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Fine particulate matter (PM 2.5 ) in Northeast China was targeted by national-level clean air policy for the first time in 2022, with the release of Action Plan to eliminate heavy air pollution events. In this study, we investigated sources of PM 2.5 during three successive winters in Harbin, a megacity in Northeast China, based on observational results from several recent campaigns in 2018-2021. During the 2020-2021 campaign, daytime and nighttime samples were collected in specific months in addition to 24-h integrated measurements, and the two sets of samples were combined in different ways to run a positive matrix factorization model. The source apportionment results suggested that the resolved secondary organic carbon (SOC PMF ) had an uncertainty of ∼12%. Secondary aerosols were found to show the following features for the typical winters without agricultural fires. First, SOC PMF could be properly constrained by results from another widely-used approach for SOC estimation, the elemental carbon-tracer method. Second, secondary PM 2.5 calculated using SOC PMF and secondary inorganic ions were generally in line with the independent estimations based on air quality data. Third, secondary components accounted for more than 50% of PM 2.5 on average and contributed even more significantly during severe haze episodes, which were the focus of the latest Action Plan. This study also found that the wintertime PM 2.5 decreased more slowly during 2017-2021 compared to 2013-2017, by ∼1 and 10 μg/m 3 per year, respectively, for the metropolitan area where Harbin is located at. Our results highlighted the importance of secondary aerosols for further improving air quality in Northeast China, and for avoiding heavy pollution as required by the latest Action Plan., 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.)

COVID-19 rebounded in China in January 2021, with Heilongjiang as one of the worst-affected provinces. This resulted in a new round of lockdown in Harbin, the capital city of Heilongjiang, from 20 January to 22 February of 2021. A field campaign was conducted to explore the responses of haze pollution in Harbin to the lockdown. Levoglucosan was used to reflect biomass burning emissions, while the molar ratio of sulfur (the sum of sulfur dioxide and sulfate) to nitrogen (the sum of nitrogen dioxide and nitrate), i.e., R S/N , was used as an indicator for the relative importance of coal combustion and vehicle emissions. Based on a synthesis of the levoglucosan and R S/N results, reference period was selected with minimal influences of non-lockdown-related emission variations. As indicated by the almost unchanged sulfur dioxide concentrations, coal combustion emissions were relatively stable throughout the lockdown and reference periods, presumably because the associated activities, e.g., heating supply, power generation, etc., were usually uninterruptible. On the other hand, as suggested by the increase of R S/N , vehicle emissions were considerably reduced during lockdown, likely due to the stay-at-home orders. Compared to results from the reference samples, the lockdown period exhibited higher levels of ozone and various indicators for secondary aerosol formation, pointing to an enhancement of secondary pollution. In addition, photochemistry-related reactions in aqueous phase appeared to be present during the lockdown period, which have not been reported in the frigid atmosphere over Northeast China., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Severe haze hovered over Harbin during the heating season of 2019-2020, making it one of the ten most polluted Chinese cities in January of 2020. Here we focused on the optical properties and sources of brown carbon (BrC) during the extreme atmospheric pollution periods. Enhanced formation of secondary BrC (BrC sec ) was evident as relative humidity (RH) became higher, accompanied with a decrease of ozone but concurrent increases of aerosol water content and secondary inorganic aerosols. These features were generally similar to the characteristics of haze chemistry observed during winter haze events in the North China Plain, and indicated that heterogeneous reactions involving aerosol water might be at play in the formation of BrC sec , despite the low temperatures in Harbin. Although BrC sec accounted for a substantial fraction of brown carbon mass, its contribution to BrC absorption was much smaller (6 vs. 28%), pointing to a lower mass absorption efficiency (MAE) of BrC sec compared to primary BrC. In addition, emissions of biomass burning BrC (BrC BB ) were inferred to increase with increasing RH, coinciding with a large drop of temperature. Since both the less absorbing BrC sec and the more absorbing BrC BB increased as RH became higher, the MAE of total BrC were largely unchanged throughout the measurement period. This study unfolded the contrast in the source apportionment results of BrC mass and absorption, and could have implications for the simulation of radiative forcing by brown carbon., (Copyright © 2021 Elsevier Inc. All rights reserved.)

