from central north China (105 degrees E-124 degrees E, 34 degrees N-42 degrees N) accounts for 50-60% of PM2.5 at Fukue Island except in summer; it significantly decreases in summer (18%). Central south China (105 degrees E-123 degrees E, 26 degrees N-34 degrees N) has the relative contribution of 15-30%. The contribution from the Korean Peninsula is estimated at about 10% except in summer. The domestic contribution accounts for about 7% in spring and autumn and increases to 19% in summer. We also estimate the relative contribution to daily average concentration in high PM2.5 days (> 35 microg m(-3)). Central north China has a significant contribution of 60-70% except in summer. The relative contribution from central south China is estimated at 46% in summer and about 30% in the other seasons. The contributions from central north and south China on high PM2.5 days are generally larger than those of their seasonal mean contributions. The domestic contribution is smaller than the seasonal mean value in every season; it is less than 10% even in summer. These model results suggest that foreign anthropogenic sources have a substantial impact on attainment of the atmospheric environmental standard of Japan at Fukue Island., Implications: The contribution from several source regions in East Asia to PM2.5 concentration at Fukue Island, a remote island located in the western part of Japan and close to the Asian continent, is estimated using a three-dimensional chemical transport model. The model results suggest that PM2.5 that is attributed to foreign anthropogenic sources have a larger contribution than that of domestic pollution and have a substantial impact on attainment of the atmospheric environmental standard of Japan at Fukue Island.

The unprecedented lockdown of human activities during the COVID-19 pandemic has significantly influenced social life in China. However, understanding the impact of this unique event on the emissions of different species is still insufficient, prohibiting the proper assessment of the environmental impacts of COVID-19 restrictions. Here we developed a multi-air-pollutant inversion system to simultaneously estimate the emissions of NO x , SO 2 , CO, PM 2.5 and PM 10 in China during COVID-19 restrictions with high temporal (daily) and horizontal (15 km) resolutions. Subsequently, contributions of emission changes versus meteorological variations during the COVID-19 lockdown were separated and quantified. The results demonstrated that the inversion system effectively reproduced the actual emission variations in multi-air pollutants in China during different periods of COVID-19 lockdown, which indicate that the lockdown is largely a nationwide road traffic control measure with NO x emissions decreasing substantially by ∼40 %. However, emissions of other air pollutants were found to only decrease by ∼10% because power generation and heavy industrial processes were not halted during lockdown, and residential activities may actually have increased due to the stay-at-home orders. Consequently, although obvious reductions of PM 2.5 concentrations occurred over the North China Plain (NCP) during the lockdown period, the emission change only accounted for 8.6 % of PM 2.5 reductions and even led to substantial increases in O 3. The meteorological variation instead dominated the changes in PM 2.5 concentrations over the NCP, which contributed 90 % of the PM 2.5 reductions over most parts of the NCP region. Meanwhile, our results suggest that the local stagnant meteorological conditions, together with inefficient reductions of PM 2.5 emissions, were the main drivers of the unexpected PM 2.5 pollution in Beijing during the lockdown period. These results highlighted that traffic control as a separate pollution control measure has limited effects on the coordinated control of O 3 and PM 2.5 concentrations under current complex air pollution conditions in China. More comprehensive and balanced regulations for multiple precursors from different sectors are required to address O 3 and PM 2.5 pollution in China. [ABSTRACT FROM AUTHOR]

Many efforts have been devoted to quantifying the impact of intercontinental transport on global air quality by using global chemical transport models with horizontal resolutions of hundreds of kilometers in recent decades. In this study, a global online air quality source–receptor model (GNAQPMS-SM) is designed to effectively compute the contributions of various regions to ambient pollutant concentrations. The newly developed model is able to quantify source–receptor (S-R) relationships in one simulation without introducing errors by nonlinear chemistry. We calculate the surface and planetary boundary layer (PBL) S-R relationships in 19 regions over the whole globe for ozone (O 3), black carbon (BC), and non-sea-salt sulfate (nss-sulfate) by conducting a high-resolution (0.5 ∘ × 0.5 ∘) simulation for the year 2018. The model exhibits a realistic capacity in reproducing the spatial distributions and seasonal variations of tropospheric O 3 , carbon monoxide, and aerosols at global and regional scales – Europe (EUR), North America (NAM), and East Asia (EA). The correlation coefficient (R) and normalized mean bias (NMB) for seasonal O 3 at global background and urban–rural sites ranged from 0.49 to 0.87 and - 2 % to 14.97 %, respectively. For aerosols, the R and NMB in EUR, NAM, and EA mostly exceed 0.6 and are within ± 15 %. These statistical parameters based on this global simulation can match those of regional models in key regions. The simulated tropospheric nitrogen dioxide and aerosol optical depths are generally in agreement with satellite observations. The model overestimates ozone concentrations in the upper troposphere and stratosphere in the tropics, midlatitude, and polar regions of the Southern Hemisphere due to the use of a simplified stratospheric ozone scheme and/or biases in estimated stratosphere–troposphere exchange dynamics. We find that surface O 3 can travel a long distance and contributes a non-negligible fraction to downwind regions. Non-local source transport explains approximately 35 %–60 % of surface O 3 in EA, South Asia (SAS), EUR, and NAM. The O 3 exported from EUR can also be transported across the Arctic Ocean to the North Pacific and contributes nearly 5 %–7.5 % to the North Pacific. BC is directly linked to local emissions, and each BC source region mainly contributes to itself and surrounding regions. For nss-sulfate, contributions of long-range transport account for 15 %–30 % within the PBL in EA, SAS, EUR, and NAM. Our estimated international transport of BC and nss-sulfate is lower than that from the Hemispheric Transport of Air Pollution (HTAP) assessment report in 2010, but most surface O 3 results are within the range. This difference may be related to the different simulation years, emission inventories, vertical and horizontal resolutions, and S-R revealing methods. Additional emission sensitivity simulation shows a negative O 3 response in receptor region EA in January from EA. The difference between two methods in estimated S-R relationships of nss-sulfate and O 3 are mainly due to ignoring the nonlinearity of pollutants during chemical processes. The S-R relationship of aerosols within EA subcontinent is also assessed. The model that we developed creates a link between the scientific community and policymakers. Finally, the results are discussed in the context of future model development and analysis opportunities. [ABSTRACT FROM AUTHOR]

