Insights into air pollution chemistry and sulphate formation from nitrous acid (HONO) measurements during haze events in Beijing.

Wintertime urban air pollution in many global megacities is characterised by episodic rapid increase in particulate matter concentrations associated with elevated relative humidity - so-called haze episodes, which have become characteristic of cities such as Beijing. Atmospheric chemistry within haze combines gas- and condensed-phase chemical processes, leading to the growth in secondary species such as sulphate aerosols. Here, we integrate observations of reactive gas phase species (HONO, OH, NOx) and time-resolved aerosol composition, to explore observational constraints on the mechanisms responsible for sulphate growth during the onset of haze events. We show that HONO abundance is dominated by established fast gas-phase photochemistry, but the consideration of the additional formation potentially associated with condensed-phase oxidation of S species by aqueous NO2 leading to NO2- production and hence HONO release, improves agreement between observed and calculated gas-phase HONO levels. This conclusion is highly dependent upon aerosol pH, ionic strength and particularly the parameterisation employed for S(iv) oxidation kinetics, for which an upper limit is derived.

An evaluation of source apportionment of fine OC and PM2.5 by multiple methods: APHH-Beijing campaigns as a case study.

This study aims to critically evaluate the source apportionment of fine particles by multiple receptor modelling approaches, including carbon mass balance modelling of filter-based radiocarbon (14C) data, Chemical Mass Balance (CMB) and Positive Matrix Factorization (PMF) analysis on filter-based chemical speciation data, and PMF analysis on Aerosol Mass Spectrometer (AMS-PMF) or Aerosol Chemical Speciation Monitor (ACSM-PMF) data. These data were collected as part of the APHH-Beijing (Atmospheric Pollution and Human Health in a Chinese Megacity) field observation campaigns from 10th November to 12th December in winter 2016 and from 22nd May to 24th June in summer 2017. 14C analysis revealed the predominant contribution of fossil fuel combustion to carbonaceous aerosols in winter compared with non-fossil fuel sources, which is supported by the results from other methods. An extended Gelencsér (EG) method incorporating 14C data, as well as the CMB and AMS/ACSM-PMF methods, generated a consistent source apportionment for fossil fuel related primary organic carbon. Coal combustion, traffic and biomass burning POC were comparable for CMB and AMS/ACSM-PMF. There are uncertainties in the EG method when estimating biomass burning and cooking OC. The POC from cooking estimated by different methods was poorly correlated, suggesting a large uncertainty when differentiating this source type. The PM2.5 source apportionment results varied between different methods. Through a comparison and correlation analysis of CMB, PMF and AMS/ACSM-PMF, the CMB method appears to give the most complete and representative source apportionment of Beijing aerosols. Based upon the CMB results, fine aerosols in Beijing were mainly secondary inorganic ion formation, secondary organic aerosol formation, primary coal combustion and from biomass burning emissions.

Characteristics and source attribution of PM2.5 during 2016 G20 Summit in Hangzhou: Efficacy of radical measures to reduce source emissions.

A field campaign was conducted to study the PM2.5 and atmospheric gases and aerosol's components to evaluate the efficacy of radical measures implemented by the Chinese government to improve air quality during the 2016 G20 Summit in Hangzhou China. The lower level of PM2.5 (32.48 ± 11.03 µg/m3) observed during the control period compared to pre-control and post-control periods showed that PM2.5 was alleviated by control policies. Based on the mass concentrations of particulate components, the emissions of PM2.5 from local sources including fossil fuel, coal combustion, industry and construction were effectively reduced, but non-exhaust emission was not reduced as effectively as expected. The accumulation of SNA (SO42-, NO3-, NH4+) was observed during the control period, due to the favourable synoptic weather conditions for photochemical reactions and heterogeneous hydrolysis. Because of transboundary transport during the control period, air masses from remote areas contributed significantly to local PM2.5. Although, secondary organic carbon (OCsec) exhibited more sensitivity than primary organic carbon (OCpri) to control measures, and the increased nitrogen oxidation ratio (NOR) implied the regional transport of aged secondary aerosols to the study area. Overall, the results from various approaches revealed that local pollution sources were kept under control, indicating that the implementation of mitigation measures were helpful in improving the air quality of Hangzhou during G20 summit. To reduce ambient levels of PM2.5 further in Hangzhou, regional control policies may have to be taken so as to reduce the impact of long-range transport of air masses from inland China.