The massive agricultural sector in the Northeast Plain, which is of great importance for the food security in China, results in a huge amount of crop residues and thus substantial concern on haze pollution due to biomass burning (BB). To seek for effective control measures on BB emissions, a dramatic transition of open burning policy occurred in Heilongjiang Province, from the "legitimate burning" policy released in 2018 to the "strict prohibition" policy implemented in 2019 and beyond. Here we explored the BB aerosols during 2020-2021 in Harbin, the capital city of Heilongjiang. Although open burning was strictly prohibited by mandatory bans, agricultural fires were not actually eliminated, as indicated by the levoglucosan levels and fire count results. In general, the BB aerosols in Harbin were attributed to the overlaying of household burning and agricultural fire emissions. The former factor laid the foundation of biomass burning impacts, with BB contributions to organic carbon and elemental carbon (f BBOC and f BBEC ) of 35 and 47%, respectively. The latter further enhanced the BB impacts during specific episodes breaking out in the spring of 2021 as well as the fall of 2020, when f BBOC and f BBEC increased to 64 and 57%, respectively. In addition, comparing to the fires of 2018-2019 which occurred in winter (in response to the "legitimate burning" policy), the agricultural fires were shifted to spring and fall in the 2020-2021 campaign, accompanied with an increase of combustion efficiency. This study illustrated how the agricultural fire emissions were influenced by the transition of open burning policy., 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.)

Quantifying the sources of atmospheric particles is essential to air quality control but remains challenging, especially for the source apportionment of particles based on number concentration with wide size range. Here, particle number concentrations (PNC) with size range 19-20,000 nm involving four modes Nucleation, Aitken, Accumulation, and Coarse are used to do source apportionment of PNC at the Guangdong Atmospheric Supersite (Heshan) during July-October 2015 by nonnegative matrix factorization (NMF) with 6 factors. For July 2015, separated source apportionments for three different size ranges from collocated instruments nano scanning mobility particle sizer (NSMPS), SMPS, and aerodynamic particle sizer (APS) and for two different size ranges (below and above 100 nm) show similar quantitative source information with that for the one whole size range. The mean absolute difference of contribution percentages of total particle number concentrations (TPNC) based on 5 unique apportioned sources is 5.6 % (4.3-7.6 %) for the instrument segregated apportionment and 4.2 % (0-5.3 %) for the size range segregated apportionment respectively, relative to the one whole apportionment. Moreover, the contribution percentages of TPNC are close to the weighted sum of contribution percentages of all size bins, with a mean absolute difference of 1.1 % (0-3.4 %). In both these two aspects, the consistency among different technical paths proves the matrix factorization by NMF is practically desirable and the simplicity of reducing some steps or calculations saves time. Besides, dust can be identified with the wide size range including larger than 3000 nm. Six apportioned sources in the 4 months are Accumulation (32.4 %), Nucleation (20.0 %), Aitken (15.2 %), traffic (14.6 %), dust (10.6 %), and Coarse (7.1 %). Therefore, NMF would serve as a promising tool for PNC source apportionment with wide size range and conducting the apportionment with the whole size range in one matrix factorization procedure and using the single TPNC contribution percentage are feasible., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Complex air pollutant sources and distinct meteorological conditions resulted in unique wintertime haze pollution in the Harbin-Changchun (HC) metropolitan area, China's only national-level city cluster located in the severe cold climate region. In this study, field observation and air quality modeling were combined to investigate fine particulate matter (PM 2.5 ) pollution during a six-month long heating season in HC's central city (Harbin). The model significantly underpredicted PM 2.5 and organic carbon (by up to ∼230 μg/m 3 and 110 μgC/m 3 , respectively, in terms of daily average) when levoglucosan concentrations were above 0.5 μg/m 3 . Based on a synthesis of levoglucosan concentrations and fire counts, the large gaps were attributed to underestimation of open burning emissions by the model. However, the model tended to overpredict elemental carbon (more significantly at higher NO 2 ), likely pointing to an overestimation of vehicle emissions. With increasing levoglucosan, the difference between observed and simulated nitrate (nitrate obs ‒ nitrate mod , i.e., Δnitrate) showed a transition from negative to positive values. The positive Δnitrate were attributed to underprediction of the open-burning related nitrate, whereas the negative Δnitrate were likely caused by overprediction of nitrate from other sources (presumably vehicle emissions). The dependence of Δnitrate on levoglucosan indicated that with stronger impact of open burning, the overprediction effect was gradually offset and finally overwhelmed. Influence of open burning on sulfate formation was evident as well, but less apparent compared to nitrate. This study illustrates how the uncertainties in open burning emissions will influence PM 2.5 simulation, on not only primary components but also secondary species., 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.)

The characteristics of secondary inorganic aerosol including sulfate, nitrate and ammonium (SNA) were investigated during a six-month long heating season in the Harbin-Changchun metropolitan area, i.e., China's only national-level city cluster located in the severe cold climate region. The contribution of SNA to fine particulate matter (PM 2.5 ) tended to decrease with increasing PM 2.5 concentration, opposite to the trend repeatedly observed during winter in Beijing. Heterogeneous sulfate formation was still evident when the daily average temperature was as low as below -10 °C, with the preconditions of high relative humidity (RH; above ∼80%) and high nitrogen dioxide (above ∼60 μg/m 3 ). Both the sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR) were enhanced at high RH, reaching ∼0.3. However, the high RH conditions were not commonly seen during the heating season, which should be responsible for the overall lack of linkage between the SNA contribution and PM 2.5 temporal variation., 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.)

