Estimation of gaseous polycyclic aromatic hydrocarbons (PAHs) and characteristics of atmospheric PAHs at a traffic site in Kanazawa, Japan.

Size-fractionated particulate matter (PM2.5 and PM>2.5) was collected at a traffic site in Kanazawa, Japan in a seasonal sampling work in 2020. Nine polycyclic aromatic hydrocarbons (4- to 6-ring PAHs) were determined in fine and coarse particles. The gas/particle partitioning coefficients (Kp) of the PAHs were calculated from the supercooled liquid vapour pressure and octanol-air partitioning coefficient based on the relationships obtained in previous traffic pollution-related studies. Gaseous PAHs were estimated by Kp and the concentrations of PM and particulate PAHs. The concentrations of total PAHs were 32.5, 320.1 and 5646.2 pg/m3 in the PM>2.5, PM2.5 and gas phases, respectively. Significant seasonal trends in PAHs were observed (particle phase: lowest in summer, gas phase: lowest in spring, particle and gas phase: lowest in spring). Compared to 2019, the total PAH concentrations (in particles) decreased in 2020, especially in spring and summer, which might be due to reduced traffic trips during the COVID-19 outbreak. The incremental lifetime cancer risk (ILCR) calculated from the toxic equivalent concentrations relative to benzo[a]pyrene (BaPeq) was lower than the acceptable limit issued by the US Environmental Protection Agency, indicating a low cancer risk in long-term exposure to current PAH levels. It is notable that gaseous PAHs considerably contributed to BaPeq and ILCR (over 50%), which highlighted the significance of gaseous PAH monitoring for public health protection. This low-cost estimation method for gaseous PAHs can be expected to reliably and conveniently obtain PAH concentrations as a surrogate for traditional sampling in the future work.

Size-resolved gas-particle partitioning of polycyclic aromatic hydrocarbons in a large temperature range of 50 ℃.

Size-resolved gas-particle partitioning of semi-volatile organic compounds (SVOCs) can affect their environmental behaviors and health effects, which has not been widely studied in comparing with the gas-total suspended particle partitioning. Herein, the size-resolved gas-particle partitioning quotient (KPi) of polycyclic aromatic hydrocarbons (PAHs) in a large temperature range (-20.6 â„ƒ ∼ 29.4 â„ƒ) was firstly comprehensively studied. The log KPi values of PAHs related to fine particles were significantly higher than those related to coarse particles. When the logarithm of subcooled liquid-vapor pressure (log PL0) ∈ [-7, -1), the regression slopes of log KPi vs log PL0 related to the particle size > 1.0 µm were shallower than those with the particle size range of 0.10-1.0 µm, which indicated the influence of particle size on KPi. Among the three previous prediction equations of gas-particle partitioning quotient, the empirical equation based on the ambient temperature matched better with the measured log KPi. Therefore, a new prediction equation including ambient temperature and particle size as the two major parameters was established. For most particle size ranges, the new equation showed better prediction performance than the three previous equations. In summary, this study provided new insights for the size-resolved gas-particle partitioning mechanism and quotient.

Species-specific effect of particle viscosity and particle-phase reactions on the formation of secondary organic aerosol.

Secondary organic aerosol (SOA) is a major component of atmospheric fine particulate matter. Both particle viscosity and particle-phase chemistry play a crucial role in the formation and evolution of SOA; however, our understanding on how these two factors together with gas-phase chemistry collectively determine the formation of SOA is still limited. Here we developed a kinetic aerosol multilayer model coupled with gas-phase and particle-phase chemistry to simulate SOA formation. We take the atmospherically important α-pinene + OH oxidation system as an example application of the model. The simulations show that although the particle viscosity has negligible to small influences on the total SOA mass concentration, it strongly changes the concentration and distribution of individual compounds within the particle. This complicated effect of particle viscosity on SOA formation is a combined result of inhibited condensation or evaporation of specific organics due to slowed particle-phase diffusion. Furthermore, the particle-phase reactions alter the volatility and abundance of specific compounds and exacerbate their non-uniform distribution in highly viscous particles. Our results highlight an important species-specific effect of particle viscosity and particle-phase chemistry on SOA formation and demonstrate the capability of our model for quantifying such complicated effects on SOA formation and evolution.