Comparison of physical and chemical properties of ambient aerosols during the 2009 haze and non-haze periods in Southeast Asia.

Recurrent smoke-haze episodes that occur in Southeast Asia (SEA) are of much concern because of their environmental and health impacts. These haze episodes are mainly caused by uncontrolled biomass and peat burning in Indonesia. Airborne particulate matter (PM) samples were collected in the southwest coast of Singapore from 16 August to 9 November in 2009 to assess the impact of smoke-haze episodes on the air quality due to the long-range transport of biomass and peat burning emissions. The physical and chemical characteristics of PM were investigated during pre-haze, smoke-haze, and post-haze periods. Days with PM2.5 mass concentrations of ≥35 µg m(-3) were considered as smoke-haze events. Using this criterion, out of the total 82 sampling days, nine smoke-haze events were identified. The origin of air masses during smoke-haze episodes was studied on the basis of HYSPLIT backward air trajectory analysis for 4 days. In terms of the physical properties of PM, higher particle surface area concentrations and particle gravimetric mass concentrations were observed during the smoke-haze period, but there was no consistent pattern for particle number concentrations during the haze period as compared to the non-haze period except that there was a significant increase at about 08:00, which could be attributed to the entrainment of PM from aloft after the breakdown of the nocturnal inversion layer. As for the chemical characteristics of PM, among the six key inorganic water-soluble ions (Cl(-), NO3(-), nss-SO4(2-), Na(+), NH4(+), and nss-K(+)) measured in this study, NO3(-), nss-SO4(2-), and NH4(+) showed a significant increase in their concentrations during the smoke-haze period together with nss-K(+). These observations suggest that the increased atmospheric loading of PM with higher surface area and increased concentrations of optically active secondary inorganic aerosols [(NH4)2SO4 or NH4HSO4 and NH4NO3] resulted in the atmospheric visibility reduction in SEA due to the advection of biomass and peat burning emissions.

Could wastewater analysis be a useful tool for China? - A review.

Analysing wastewater samples is an innovative approach that overcomes many limitations of traditional surveys to identify and measure a range of chemicals that were consumed by or exposed to people living in a sewer catchment area. First conceptualised in 2001, much progress has been made to make wastewater analysis (WWA) a reliable and robust tool for measuring chemical consumption and/or exposure. At the moment, the most popular application of WWA, sometimes referred as sewage epidemiology, is to monitor the consumption of illicit drugs in communities around the globe, including China. The approach has been largely adopted by law enforcement agencies as a device to monitor the temporal and geographical patterns of drug consumption. In the future, the methodology can be extended to other chemicals including biomarkers of population health (e.g. environmental or oxidative stress biomarkers, lifestyle indicators or medications that are taken by different demographic groups) and pollutants that people are exposed to (e.g. polycyclic aromatic hydrocarbons, perfluorinated chemicals, and toxic pesticides). The extension of WWA to a huge range of chemicals may give rise to a field called sewage chemical-information mining (SCIM) with unexplored potentials. China has many densely populated cities with thousands of sewage treatment plants which are favourable for applying WWA/SCIM in order to help relevant authorities gather information about illicit drug consumption and population health status. However, there are some prerequisites and uncertainties of the methodology that should be addressed for SCIM to reach its full potential in China.

Assessing the particulate matter emission reduction characteristics of small turbofan engine fueled with 100 % HEFA sustainable aviation fuel.