Fine particulate matter (PM 2.5 ) pollution in Beijing was investigated based on field observation and air quality modeling. Measurement results showed that when using elemental carbon (EC) as the reference component, concurrent increases were observed in the relative abundances of sulfate, nitrate, organic carbon (OC) and water-soluble organic carbon (WSOC) when RH exceeded ∼65% during winter. The observed increases could not be explained by variations of primary biomass burning emissions, instead they likely pointed to heterogeneous chemistry and presumably indicated that formation of secondary inorganic and organic aerosols might be related during winter haze events in Beijing. Large gaps were found in winter when comparing the observational and modeling results. In summer, RH exhibited little influence on the observed sulfate/EC, OC/EC or WSOC/EC, and the observed and modeled results were in general comparable for the concentrations of sulfate, EC and OC. This study suggests that distinct yet poorly-understood atmospheric chemistry may be at play in China's winter haze events, and it could be a substantial challenge to properly incorporate the related mechanisms into air quality models., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Carbonaceous aerosol was measured during fall of 2010 in Beijing. Daily variation of organic carbon (OC) was found to coincide with that of relative humidity (RH), and the OC to elemental carbon (EC) ratios were more than doubled during the more humid periods (RH above 0.75) compared to other conditions. This large increase in OC/EC could not be explained by the variations of primary biomass burning emissions but was accompanied by a five-fold increase in the sulfate to EC ratio. It was then inferred that secondary organic aerosol (SOA) formation was enhanced under the more humid conditions, presumably through aqueous-phase processes. This enhanced SOA formation might be partially associated with particles externally mixed with black carbon, as indicated by the RH-dependent relationships between aerosol optical attenuation and EC loading. In addition, organic aerosols exhibited different properties between the more humid and the other periods, such that they were less volatile and charred more significantly during thermal-optical analysis in the former case. These differences coincided with the evidence of enhanced SOA formation under the more humid conditions. This study highlights the necessity of incorporating aqueous-phase chemistry into air quality models for SOA., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Exposure to ambient fine particulate matter (PM 2.5 ) is a leading risk factor for the global burden of disease. However, uncertainty remains about PM 2.5 sources. We use a global chemical transport model (GEOS-Chem) simulation for 2014, constrained by satellite-based estimates of PM 2.5 to interpret globally dispersed PM 2.5 mass and composition measurements from the ground-based surface particulate matter network (SPARTAN). Measured site mean PM 2.5 composition varies substantially for secondary inorganic aerosols (2.4-19.7 μg/m 3 ), mineral dust (1.9-14.7 μg/m 3 ), residual/organic matter (2.1-40.2 μg/m 3 ), and black carbon (1.0-7.3 μg/m 3 ). Interpretation of these measurements with the GEOS-Chem model yields insight into sources affecting each site. Globally, combustion sectors such as residential energy use (7.9 μg/m 3 ), industry (6.5 μg/m 3 ), and power generation (5.6 μg/m 3 ) are leading sources of outdoor global population-weighted PM 2.5 concentrations. Global population-weighted organic mass is driven by the residential energy sector (64%) whereas population-weighted secondary inorganic concentrations arise primarily from industry (33%) and power generation (32%). Simulation-measurement biases for ammonium nitrate and dust identify uncertainty in agricultural and crustal sources. Interpretation of initial PM 2.5 mass and composition measurements from SPARTAN with the GEOS-Chem model constrained by satellite-based PM 2.5 provides insight into sources and processes that influence the global spatial variation in PM 2.5 composition.