Emission characteristics of lead and particulate matter from lead and zinc smelters in China.

Understanding the emission characteristics of particulate matter and associated heavy metals is essential for assessing their environmental and health impacts post-emission, as well as for identifying potential control technologies for the sources. Here, a field test was conducted at two advanced smelting plants equipped with comprehensive air pollution control devices. The particles emitted from different stages of lead and zinc smelting exhibited bi-modal size distributions, with peaks observed in PM0.1-1.0 and PM2.5-10, respectively. Particulate-bound Pb was identified as the predominant Pb species in the flue gas, primarily originating from ore crushing. Consequently, over 80 % of Pb was emitted in the form of coarse particles, a marked contrast to coal-fired power plants where Pb concentrated on fine particles. High efficiencies in Pb removal were achieved by dust collectors, flue gas purification systems, and acid plants with desulfurization systems, resulting in overall Pb emission factors in lead and zinc smelting were only 89.3 and 2.60 g t-1 (of metal production), respectively. Importantly, the contribution of gas-phase Pb, which accounts for approximately 16.6 % of total emissions, must not be neglected in future emission monitoring and control efforts.

Characterization and health risks of short- and medium-chain chlorinated paraffins in the gas and size-fractionated particulate phases in ambient air.

Short-chain and medium-chain chlorinated paraffins (SCCPs and MCCPs) have garnered significant attention because they have persistence and potential toxicity, and can undergo long-distance transport. Chlorinated paraffins (CPs) inhaled in the size-fractionated particulate phase and gas phase can carry different risks to human health due to their ability to accumulate in different regions of the respiratory tract and exhibit varying deposition efficiencies. In our study, large-volume ambient air samples in both the size-fractionated particulate phase (Dp < 1.0 µm, 1.0-2.5 µm, 2.5-10 µm, and Dp ≥ 10 µm) and gas phase were collected simultaneously in Beijing using an active sampler. The overall levels of SCCPs and MCCPs were relatively high, the ranges being 57-881 and 30-385 ng/m3, respectively. SCCPs tended to be partitioned in the gas phase (on average 75% of the ΣSCCP concentration), while MCCPs tended to be partitioned in the particulate phase (on average 62% of the ΣMCCP concentration). Significant correlations were discovered between the logarithm-transformed gas-particle partition coefficients (KP) and predicted subcooled vapor pressures (PL0) (p < 0.01 for SCCPs and MCCPs) and between the logarithm-transformed KP values and octanol-air partition coefficients (KOA) (p < 0.01 for SCCPs and MCCPs). Thus, the slopes indicated that organic matter absorption was the dominant process involved in gas-particle partitioning. We used the ICRP model to calculate deposition concentrations for particulate-associated CPs in head airways region (15.6-71.4 ng/m³), tracheobronchial region (0.8-4.8 ng/m³), and alveolar region (5.1-21.9 ng/m³), then combined these concentrations with the CP concentrations in the gas phase to calculate estimated daily intakes (EDIs) for inhalation. The EDIs for SCCPs and MCCPs through inhalation of ambient air for the all-ages group were 67.5-184.2 ng/kg/day and 19.7-53.7 ng/kg/day, respectively. The results indicated that SCCPs and MCCPs in ambient air do not currently pose strong risks to human health in the study area.

Role of gas-particle conversion of ammonia in haze pollution under ammonia-rich environment in Northern China and prospects of effective emission reduction.