With the continuous increase in global air transportation, the impact of ultrafine particulate matter (PM) emissions from aviation on human health and environmental pollution is becoming increasingly severe. In addition to carbon reduction throughout the lifecycle, Sustainable Aviation Fuels (SAF) also represent a significant pathway for reducing PM emissions. However, due to issues such as airworthiness safety and adaptability, existing research has mostly focused on the emission performance of SAF when blended with traditional fuels at <50 %, leaving the emission characteristics of higher blending ratios to be explored. In this study, using measurement methods recommended by the International Civil Aviation Organization (ICAO), the PM emission reduction characteristics of small turbofan engines fueled with 100 % Hydroprocessed Esters and Fatty Acids (HEFA)-SAF were experimentally evaluated and compared with traditional fuels RP-3 and Diesel, while avoiding the interference of lubricant blending combustion. The results showed that the peak number concentration of particle size distribution (PSD), PM total number, as well as the number and mass concentration of non-volatile particulate matter (nvPM) decreased initially and then increased with rising thrust conditions. HEFA-SAF exhibits PSD with smaller diameters, and the Geometric Mean Diameter (GMD) ranges from 7.7 nm to 20.3 nm under all conditions. Both volatile particulates (vPM) and nvPM from HEFA-SAF are significantly reduced, with nvPM number emission index (EIn) being 92 % and 71 % lower than Diesel and RP-3, respectively. The nvPM mass emission index (EIm) also shows reductions of 96 % and 89 % compared to Diesel and RP-3. Microscopic characterization also indicated that using HEFA-SAF emitted fewer and smaller PMs. This study establishes a foundation for evaluating the effectiveness of 100 % SAF in reducing PM emissions within the aviation sector, and contributes to the airworthiness regulations development related to the use of SAF in a variety of application environments, alongside enhancing environmental protection measures.

Fine Structure in Isotopic Peak Distributions Measured Using Fourier Transform Ion Cyclotron Resonance Mass Spectrometry: A Comparison between an Infinity ICR Cell and a Dynamically Harmonized ICR Cell.

The fine structure of isotopic peak distributions of glutathione in mass spectra is measured using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) at 12 and 15 T magnetic field, with an infinity cell and a dynamically harmonized cell (DHC) respectively. The resolved peaks in the fine structure of glutathione consist of 2H, 13C, 15N, 17O, 18O, 33S, 34S, 36S, and combinations of them. The positions of the measured fine structure peaks agree with the simulated isotopic distributions with the mass error less than 250 ppb in broadband mode for the infinity cell and no more than 125 ppb with the DHC after internal calibration. The 15 T FT-ICR MS with DHC cell also resolved around 30 isotopic peaks in broadband with a resolving power (RP) of 2 M. In narrowband (m/z 307-313), our current highest RP of 13.9 M in magnitude mode was observed with a 36 s transient length by the 15 T FT-ICR MS with the DHC and 2ω detection on the 15 T offers slightly higher RP (14.8 M) in only 18 s. For the 12 T FT-ICR MS with the infinity cell, the highest RP achieved was 15.6 M in magnitude mode with a transient length of 45 s. Peak decay was observed for low abundance peaks, which could be due to the suppression effects from the most abundant peak, as result of ion cloud Coulombic interactions (space-charge).

PM2.5-bound silicon-containing secondary organic aerosols (Si-SOA) in Beijing ambient air.

Volatile methyl siloxanes (VMS) have been widely used in personal care products and industrial applications, and are an important component of VOCs (volatile organic compounds) indoors. They have sufficiently long lifetimes to undergo long-range transport and to form secondary aerosols through atmospheric oxidation. To investigate these silicon-containing secondary organic aerosols (Si-SOA), we collected PM2.5 samples during 8th-21st August 2018 (summer) and 3rd-23rd January 2019 (winter) at an urban site of Beijing. As the oxidation of VMS mainly results in hydrophilic polar semi-volatile and non-volatile oxidation products, the differences between total water-soluble Si and total water-soluble inorganic Si were used to estimate water-soluble organic Si, considered to be secondary organic Si (SO-Si). The average concentrations of SO-Si during the summer and winter campaigns were 4.6 ± 3.7 and 13.2 ± 8.6 ng m-3, accounting for approximately 80.1 ± 10.1% and 80.2 ± 8.7% of the total water-soluble Si, and 1.2 ± 1.2% and 5.0 ± 6.9% of total Si in PM2.5, respectively. The estimated Si-SOA concentrations were 12.7 ± 10.2 ng m-3 and 36.6 ± 23.9 ng m-3 on average in summer and winter, which accounted for 0.06 ± 0.07% and 0.16 ± 0.22% of PM2.5 mass, but increased to 0.26% and 0.92% on certain days. We found that net solar radiation is positively correlated with SO-Si levels in the summer but not in winter, suggesting seasonally different formation mechanisms.