High molecular weight organic compounds (HMW-OCs), formed as secondary organic aerosols (SOA), have been reported in many laboratory studies. However, little evidence of HMW-OCs formation, in particular during winter season in the real atmosphere, has been reported. In January 2013, Beijing faced historically severe haze pollution, in which the hourly PM 2.5 concentration reached as high as 974 μg m -3 . Four typical haze events (HE1 to HE4) were identified, and HE2 (Jan. 9-16) was the most serious of these. Based on the hourly observed chemical composition of PM 2.5 and the daily organic composition analyzed by matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF-MS), we found that abundant ion peaks in m/z 200-850 appeared on heavy haze days, whereas these were negligible on a clear day, indicating the existence of HMW-OCs in the wintertime haze. A negative nonlinear correlation between HMW-OCs and O 3 suggested that gas oxidation was not likely to be the dominant mechanism for HMW-OCs formation. During the heavy haze events, the relative humidity and mass ratio of H 2 O/PM 2.5 reached as high as 80% and 0.2, respectively. The high water content and its good positive correlation with HMW-OCs indicated that an aqueous-phase process may be a significant pathway in wintertime. The evidence that acidity was much higher during HE2 (0.37 μg m -3 ) than on other days, as well as its strong correlation with HMW-OCs, indicated that acid-catalyzed reactions likely resulted in HMW-OCs formation during the heavy winter haze in Beijing., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Pollution characteristic and variation trend of atmospheric carbonyls were investigated in November during the 2014 Beijing APEC. Formaldehyde, acetaldehyde and acetone were the dominant carbonyls, accounting for 82.66% of total carbonyls, and especially, formaldehyde accounted for 40.12% of total carbonyls. Atmospheric concentrations of total carbonyls decreased by around 64.10% after the clean air policy was carried out during the Beijing APEC, and the variation trend of carbonyls showed a similar pattern to those of other pollutants like PM₂.₅ during the APEC. Strong correlations (R² of 0.67-0.98) were observed among formaldehyde, acetaldehyde, acetone and total carbonyls during and after the APEC, indicating that they had similar sources; however, poor correlations (R² of -0.11-0.42 and 0.16-0.94, respectively) were observed before the APEC, implying different emission sources for ambient carbonyls. The calculated ratios of C1/C2, C2/C3 and OC/EC indicated that both vehicles and coal emissions were responsible for atmospheric carbonyls before the APEC, and emissions from coal burning were the major contributor to atmospheric carbonyls during and after the APEC, especially after the APEC.

Recently, PM2.5 (atmospheric fine particulate matter with aerodynamic diameter ≤ 2.5 μm) have received so much attention that the observations, source appointment and countermeasures of it have been widely studied due to its harmful impacts on visibility, mood (mental health), physical health, traffic safety, construction, economy and nature, as well as its complex interaction with climate. A review on the PM2.5 related research is necessary. We start with summary of chemical composition and characteristics of PM2.5 that contains both macro and micro observation results and analysis, wherein the temporal variability of concentrations of PM2.5 and major components in many recent reports is embraced. This is closely followed by an overview of source appointment, including the composition and sources of PM2.5 in different countries in the six inhabitable continents based on the best available results. Besides summarizing PM2.5 pollution countermeasures by policy, planning, technology and ideology, the World Air Day is proposed to be established to inspire and promote the crucial social action in energy-saving and emission-reduction. Some updated knowledge of the important topics (such as formation and evolution mechanisms of hazes, secondary aerosols, aerosol mass spectrometer, organic tracers, radiocarbon, emissions, solutions for air pollution problems, etc.) is also included in the present review by logically synthesizing the studies. In addition, the key research challenges and future directions are put forward. Despite our efforts, our understanding of the recent reported observations, source identifications and countermeasures of PM2.5 is limited, and subsequent efforts both of the authors and readers are needed., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Current understanding of organic aerosol (OA) is challenged by the large gap between simulation results and observational data. Based on six campaigns conducted in a representative mega city in China, this study provided an annual perspective of the uncertainties in observational OA data caused by sampling artifacts. Our results suggest that for the commonly-used sampling approach that involves collection of particles on a bare quartz filter, the positive artifact could result in a 20-40 % overestimation of OA concentrations. Based on an evaluation framework that includes four criteria, an activated carbon denuder was demonstrated to be able to effectively eliminate the positive artifact with a long useful time of at least one month, and hence it was recommended to be a good choice for routine measurement of carbonaceous aerosol., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Based on the newly established high-performance anion exchange chromatography with pulsed amperometric detection (HPAEC-PAD), the saccharides in PM2.5 and PM10 in Beijing from 2011 - 2012 were quantified. Fourteen saccharides were synchronously detected in the aerosols samples in Beijing, which can be divided into three categories, i. e. anhydrosugar, sugar and sugar alcohol. Anhydrosugar, coming from biomass burning, include levoglucosan, mannosan and galactosan. Sugar and sugar alcohol, emitted by the primary biogenic emission, include glucose, fructose, trehalose, arabitol, mannitol, glycerol, threitol, 2-meythltrtols (2-methylthreitol and 2-methylerythrito), xylitol and inositol. The concentrations of monosaccharide anhydrides in summer and autumn were obviously higher than those in spring and winter, while the concentrations of sugar and sugar alcohol in winter were significantly lower than those in other seasons. The results of positive matrix factorization analysis suggested that saccharides compounds in atmospheric PM in Beijing can be derived from biomass burning, suspended soil or dust, isoprene SOA, as well as direct release of airborne fungal spores and pollen.