As an important precursor of secondary inorganic aerosols (SIAs), ammonia (NH3) plays a key role in fine particulate matter (PM2.5) formation. In order to investigate its impacts on haze formation in the North China Plain (NCP) during winter, NH3 concentrations were observed at a high-temporal resolution of 1 min by using the SP-DOAS in Tai'an from December 2021 to February 2022. During the observation period, the average NH3 concentration was 11.84 ± 5.9 ppbv, and it was determined as an ammonia-rich environment during different air quality conditions. Furthermore, the average concentrations of sulfate (SO42-), nitrate (NO3-) and ammonium (NH4+) were 9.54 ± 5.97 µg/m3, 19.09 ± 14.18 µg/m3 and 10.72 ± 6.53 µg/m3, respectively. Under the nitrate-dominated atmospheric environment, aerosol liquid water content (ALWC) was crucial for NH3 particle transformation during haze aggravation, and the gas-particle partitioning of ammonia played an important role in the SIAs formation. The reconstruction of the molecular composition further indicated that ammonium nitrate (NH4NO3) plays a dominant role in the increase of PM2.5 during haze events. Consequently, future efforts to mitigate fine particulate pollution in this region should focus on controlling NH4NO3 levels. In ammonia-rich environments, NO3- formation is more dependent on the concentration of nitric acid (HNO3). The sensitive analysis of TNO3 (HNO3 + NO3-) and NHX (NH3 + NH4+) reduction using the thermodynamic model suggested that the NO3- concentration decreases linearly with the reduction of TNO3. And the concentration of NO3- decreases rapidly only when NHX is reduced by 50-60 %. Reducing NOX emissions is the most effective way to alleviate nitrate pollution in this region.

Evidences for the influence from key chemical structures of per- and polyfluoroalkyl substances on their environmental behaviors.

This study carried out the atmospheric and precipitation observation in Beijing for nearly one year, and firstly simultaneously observed the pollution characteristics of PFASs and their main isomers, focusing on their gas-particle partitioning mechanism and dry and wet deposition characteristics. After deducting PFASs in the aqueous phase of particulate matter, the gas-particle partitioning coefficients (-7.04 to -5.49) were about 3-4 units smaller than before (-2.77 to -1.51), and all were smaller than 0, which indicated that each PFAS and isomer were more distributed in the gas phase. Dry deposition was dominant in the atmospheric deposition of each PFAS and isomer with relative contribution of 66 ± 17%, but the relative contribution of dry deposition was significantly different. It was found that the gas-particle partitioning coefficient can be influenced by key chemical structures such as carbon chain length, functional group type, and isomer structure. Furthermore, the gas-particle partitioning can influence the dry and wet deposition of PFASs. Specifically, PFASs with longer carbon chains, carboxylic acid functional group (compared to sulfonic acid functional group) or PFOA branched chain structures had larger gas-particle partitioning coefficients and can be more distributed in the hydrophobic phase of particulate matter, and their relative contributions of dry deposition were smaller.

Enhanced Light Absorption and Elevated Viscosity of Atmospheric Brown Carbon through Evaporation of Volatile Components.

Samples of brown carbon (BrC) material were collected from smoke emissions originating from wood pyrolysis experiments, serving as a proxy for BrC representative of biomass burning emissions. The acquired samples, referred to as "pyrolysis oil (PO1)," underwent subsequent processing by thermal evaporation of their volatile compounds, resulting in a set of three additional samples with volume reduction factors of 1.33, 2, and 3, denoted as PO1.33, PO2, and PO3. The chemical compositions of these POx samples and their BrC chromophore features were analyzed using a high-performance liquid chromatography instrument coupled with a photodiode array detector and a high-resolution mass spectrometer. The investigation revealed a noteworthy twofold enhancement of BrC light absorption observed for the progression of PO1 to PO3 samples, assessed across the spectral range of 300-500 nm. Concurrently, a decrease in the absorption Ångstrom exponent (AAE) from 11 to 7 was observed, indicating a weaker spectral dependence. The relative enhancement of BrC absorption at longer wavelengths was more significant, as exemplified by the increased mass absorption coefficient (MAC) measured at 405 nm from 0.1 to 0.5 m2/g. Molecular characterization further supports this darkening trend, manifesting as a depletion of small oxygenated, less absorbing monoaromatic compounds and the retention of relatively large, less polar, more absorbing constituents. Noteworthy alterations of the PO1 to PO3 mixtures included a reduction in the saturation vapor pressure of their components and an increase in viscosity. These changes were quantified by the mean values shifting from approximately 1.8 × 103 µg/m3 to 2.3 µg/m3 and from ∼103 Pa·s to ∼106 Pa·s, respectively. These results provide quantitative insights into the extent of BrC aerosol darkening during atmospheric aging through nonreactive evaporation. This new understanding will inform the refinement of atmospheric and chemical transport models.