Many efforts have been devoted to quantifying the impact of intercontinental transport on global air quality by using global chemical transport models with horizontal resolutions of hundreds of kilometers in recent decades. In this study, a global online air quality source-receptor model (GNAQPMS-SM) is designed to effectively compute the contributions of various regions to ambient pollutant concentrations. The newly developed model is able to quantify source-receptor (S-R) relationships in one simulation without introducing errors by nonlinear chemistry, which largely reduces the computation costs compared to the brute force method. We calculate the surface and planetary boundary layer (PBL) S-R relationships in 19 regions over the whole globe for ozone, black carbon (BC) and non-sea-salt sulphate (nss-sulphate) by conducting a high-resolution (0.5° × 0.5°) simulation for the year 2018. The model exhibits a realistic capacity in reproducing the spatial distributions and seasonal variations of tropospheric ozone, carbon monoxide, and aerosols at global and regional scales (Europe, North America and East Asia). The correlation coefficient (R) and normalized mean bias (NMB) for seasonal ozone at global background and urban-rural sites ranged from 0.49 to 0.87 and −2 % to 14.97 %, respectively. For aerosols, the R and NMB in Europe, North America and East Asia mostly exceed 0.6 and are within ±15 %. These statistical parameters based on this global simulation can match those of regional models in key regions. The simulated tropospheric nitrogen dioxide and aerosol optical depths are generally in agreement with satellite observations. The model overestimates ozone mixing ratios in the upper troposphere and stratosphere in the tropics, mid-latitude and polar regions of the Southern Hemisphere due to the use of a simplified stratospheric ozone scheme and/or biases in estimated stratosphere-troposphere exchange dynamics. We find that O3 in the surface layer can travel a long distance and contributes a nonnegligible fraction to downwind regions. Nonlocal source transport explains approximately 35-60 % of surface O3 in East Asia, South Asia, Europe and North America. The O3 exported from Europe can also be transported across the Arctic Ocean to the North Pacific and contributes nearly 5-7.5 % to the North Pacific. BC, as a primary aerosol, is directly linked to local emissions, and each BC source region mainly contributes to itself and surrounding regions. For nss-sulphate, contributions of long-range transport account for 15-30 % within the PBL in East Asia, South Asia, Europe and North America. Our estimated international transport is lower than that from the Hemispheric Transport of Air Pollution (HTAP) assessment report in 2010. In this study, local contributions to surface nss-sulphate and BC exceed the ranges given in the HTAP model, while local contributions to nss-sulphate and BC within the PBL are mainly within the ranges. This difference may be related to the different simulation years, emission inventories, horizontal resolutions and S-R revealing methods. The S-R relationship of aerosols within the East Asia subcontinent is also assessed. The model that we developed creates a link between the scientific community and policymakers. Finally, the results are discussed in the context of future model development and analysis opportunities. [ABSTRACT FROM AUTHOR]

The uncertainty in the quantitative estimates of long-range transport of pollutants in air quality models is large. In this study, based on the Global Nested Air Quality Prediction Modeling System (GNAQPMS-SM), using Latin hypercube sampling (LHS) method, we conducted a base simulation and an ensemble of 1° × 1° simulations in April 2017 to assess the uncertainty in model estimates of O 3 and PM 2.5 intercontinental transport from uncertainties in input parameters (emissions, temperature, wind field). The results show that the base simulation has biases in some regions, and when the uncertainty of input parameters is taken into account, the observations mostly lie within the uncertainty range of the 50 simulated group samples. The uncertainties of input parameters are reasonably quantified in terms of their propagation during computation in GNAQPMS-SM. The best performance occurs with the multiple linear regression (MLR) method, which is used to fit ensemble simulation results. The uncertainty range of monthly O 3 transport from North America (NAM) to Europe (EUR) at a 1.2 km altitude is 4.91–5.44 ppb, from EUR to China is 0.78–0.96 ppb, and from China to NAM is 0.76–0.85 ppb. Correspondingly, the MLR result of each is 5.12 ppb, 0.80 ppb, and 0.77 ppb, respectively. The MLR result is thought to be closer to the actual transport amounts, and most of them lie within the uncertainty range. The appreciable differences between base simulation and MLR results reflect the uncertainties in the input parameters. Finally, taking O 3 transport from China to Japan as an example, the maximum absolute value of the daily average Spearman correlation coefficient | ρ ‾ | max between input parameters and contributions is calculated to identify the key uncertainty sources in several regions of O 3 transport to Japan. Meteorological and air pollutant observations and the performance of meteorological simulations should be strengthened. [Display omitted] • An uncertainty analysis is conducted to estimate uncertainties of S-R relationships. • The uncertainties of input parameters well explain most of the simulation deviation. • The uncertainties of S-R relationships are reasonably quantified. • Key uncertainty source during O 3 transport from East China to Japan is identified. • Meteorological and air pollutant monitoring are suggested to be strengthened. [ABSTRACT FROM AUTHOR]