Heavily-polluted PM₂.₅ (fine particulate matter) episodes frequently impacting Beijing, especially during winter, have become a substantial concern. We found that during winter, the daily variation of PM2.5 in Beijing tracked the pattern of relative humidity (RH). With the increase of PM₂.₅ (or RH), water-soluble components (especially inorganic ions) became more abundant, and the water-soluble organic carbon to organic carbon ratios increased. The nitrate to sulfate ratios also exhibited dependence on RH, and were higher than those measured about a decade ago, consistent with the increasing trend of nitrogen oxides emissions. Surprisingly, the ratios of water-insoluble organic carbon to elemental carbon showed significant increase at high RH levels, presumably indicating the formation of secondary organic aerosol that is not soluble in water. In addition, humid winters were occasionally identified during 1996-2013 which are expected to be favorable for the formation of air pollution episodes with high PM₂.₅ concentrations., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Foshan is a ceramics manufacturing center in the world and the most polluted city in the Pearl River Delta (PRD) in southern China measured by the levels of atmospheric heavy metals. PM2.5 samples were collected in Foshan in winter 2008. Among the 22 elements and ions analyzed, 7 heavy metals (Zn, V, Mn, Cu, As, Cd and Pb) were studied in depth for their levels, spatiotemporal variations and sources. The ambient concentrations of the heavy metals were much higher than the reported average concentrations in China. The levels of Pb (675.7 ± 378.5 ng/m(3)), As (76.6 ± 49.1 ng/m(3)) and Cd (42.6 ± 45.2 ng/m(3)) exceeded the reference values of NAAQS (GB3095-2012) and the health guidelines of the World Health Organization. Generally, the levels of atmospheric heavy metals showed spatial distribution as: downtown site (CC, Chancheng District)>urban sites (NH and SD, Nanhai and Shunde Districts)>rural site (SS, Shanshui District). Two sources of heavy metals, the ceramic and aluminum industries, were identified during the sampling period. The large number of ceramic manufactures was responsible for the high levels of atmospheric Zn, Pb and As in Chancheng District. Transport from an aluminum industry park under light north-west winds contributed high levels of Cd to the SS site (Shanshui District). The average concentration of Cd under north-west wind was 220 ng/m(3), 20.5 times higher than those under other wind directions. The high daily maximum enrichment factors (EFs) of Cd, Pb, Zn, As and Cu at all four sites indicated extremely high contamination by local emissions. Back trajectory analysis showed that the heavy metals were also closely associated with the pathway of air mass. A positive matrix factorization (PMF) method was applied to determine the source apportionment of these heavy metals. Five factors (industry including the ceramic industry and coal combustion, vehicle emissions, dust, transportation and sea salt) were identified and industry was the most important source of atmospheric heavy metals. The present paper suggests a control policy on the four heavy metals Cd, Pb, Zn, and Cu, and suggests the inclusion of As in the ceramic industry emission standard in the future., (Copyright © 2014 Elsevier B.V. All rights reserved.)

The chemical composition of Beijing aerosol was measured during summer and winter. Two distinct episodes were identified. Water-soluble potassium (K(+)) increased significantly during the firework episode in winter with an episode to non-episode ratio of 4.97, whereas the biomass burning (BB) episode in summer was characterized by high episode to non-episode ratios of levoglucosan (6.38) and K(+) (6.90). The BB and firework episodes had only a minor influence on the water-soluble OC (organic carbon) to OC ratio. Based on separate investigations of episode and non-episode periods, it was found that: (i) sulfate correlated strongly with both relative humidity and nitrate during the typical winter period presumably indicating the importance of the aqueous-phase oxidation of sulfur dioxide by nitrogen dioxide, (ii) oxalate and WSOC during both winter and summer in Beijing were mainly due to secondary formation, and (iii) high humidity can significantly enhance the formation potential of WSOC in winter., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Total suspended particles (TSP), collected during a typical haze period in Guangzhou, were analyzed for the fatty acids (C12-C30) and low molecular weight dicarboxylic acids (C3-C9) using gas chromatography/mass spectrometry (GC/MS). The results showed that the concentration of total fatty and carboxylic acids was pretty high during the haze episode. The ratios of fatty acids and carboxylic acids in haze to those in normal days were 1.9 and 2.5, respectively. During the episode of the increasing pollution, the fatty acids and carboxylic acids at night (653 ng x m(-3)) was higher than that (487 ng x m(-3)) in days. After that, the level of fatty acids and carboxylic acids in days (412 ng x m(-3)) was higher than that (336 ng x m(-3)) at night. In general, the time-series of fatty acids and carboxylic acids was similar to that of the air particle and carbonaceous species, however, the trend of the ratio of fatty acids and carboxylic acids to organic carbon was opposite to that of air particle and carbonaceous species. This ratio decreased with the increase of the concentration of air particle and after the night of 27th, the ratio increased with the decrease in the concentration of air particle. The results showed that haze pollution had a significant inhibitory effect on the enrichment of fatty and carboxylic acids. Based on the ratio of malonate to succinate (C3/C4), it could be found that primary sources contribute more to the atmospheric fatty and carboxylic acids during the autumn haze pollution periods in Guangzhou.