Potential toxic components in size-resolved particles and gas from residential combustion: Emission factor and health risk.

Particulate matter (PM) from residential combustion is an existential threat to human health. Emission factors (EFs) of multiple potential toxic components (PTCs) in size-resolved PM and gas from eight residential fuel combustion were measured, and size distribution, gas/particle partitioning and health risks of the PTCs were investigated. Average EFs from clean coal and anthracite coal were PTEs (sum of EFs of 11 Potential Toxic Elements, 6.62 mg/kg fuels) > PAHs (sum of 22 Polycyclic Aromatic Hydrocarbons, 1.12 mg/kg) > OPAHs (sum of 5 Oxygenated Polycyclic Aromatic Hydrocarbons, 0.45 mg/kg) > PAEs (sum of 6 Phthalate Esters, 0.11 mg/kg) > NPAHs (sum of 14 Nitropolycyclic Aromatic Hydrocarbons, 16.84 µg/kg) > OPEs (sum of 7 Organophosphate Esters, 7.57 µg/kg) > PCBs (sum of 6 Polychorinated Biphenyls, 0.07 µg/kg), which were 2-3 and 1-2 orders of magnitude lower than the EFs of PTCs (except PTEs) from bituminous coal and biomass. Most PAHs, OPAHs and NPAHs, which may mainly originate from chemical reactions, showed similar size distributions and averagely 85 % concentrated in PM1. PTEs, PAEs, OPEs and PCBs generated from the release from raw fuels may have a higher proportion, so their size distributions were more complex and varied with combustion temperature, volatility of compounds, binding mode of the raw fuels, and so on. In addition, clean coal and high-quality anthracite coal could reduce the health risks from the potential organic toxic components, but also reveal the stumbling block of PTEs in risk control.

Four Years of Active Sampling and Measurement of Atmospheric Polycyclic Aromatic Hydrocarbons and Oxygenated Polycyclic Aromatic Hydrocarbons in Dronning Maud Land, East Antarctica.

Antarctica, protected by its strong polar vortex and sheer distance from anthropogenic activity, was always thought of as pristine. However, as more data on the occurrence of persistent organic pollutants on Antarctica emerge, the question arises of how fast the long-range atmospheric transport takes place. Therefore, polycyclic aromatic hydrocarbons (PAHs) and oxygenated (oxy-)PAHs were sampled from the atmosphere and measured during 4 austral summers from 2017 to 2021 at the Princess Elisabeth station in East Antarctica. The location is suited for this research as it is isolated from other stations and activities, and the local pollution of the station itself is limited. A high-volume sampler was used to collect the gas and particle phase (PM10) separately. Fifteen PAHs and 12 oxy-PAHs were quantified, and concentrations ranging between 6.34 and 131 pg m3 (Σ15PAHs-excluding naphthalene) and between 18.8 and 114 pg m3 (Σ13oxy-PAHs) were found. Phenanthrene, pyrene, and fluoranthene were the most abundant PAHs. The gas-particle partitioning coefficient log(Kp) was determined for 6 compounds and was found to lie between 0.5 and -2.5. Positive matrix factorization modeling was applied to the data set to determine the contribution of different sources to the observed concentrations. A 6-factor model proved a good fit to the data set and showed strong variations in the contribution of different air masses. During the sampling campaign, a number of volcanic eruptions occurred in the southern hemisphere from which the emission plume was detected. The FLEXPART dispersion model was used to confirm that the recorded signal is indeed influenced by volcanic eruptions. The data was used to derive a transport time of between 11 and 33 days from release to arrival at the measurement site on Antarctica.