Size-resolved source apportionment of particulate matter from a megacity in northern China based on one-year measurement of inorganic and organic components.

This research apportioned size-resolved particulate matter (PM) contributions in a megacity in northern China based on a full year of measurements of both inorganic and organic markers. Ions, elements, carbon fractions, n-alkanes, polycyclic aromatic hydrocarbons (PAHs), hopanes and steranes in 9 p.m. size fractions were analyzed. High molecular weight PAHs concentrated in fine PM, while most other organic compounds showed two peaks. Both two-way and three-way receptor models were used for source apportionment of PM in different size ranges. The three-way receptor model gave a clearer separation of factors than the two-way model, because it uses a combination of chemical composition and size distributions, so that factors with similar composition but distinct size distributions (like more mature and less mature coal combustion) can be resolved. The three-way model resolved six primary and three secondary factors. Gasoline vehicles and coal and biomass combustion, nitrate and high relative humidity related secondary aerosol, and resuspended dust and diesel vehicles (exhaust and non-exhaust) are the top two contributors to pseudo-ultrafine (<0.43 µm), fine (0.43-2.1 µm) and coarse mode (>2.1 µm) PM, respectively. Mass concentration of PM from coal and biomass combustion, industrial emissions, and diesel vehicle sources showed a bimodal size distribution, but gasoline vehicles and resuspended dust exhibited a peak in the fine and coarse mode, separately. Mass concentration of sulphate, nitrate and secondary organic aerosol exhibited a bimodal distribution and were correlated with temperature, indicating strong photochemical processing and repartitioning. High relative humidity related secondary aerosol was strongly associated with size shifts of PM, NO3- and SO42- from the usual 0.43-0.65 µm to 1.1-2.1 µm. Our results demonstrated the dominance of primary combustion sources in the <0.43 µm particle mass, in contrast to that of secondary aerosol in fine particle mass, and dust in coarse particle mass in the Northern China megacity.

Characteristics, sources, and health risks of PM2.5-bound trace elements in representative areas of Northern Zhejiang Province, China.

This study aimed to characterize PM2.5-bound trace elements in Northern Zhejiang Province (NZP), one of the most economically prosperous regions in China, and assess the associated health risks for the general populations. A year-long sampling campaign was conducted at four sites representative of urban, suburban, and rural areas of NZP. The average of the sum of twenty trace elements in PM2.5 was 2.8 ± 0.4 µg m-3, dominated by K, Al, Fe, Mg, Zn, and V (>100 ng m-3). The highest total elements' concentration occurred in winter, followed by autumn, spring, and summer. Enrichment factors and principal component analysis (PCA) revealed that the major sources of trace elements in NZP were fossil fuel combustion, biomass burning, crustal dust, traffic, and industrial emissions. Elevated concentrations of certain elements reflected featured sources in different areas, e.g., V and Ni from heavy oil combustion in the port city, and Cu, Fe and Ba from traffic emissions in urban areas. Arsenic (As) represented the major non-cancer risk driver as its hazard quotient was 8.7. The cumulative cancer risk from all the carcinogenic elements was 1.7 × 10-3 in NZP, exceeding the upper limit (10-4) of the acceptable risk range. As and Cr contributed 33% and 66%, respectively, and thus were regarded as cancer risk drivers. The high health risks from PM2.5-bound elements warrant future actions to control their emissions in this region. Priorities should target industrial operations and coal combustion emissions, as informed by the risk drivers.