Volatile Organic Compounds (VOCs) in Foshan City were investigated in December 6 to 30 2008. The concentrations of VOCs in haze days were significantly higher than those in no-haze days. Toluene (68.93 microg x m(-3) +/- 37.78 microg x m(-3)) was the most abundant compound of VOCs in haze days and i-pentane (20.59 microg x m(-3) +/- 14.28 microg x m(-3)) was the most abundant compound in no-haze days, respectively. During haze episodes, the diurnal variations of alkanes and alkynes were not significantly; however, alkenes and aromatic hydrocarbon decreased significantly at noon. During no-haze episodes, the diurnal variations patterns of VOCs were stable. Propylene-equivalent concentrations in haze days were significantly higher than those in no-haze days, toluene was the most abundant compound of Propylene-equivalent concentration in haze days, followed by propene and ethene; propene was the most abundant compound in no-haze days, followed by ethene and 1-butene. High concentration of benzene (18.1 microg x m(-3)) in haze days posed a great health threat to public in Foshan city. Both diurnal variation of VOCs and measured ratios indicated vehicular emissions acted as the main sources of most VOCs and other sources like solvent application also contributed to VOCs (benzene and toluene).

PM2.5 emissions and polycyclic aromatic hydrocarbons (PAHs) in PM2.5 of pure biodiesel derived from different feedstocks were investigated and compared with diesel fuel. B100-1 (soyabean oil derived), B100-2 (waste oil derived) and diesel fuel were tested on a diesel engine bench at four operating conditions, including two steady speeds of different loads. The fine particles were collected by fiber quartz filter and particle phase PAHs were analyzed by GC-MS. Compared with diesel fuel, biodiesel decreased PM2.5 emission rates with a maximal reduction rate of 37.3% at operating modes of high loads, while increased PM2.5 emission rates at low loads. PAHs emission rates from biodiesel decreased at all tested modes, with a maximal reduction rate of 77.6%. The emission rates of PM2.5 and PAHs of B100-2 were 14.7% and 17.8% times of B100-1. Low molecular weight PAHs dominated in the emission of three fuels with phenanthrene as maxima and 2-ring and 3-ring PAHs accounted for more than 50% of the total PAHs. Toxic equivalence of PAHs emissions of biodiesel was decreased greatly compared with that of diesel.

The air quality in Beijing and surrounding area is influenced by local emission and regional transport. To study the characteristics of regional pollution, PM (particulate matter) samples were collected simultaneously at 4 sites including Tsinghua University (TH) and Miyun reservoir (MY) in Beijing, Renqiu (RQ, Hebei Province), and Shangdu (SD, Inner Mongolia) during August, 2007, and temporal/spatial distributions of PM2.5 mass concentrations along with 22 elements in TSP were characterized. PM2.5 mass concentrations were quite different at 4 sites, following the sequence as RQ > TH > MY > SD. The highest concentrations of pollution-derived elements S, Zn, Pb, Cu, As, Sb, Ni, Cd, In, Se were found in RQ, showing the most intensive anthropogenic influence around this region, and their lowest variation indicated that the pollution mostly came from local sources. Controlled by the meteorological factors, highest daily variations of these elements were found at SD with relative lower concentrations. The correlation coefficients of S, Pb, Cd, In, As, Zn concentrations between TH and MY were all higher than 0.70, which implies similar sources for these elements at the 2 sites in Beijing. At the beginning and the end of the Sawtooth pollution episode in Beijing, concentrations of most elements in Miyun were comparable with the lowest concentrations at Shangdu observed during the sampling period, which means Miyun could well represent the regional characteristics of clean air mass from the northwest. Uniform spatial distribution of high sulfate was found (about 10 microg/m3) at the peaks of Sawtooth episode, which implies the important contribution from secondary aerosol during the regional pollution. Variable sources of PM at each site and their regional influence were discussed based on the different characteristics of elemental enrichment factors.