[Characteristics of Secondary Inorganic Ions in PM2.5 and Its Influencing Factors in Summer in Zhengzhou].

Nitrate (NO3-), sulfate (SO42-), and ammonium (NH4+) are important components of PM2.5, and studying their characteristics and influencing factors is essential for the continuous improvement of air quality. A series of online instruments were used to analyze the chemical components of PM2.5 in Zhengzhou in the summer of 2020. The results showed that the average ρ(PM2.5) was (28 ±13) µg·m-3, showing a daily variation characteristic of high at night and low during the day. The main concentrations of NO3-, SO42-, and NH4+ were (7.8 ±6.7), (7.2 ±3.7), and (5.5 ±3.1) µg·m-3, accounting for 22%, 21%, and 16% in PM2.5, respectively. The proportions of NO3- (27%) and SO42- (23%) in PM2.5, respectively, increased with the increase in PM2.5 and O3 concentration. In addition, the proportions of NO3- and NH4+ increased under low wind speed, high humidity, low temperature, and rainfall conditions. Moreover, the proportion of NO3- showed a daily variation characteristic of high at night and low during the day, whereas the opposite was true for SO42-. The gas-particle partitioning process of NH4NO3 was the main factor affecting the concentrations of NO3- and NH4+ in PM2.5. Low temperature, high humidity, and high aerosol water content concentrations favored the partitioning of HNO3 and NH3 to the particulate phase. High pH also favored the partitioning of gas-phase HNO3 to NO3-; however, it was not conducive to the partition of NH3 to NH4+. These trends partially explained the increase in the concentration and proportion of NO3- in PM2.5 under different scenarios.

Sources of the Elevating Polycyclic Aromatic Hydrocarbon Pollution in the Western South China Sea and Its Environmental Implications.

The environmental implications of polycyclic aromatic hydrocarbons (PAHs) caused by the vigorous development of offshore oil exploitation and shipping on the marine ecosystem are unclear. In this study, the PAH concentrations were systematically characterized in multiple environmental media (i.e., atmosphere, rainwater, seawater, and deep-sea sediments) in the western South China Sea (WSCS) for the first time to determine whether PAH pollution increased. The average ∑15PAHs (total concentration of 15 US EPA priority controlled PAHs excluding naphthalene) in the water of WSCS has increased and is higher than the majority of the oceans worldwide due to the synergistic influence of offshore oil extraction, shipping, and river input. The systematic model comparison confirms that the Ksoot-air model can more accurately reflect the gas-particle partitioning of PAHs in the atmosphere of the WSCS. We also found that the vertical migration of the elevating PAHs is accelerated by particulate matter, driving the migration of atmospheric PAHs to the ocean through dry and wet deposition, with 16% being contributed by the particle phase. The particulate matter sinking alters the PAH distribution in the water column and generates variation in source apportionment, while the contribution of PAHs loaded on them (>20%) to the total PAH reserves cannot be ignored as before. Hence, the ecological threat of PAHs increases by the oil drilling and shipping industry, and the driving force of particulate matter deserves continuous attention.

Gas-particle partitioning of organophosphate esters in indoor and outdoor air and its implications for individual exposure.

The extensive utilization of organophosphate esters (OPEs) has resulted in their widespread presence in the environment, raising concerns about potential human health risks. In this study, 13 OPEs were analyzed in both gas and particle phases as well as in indoor and outdoor atmospheric environments. Moreover, human exposure to OPEs were investigated within a university environment, focusing on forehead contact and individual PM2.5 inhalation. The results showed similar distribution patterns of OPEs indoors and outdoors, although higher concentrations were found indoors. The average atmospheric concentration of ∑OPEs (combining particle and gaseous OPEs) was 1575 pg/m3 in the outdoor environment and 6574 pg/m3 ∑OPEs in the indoor microenvironments. The overwhelming majority of OPEs exhibit a pronounced propensity to adsorb onto PM2.5 particles. Notably, the concentration of OPEs on the forehead differed significantly from that in the atmospheric environment, whereas individual PM2.5 exposure was consistent with the concentration of indoor PM2.5. Intriguingly, some OPEs with high octanol-water partition coefficient (log Kow) were not detected in the environment but found on human foreheads. Gas-particle partitioning was predicted using the Harner-Bidleman and Li-Ma-Yang models and the results were in agreement with the monitoring data for approximately half of the OPE monomers. Correlations between OPEs exposure and gas-particle partitioning were found to be more significant for novel OPEs. No non-cancer risk to humans through individual exposure to OPEs was identified via forehead exposure or inhalation. The previously unreported relationship between individual exposure and the environmental occurrence of traditional and novel OPEs demonstrated in this study highlights the importance of evaluating the potential health risks associated with actual OPE exposure.