Abrupt but smaller than expected changes in surface air quality attributable to COVID-19 lockdowns.

The COVID-19 lockdowns led to major reductions in air pollutant emissions. Here, we quantitatively evaluate changes in ambient NO2, O3, and PM2.5 concentrations arising from these emission changes in 11 cities globally by applying a deweathering machine learning technique. Sudden decreases in deweathered NO2 concentrations and increases in O3 were observed in almost all cities. However, the decline in NO2 concentrations attributable to the lockdowns was not as large as expected, at reductions of 10 to 50%. Accordingly, O3 increased by 2 to 30% (except for London), the total gaseous oxidant (O x = NO2 + O3) showed limited change, and PM2.5 concentrations decreased in most cities studied but increased in London and Paris. Our results demonstrate the need for a sophisticated analysis to quantify air quality impacts of interventions and indicate that true air quality improvements were notably more limited than some earlier reports or observational data suggested.

A review on analysis methods, source identification, and cancer risk evaluation of atmospheric polycyclic aromatic hydrocarbons.

Polycyclic aromatic hydrocarbons (PAHs) have gained attention because of their environmental persistence and effects on ecosystems, animals, and human health. They are mutagenic, carcinogenic, and teratogenic. The review provides background knowledge about their sources, metabolism, temporal variations, and size distribution in atmospheric particulate matter. The review article briefly discusses the analytical methods suitable for the extraction, characterization, and quantification of nonpolar and polar PAHs, addressing the challenges. Herein, we discussed the molecular diagnostic ratios (DRs), stable carbon isotopic analysis (SCIA), and receptor models, with much emphasis on the positive matrix factorization (PMF) model, for apportioning PAH sources. Among which, DRs and PCA identified as the most widely employed method, but their accuracy for PAH source identification has received global criticism. Therefore, the review recommends compound-specific isotopic analysis (CSIA) and PMF as the best alternative methods to provide detailed qualitative and quantitative source analysis. The compound-specific isotopic signatures are not affected by environmental degradation and are considered promising for apportioning PAH sources. However, isotopic fractions of co-eluted compounds like polar PAHs and aliphatic hydrocarbons make the PAHs isotopic fractions interpretation difficult. The interference of unresolved complex mixtures is a limitation to the application of CSIA for PAH source apportionment. Hence, for CSIA to further support PAH source apportionment, fast and cost-effective purification techniques with no isotopic fractionation effects are highly desirable. The present review explains the concept of stable carbon isotopic analysis (SCIA) relevant to PAH source analysis, identifying the techniques suitable for sample extract purification. We demonstrate how the source apportioned PAHs can be applied in assessing the health risk of PAHs using the incremental lifetime cancer risk (ILCR) model, and in doing so, we identify the key factors that could undermine the accuracy of the ILCR and research gaps that need further investigation.

Atmospheric conditions and composition that influence PM2.5 oxidative potential in Beijing, China.