Acetal (1,1-diethoxyethane) is considered as an alternative to ethanol as bio-derived additive for diesel fuel, which is miscible in diesel fuel. Biodiesel can improve the oxygen content and flash point of the fuel blend of acetal and diesel fuel. Two oxygenated fuels were prepared: a blend of 10% acetal + 90% diesel fuel and 10% acetal + 10% biodiesel + 80% diesel fuel. The emissions of NO(x), HC and PM2.5 from oxygenated fuels were investigated on a diesel engine bench at five modes according to various loads at two steady speeds and compared with base diesel fuel. Additionally, the carbon compositions of PM2.5 were analyzed by DRI thermal/optical carbon analyzer. Oxygenated fuels have unconspicuous effect on NO(x) emission rate but HC emission rate is observed significantly increased at some modes. The emission rate of PM2.5 is decreased by using oxygenated fuels and it decreases with the increase of fuel oxygen content. The emission rates of TC (total carbon) and EC (elemental carbon) in PM2.5 are also decreased by oxygenated fuels. The emission rate of organic carbon (OC) is greatly decreased at modes of higher engine speed. The OC/EC ratios of PM2.5 from oxygenated fuels are higher than that from base diesel fuel at most modes. The carbon compositions fractions of PM2.5 from the three test fuels are similar, and OC1 and EC1 are contributed to the most fractions of OC and EC, respectively. Compared with base diesel fuel, oxygenated fuels decrease emission rate of PM2.5, and have more OC contribution to PM2.5 but have little effect on carbon composition fractions.

Vehicle specific power (VSP) and engine stress (ES) were introduced to reflect the driving characteristics of vehicles in China. Emission rates of 60 BIN based on VSP and ES for light-duty vehicles were calculated on the basis of the on-board emission test data in 5 cities of China. The driving cycle-based mobile emission model (DCMEM) was developed to simulate CO, NOx and HC emission factors of light-duty vehicles for different cities or driving cycles. The differences in CO and NOx emission factors between the DCMEM simulation results and the emissions testing results were less than 10%, and less than 18% for HC.

A bottom-up PM emission model was developed based on the production technologies and PM emission control devices in Chinese cement industry. Through analyzing the historical distribution of technologies in cement producing and the impact of standards on PM emission control from cement industry, emission factors of cement industry in China during 1990-2004 were generated by this technology-based model, and emission inventories were developed thereby. Emission factor decreased from 27.9 kg x t(-1) cement in 1990 to 8.05 kg x t(-1) cement in 2004. Emissions of PM from cement industry in China reached the peak value in 1997, with 1044 x 10(4) t of TSP, 716 x 10(4) t of PM10, 436 x 10(4) t of PM2.5 emitted, then decreased until 2001, and increased slowly again during 2001-2004. The distribution of PM emissions among provinces is uneven. Shandong, Guangdong, Hebei, Jiangsu, Zhejiang, and Henan contribute more than 50% of emissions of China. Rapid spread of pre-calcining kilns in China and implementation of Emission Standard of Air Pollutants for Cement Industry in 2004 will probably decrease PM emissions from cement industry to a large extent, leading to obvious variation on PM pollution characteristics in China.

The purpose of this study is to investigate the effect of fog processes on the physical and chemical properties of aerosol particles in an urban atmosphere. Atmospheric particles were collected in the urban atmosphere of Beijing during fog and non-fog episodes. The morphology, size and elemental composition of individual particles were characterized using a scanning electron microscope (SEM) equipped with an energy dispersive X-ray spectrometer (EDX). EDX analysis showed that elongated particles were composed of Ca-K-S or Ca-S, and most sub-round particles contained sulfur. Large amounts of elongated and sub-round particles were identified in the samples collected during fog episodes, and they were rarely detected in the samples collected during non-fog episodes. This suggests that the high relative humidity in the fogs facilitated the formation of elongated and sub-round particles. Number concentrations of particles larger than 0.2 microm were about 5 to 8 times higher during the fog episodes. In addition, a new mode around 0.4 microm appeared in number size distribution of particles during the fog episodes. These results indicate that heterogeneous reactions in the fogs could greatly change the chemical and physical properties of particles.

Number concentration and distribution of airborne particles in the size range 5.6 to 560 nm diameter were measured in Beijing for a 15-d period in winter 2005. Daily average number concentrations of nucleation mode (5.6-20 nm), Aitken mode (20-100 nm), and accumulation mode (100-560 nm) particles, and total particles were 17500, 32000, 4000, and 53500 cm(-3), respectively. Average particle size distribution was monomodal with a mode diameter of about 40 nm at night and bimodal with mode diameters of about 10 and about 40 nm during the daytime. New particle formation events, which were connected to diurnal variation of nucleation mode particles, were observed in more than half of the observation days. The events often started around 10:00-11:00 Chinese Standard Time (CST) and ended up after 3-4 h. Concentrations of Aitken and accumulation mode particles increased from midnight and reached their maxima at about 10:00 CST, and then decreased and became the lowest in the afternoon. Analysis of diurnal cycles in traffic volume and meteorological parameters revealed that the accumulation of the particles in Aitken and accumulation modes in the morning was influenced by formation of an inversion and increase in vehicle emission, and dispersion of such particles in the afternoon was associated with more effective vertical mixing and higher wind speed.