Impact of pH on Gas-Particle Partitioning of Semi-Volatile Organics in Multicomponent Aerosol.

The partitioning of semivolatile organic compounds (SVOCs) between the condensed and gas phases can have significant implications for the properties of aerosol particles. In addition to affecting size and composition, this partitioning can alter radiative properties and impact cloud activation processes. We present measurements and model predictions on how activity and pH influence the evaporation of SVOCs from particles to the gas phase, specifically investigating aqueous inorganic particles containing dicarboxylic acids (DCAs). The aerosols are studied at the single-particle level by using optical trapping and cavity-enhanced Raman spectroscopy. Optical resonances in the spectra enable precise size tracking, while vibrational bands allow real-time monitoring of pH. Results are compared to a Maxwell-type model that accounts for volatile and nonvolatile solutes in aqueous droplets that are held at a constant relative humidity. The aerosol inorganic-organic mixture functional group activity coefficients thermodynamic model and Debye-Hückel theory are both used to calculate the activities of the species present in the droplet. For DCAs, we find that the evaporation rate is highly sensitive to the particle pH. For acidity changes of approximately 1.5 pH units, we observe a shift from a volatile system to one that is completely nonvolatile. We also observe that the pH itself is not constant during evaporation; it increases as DCAs evaporate, slowing the rate of evaporation until it eventually ceases. Whether a DCA evaporates or remains a stable component of the droplet is determined by the difference between the lowest pKa of the DCA and the pH of the droplet.

Cross-regional scale studies of organochlorine pesticides in air in China: Pollution characteristic, seasonal variation, and gas/particle partitioning.

Few simultaneous studies of organochlorine pesticides (OCPs) in the atmosphere have been conducted across Southeast and Northeast China, and no data on the gas/particle (G/P) partitioning behaviors of several current-use OCPs are available. In this study, a one-year synchronous monitoring program was conducted for OCPs in Chinese atmosphere spanning 30° latitude and 60 °C temperature. A total of 111 pairs of gas and particle samples were collected from Mohe and Harbin in Northeast China and from Shenzhen in Southeast China. The detection frequency for 66.7 % of the OCPs exceeded 80 %, indicating their prevalence in the atmosphere. The concentrations of individual OCPs spanned six orders of magnitude, indicating different pollution levels. Highest levels of hexachlorobenzene were observed at all sites. Banned OCPs were found predominantly in secondary distribution patterns, whereas current-use OCPs were dominated by primary distribution patterns. In Harbin and Mohe, the concentrations of OCPs were highest in summer, followed by autumn and winter. No obvious seasonal variation was observed in Shenzhen associated with different cultivation types. At all three sites, OCPs were predominantly found in the gas phase, and higher percentages of particle-phase OCPs were observed in Harbin and Mohe than in Shenzhen. In this study, G/P partitioning models were used to study the G/P partitioning mechanism of OCPs. The Li-Ma-Yang model provided the most accurate prediction of the G/P partitioning behavior of OCPs with high molecular weights and low vapor pressures, particularly at low temperatures. However, OCPs with lower molecular weights and higher vapor pressures were predominantly in the equilibrium state, for which the Junge-Pankow model was suitable. This systematic cross-scale study provides new insights into pollution, G/P partitioning, and the environmental behavior of OCPs in the atmosphere.

Atmospheric mercury in a developed region of eastern China: Interannual variation and gas-particle partitioning.

Atmospheric mercury plays a crucial role in the biogeochemical cycle of mercury. This study conducted an intensive measurement of atmospheric mercury from 2015 to 2018 at a regional site in eastern China. During this period, the concentration of particle-bound mercury (PBM) decreased by 13%, which was much lower than those of gaseous elemenral mercury (GEM, 30%) and reactive gaseous mercury (GOM, 62%). The gradual decrease in the correlation between PBM and CO, K, and Pb indicates that the influence of primary emissions on PBM concentration was weakening. Moreover, the value of the partitioning coefficient (Kp) increased gradually from 0.05 ± 0.076 m3/µg in 2015 to 0.16 ± 0.37 m3/µg in 2018, indicating that GOM was increasingly inclined to adsorb onto particulate matter. Excluding the influence of meteorological conditions and the primary emissions, the change in aerosol composition is designated as the main trigger factor for the increasing gas-particle partitioning of reactive mercury (RM). The increasing ratio of Cl-, NO3-, and organics (Org) in the chemical composition of particle matters (PM2.5), as well as the decrease in the proportion of SO42-, NH4+, and K+, are conducive to the adsorption of GOM onto particles, forming PBM, which led to an increase of Kp and a lag of PBM reduction compared to GEM and GOM under the continuous control measures of anthropogenic mercury emissions. The evolution of aerosol compositions in recent years affects the migration and transformation of atmospheric mercury, which in turn can affect the biogeochemical cycle of mercury.

Atmospheric occurrences and health risk assessment of polycyclic aromatic hydrocarbons and their derivatives in a typical coking facility and surrounding areas.

Coking facilities release large quantities of polycyclic aromatic hydrocarbons (PAHs) and their derivatives into the ambient air. Here we examined the profiles, spatial distributions, and potential sources of atmospheric PAHs and their derivatives in an industrial coking plant and its surrounding environment (gaseous and particulate). The mean concentrations of PAHs, nitrated PAHs (NPAHs), chlorinated PAHs (ClPAHs), and brominated PAHs (BrPAHs) in the air of the coking facility were 923, 23.8, 16.7 and 4.25 ng m-³, respectively, 1-2 orders of magnitude higher than those in the surrounding area and the control area. Linear regressions between contaminant concentrations and distance from the coking facility suggested that the concentrations of PAHs (r2 = 0.82, p < 0.05), NPAHs (r2 = 0.77, p < 0.01), and BrPAHs (r2 = 0.62, p < 0.01) were negatively correlated with distance. Additionally, the particle-bound fractions of PAHs and their derivatives were significantly correlated with their molecular weights (p < 0.01). Based on the calculation of the gas/particle partitioning coefficients (log KP) for PAHs and their derivatives and the corresponding subcooled liquid vapor pressures (log PL), the slope values for PAHs, NPAHs, ClPAHs, and BrPAHs ranged from -1 to -0.6, indicating that deposition of PAHs and their derivatives occurred through both adsorption and absorption. Five emissions sources were identified by positive matrix factorization (PMF), including coking emissions, oil pollution, industrial and combustion sources, secondary formation, and traffic emissions, with coking emissions accounting for more than 50% of total emissions. Furthermore, the results of the health risks assessment suggested that atmospheric PAHs and their derivatives in the coke plant and surrounding area negatively impacted human health.

Comparison of Gas-Particle Partitioning of Glyoxal and Methylglyoxal in the Summertime Atmosphere at the Foot and Top of Mount Hua.