This paper introduced IVE model and presented the method to quantify the main parameters by taking Beijing city as a case. Emissions from different vehicle fleets of Beijing were calculated using IVE model. The results show that emissions factors of buses and trucks were much higher, especially for PM, which were 14 and 44 times those of passenger cars. The daily CO, VOC, NO, and PM emissions of vehicles in Beijing city were 2767.4, 182.5, 353.8 and 7.1 t respectively. Common light duty vehicles were the main emission source of CO and VOC, with the contribution of 42.0% and 34.7% respectively, Trucks were the largest contributor of NO, and PM emissions, with the contribution of 66.3% and 83.0% respectively. The methodology and calculating results of MOBILE6 and IVE model were compared, and advantages of IVE model's application in China were discussed.

Total suspended particulates (TSP) samples were collected from Sep., 2003 to Jul., 2004 in Beijing, and 15 kinds of PAHs, ranging from 3 to 7 rings were analyzed. The maximum concentrations sigma PAHs and BaP were 705 ng/m3 and 52 ng/m3 respectively. Average sigma PAHs concentrations in four seasons were 46 ng/m3, 16 ng/m3, 52 ng/m3 and 268 ng/m3 respectively; and the average BaP concentrations in four seasons were 2.8 ng/m3, 0.23 ng/m3, 3.3 ng/m3, 16 ng/m3 respectively. Regarding to the meteorological parameters, precipitation distinctly lowered the concentration; in heating period, PAHs concentrations fall with the temperature goes up, but there is no obvious relation between concentration and temperature in non-heating period; the increase of wind speed level causes the decrease of PAH concentrations in the heating period, but relation between PAH concentrations and wind speed varied with aromatic rings of PAHs and levels of wind speed in the non-heating period.

Weekly PM2.5 samples were simultaneously collected at a semi-residential (Tsinghua University) and a downtown (Chegongzhuang) site in Beijing from August 2001 through September 2002. The ambient mass concentration and chemical composition of PM2.5 were determined. Analyses including elemental composition, water-soluble ions, and organic and elemental carbon were performed. The annual average concentrations of PM2.5 were 96.5 microg m(-3) and 106.9 microg m(-3) at CGZ and HU site, respectively. More than 80% of the PM2.5 mass concentrations were explained by carbonaceous species, secondary particles, crustal matters and trace elements at the two sites. Carbonaceous species were the most abundant components, constituting about 45% and 48% of the total PM2.5 mass concentrations at CGZ and THU site, respectively. SO4(2-), NO3- and NH4+ were three major ions, accounting for 37%, 23% and 20%, respectively, of the total mass of inorganic water-soluble ions.

To understand the concentration levels and temporal variations of the mineral component of PM2.5 in the ambient air of Beijing, weeklong samples were simultaneously collected for one year at Qinghuayuan and Chegongzhuang. The concentrations of five major crustal elements Al, Si, Ca, Mg, and Fe exhibited similar significant weekly variations, with their maximum values in the week of a serious dust event in the spring of 2000. Obvious seasonal pattern was also found for these elements, indicating different influences on fine mineral particles from the source emissions and meteorology in different seasons. Soil dust concentration increased from a low level in summer to the peak value (21.1 microg x m(-3)) in spring, suggesting that frequent dust events made a significant contribution to fine soil dust. A large number of construction activities in Beijing substantially increased the loading of fine calcium-bearing particles, and their emissions thus need to be further controlled.

Total suspended particulate (TSP) samples were collected during wintertime from November 24, 1998 to February 12, 1999 in Beijing. Ionic species including Cl-, NO3(-), SO4(2-), Na+, NH4(+), K+, Mg2+ and Ca2+ were determined by Ion Chromatography (IC). The sum average concentration of all the determined ions accounted for 18.9% of the TSP concentration, and SO4(2-) appeared the dominant ion with an average concentration of 30.84 microg m(-3); the sum mass concentration of SO4(2-), NO3(-), Ca2+ and NH4(+) accounted for about 83.2% of all the eight ions measured. The study indicated that the chemical form of sulfate and ammonium varies with TSP concentration levels. During heavy pollution periods, the average TSP concentration was 0.66 mg m(-3), and the NH4(+)/SO4(2-) molar ratio was low (0.58). It indicated that sulfate may present as CaSO4 and (NH4)2SO4 x CaSO4 x 2H2O. When TSP concentration (average 0.186 mg m(-3)) was relatively low, the NH4(+)/SO4(2-) molar ratio was 1.94, close to the theoretical ratio of 2 of (NH4)2SO4. Under this condition (NH4)2SO4 is expected to exist as the major form of sulfate. When the TSP concentration level was medium (average 0.35 mg m(-3)), the NH4+/SO4(2-) molar ratio appeared an average value (1.27), (NH4)2SO4, (NH4)2SO4 x CaSO4 x 2H2O and CaSO4 are expected to be present in those aerosol particles. Meteorological conditions including wind speed and wind direction were related to the TSP concentration level.