Glyoxal and methylglyoxal are important volatile organic compounds in the atmosphere. The gas-particle partitioning of these carbonyl compounds makes significant contributions to O3 formation. In this study, both the gas- and particle-phase glyoxal and methylglyoxal concentrations at the foot and top of Mount Hua were determined simultaneously. The results showed that the gaseous-phase glyoxal and methylglyoxal concentrations at the top were higher than those at the foot of the mountain. However, the concentrations for the particle phase showed the opposite trend. The average theoretical values of the gas-particle partitioning coefficients of the glyoxal and methylglyoxal concentrations (4.57 × 10-10 and 9.63 × 10-10 m3 µg-1, respectively) were lower than the observed values (3.79 × 10-3 and 6.79 × 10-3 m3 µg-1, respectively). The effective Henry's law constants (eff.KH) of the glyoxal and methylglyoxal were in the order of 108 to 109 mol/kgH2O/atm, and they were lower at the foot than they were at the top. The particle/gas ratios (P/G ratios) of the glyoxal and methylglyoxal were 0.039 and 0.055, respectively, indicating more glyoxal and methylglyoxal existed in the gas phase. The factors influencing the partitioning coefficients of the glyoxal and methylglyoxal were positively correlated with the relative humidity (RH) and negatively correlated with the PM2.5 value. Moreover, the partitioning coefficient of the glyoxal and methylglyoxal was more significant at the top than at the foot of Mount Hua.

Atmospheric phthalate esters in a multi-function area of Hangzhou: Temporal variation, gas/particle phase distribution, and population exposure risk.

Phthalate esters (PAEs) are prevalent in both indoor and outdoor environments. However, there are relatively few studies on phthalate contamination in the air of multi-function areas. Experiments were conducted to analyze the concentrations of 14 distinct PAEs in outdoor air in the college town of Hangzhou throughout both the warm and cold seasons. Correlation and principal component analyses were performed to investigate the influence and source factors of PAEs. This study also focused on the relationship between the gas/particle partition coefficient Kp and temperature, as well as the application of the gas/particle partition model. The risk of exposure to PAEs via inhalation was predicted for four groups of the general population: toddlers, adolescents, adults, and older adults. The results indicated that the concentration levels of Σ14PAEs in outdoor air were 1573 ng/m3 in the gaseous phase and 126 ng/m3 in the particulate phase. Additionally, this study indicated three primary sources of PAEs: indoor diffuse sources, industrial emission sources, and building construction sources. The gas/particle partitioning of PAEs also revealed that low-molecular-weight PAEs are more prevalent in gas, whereas high-molecular-weight PAEs are more predominant in the particle phase. A health risk analysis revealed high estimations of daily intakes (EDI) for toddlers and adolescents and high lifetime average daily doses (LADD) for older adults. This study establishes a solid foundation for formulating scientific and effective air pollution control measures by analyzing the characteristics and assessing the health risks of PAEs.

Emission and gas-particle partitioning characteristics of atmospheric halogenated and organophosphorus flame retardants in decabromodiphenyl ethane-manufacturing functional areas.

The emission and gas-particle partitioning characteristics in various functional areas of production lines are still unknown. However, flame-retardant manufacturing activities are the primary emission source of flame retardants. Thus, fine particles and gases were investigated in three functional areas of a decabromodiphenyl ethane production line, i.e., polybrominated diphenyl ethers (PBDEs), novel brominated flame retardants (NBFRs), dechlorane plus (DPs), and organophosphorus flame retardants (OPFRs) in a flame-retardant manufacturing factory. High levels of PBDEs (8.02 × 103-4.16 × 104 pg/m3), NBFRs (6.05 × 103-1.92 × 105 pg/m3), and DPs (89.5-5.20 × 103 pg/m3) were found in various functional areas, suggesting manufacturing activities were a primary emission source. In contrast, OPFRs were derived from long-range transport or other non-industrial sources. Varied concentrations of PBDEs, NBFRs, and DPs were observed in different production lines, higher in the reaction zone area than others. As the predominant compounds, decabromodiphenyl ether, decabromodiphenyl ethane, syn-DP, and tris(chloropropyl) phosphate accounted for 54.7%, 89.3%, 93.4%, and 34.7% of PBDEs, NBFRs, DPs, and OPFRs, respectively. Three models were used to predict the gas-particle partitioning of the halogenated flame retardants emitted from manufacturing activities. The Li-Jia Empirical Model predicted the gas-particle partitioning behavior well. This research shows that the adsorption-desorption process of the halogenated flame retardants between the gaseous and particulate phases did not reach equilibrium.