Epidemiological studies have consistently linked exposure to PM2.5 with adverse health effects. The oxidative potential (OP) of aerosol particles has been widely suggested as a measure of their potential toxicity. Several acellular chemical assays are now readily employed to measure OP; however, uncertainty remains regarding the atmospheric conditions and specific chemical components of PM2.5 that drive OP. A limited number of studies have simultaneously utilised multiple OP assays with a wide range of concurrent measurements and investigated the seasonality of PM2.5 OP. In this work, filter samples were collected in winter 2016 and summer 2017 during the atmospheric pollution and human health in a Chinese megacity campaign (APHH-Beijing), and PM2.5 OP was analysed using four acellular methods: ascorbic acid (AA), dithiothreitol (DTT), 2,7-dichlorofluorescin/hydrogen peroxidase (DCFH) and electron paramagnetic resonance spectroscopy (EPR). Each assay reflects different oxidising properties of PM2.5, including particle-bound reactive oxygen species (DCFH), superoxide radical production (EPR) and catalytic redox chemistry (DTT/AA), and a combination of these four assays provided a detailed overall picture of the oxidising properties of PM2.5 at a central site in Beijing. Positive correlations of OP (normalised per volume of air) of all four assays with overall PM2.5 mass were observed, with stronger correlations in winter compared to summer. In contrast, when OP assay values were normalised for particle mass, days with higher PM2.5 mass concentrations (µgm-3) were found to have lower mass-normalised OP values as measured by AA and DTT. This finding supports that total PM2.5 mass concentrations alone may not always be the best indicator for particle toxicity. Univariate analysis of OP values and an extensive range of additional measurements, 107 in total, including PM2.5 composition, gas-phase composition and meteorological data, provided detailed insight into the chemical components and atmospheric processes that determine PM2.5 OP variability. Multivariate statistical analyses highlighted associations of OP assay responses with varying chemical components in PM2.5 for both mass- and volume-normalised data. AA and DTT assays were well predicted by a small set of measurements in multiple linear regression (MLR) models and indicated fossil fuel combustion, vehicle emissions and biogenic secondary organic aerosol (SOA) as influential particle sources in the assay response. Mass MLR models of OP associated with compositional source profiles predicted OP almost as well as volume MLR models, illustrating the influence of mass composition on both particle-level OP and total volume OP. Univariate and multivariate analysis showed that different assays cover different chemical spaces, and through comparison of mass- and volume-normalised data we demonstrate that mass-normalised OP provides a more nuanced picture of compositional drivers and sources of OP compared to volume-normalised analysis. This study constitutes one of the most extensive and comprehensive composition datasets currently available and provides a unique opportunity to explore chemical variations in PM2.5 and how they affect both PM2.5 OP and the concentrations of particle-bound reactive oxygen species.

Biomass burning and fungal spores as sources of fine aerosols in Yangtze River Delta, China - Using multiple organic tracers to understand variability, correlations and origins.

Research is restricted regarding impacts of biomass burning (BB) on fine aerosol (PM2.5), due mainly to lack of specific BB tracers. This study aims to characterize the variability, distributions, and contributions of BB and fungal spores as sources of PM2.5 using a multiple organic tracer approach. PM2.5 samples were collected at four representative sites in Yangtze River Delta (YRD), China every 6 days for one year. In the laboratory, samples were analyzed for three anhydrides (levoglucosan, mannosan, and galactosan), two sugar alcohols (arabitol and mannitol), water-soluble inorganic ions, and elemental/organic carbon (EC/OC). Levoglucosan was the most abundant BB tracer (mean concentration = 81 ng/m3), and fungal spore tracers arabitol and mannitol had similar abundances (5.6 and 5.7 ng/m3, respectively). Anhydrides and sugar alcohols had high within-group correlations, indicating their respective common sources. Concentrations of tracers displayed large temporal variations but small spatial variations, suggesting strong seasonality in BB and fungal spore sources. BB sources were burning of grass, pine needles, hardwood and crop straw, which were originated from transboundary/cross-region transport and local fire spots. PCA analyses revealed that the common sources of fine aerosols in YRD were secondary inorganic aerosols, soil dust, BB and fungal spores.

Simultaneous measurement of multiple organic tracers in fine aerosols from biomass burning and fungal spores by HPLC-MS/MS.

Three monosaccharide anhydrides (MAs: levoglucosan, mannosan, and galactosan) and sugar alcohols (arabitol and mannitol) are widely used as organic tracers for source identification of aerosols emitted from biomass burning and fungal spores, respectively. In the past, these two types of organic tracer have been measured separately or conjointly using different analytical techniques, with which a number of disadvantages have been experienced during the application to environmental aerosol samples, including organic solvent involved extraction, time-consuming derivatization, or poor separation efficiency due to overlapping peaks, etc. Hence, in this study a more environment-friendly, effective and integrated extraction and analytical method has been developed for simultaneous determination of the above mentioned organic tracers in the same aerosol sample using ultrasonication and high performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The ultrasonication assisted extraction process using ultrapure water can achieve satisfactory recoveries in the range of 100.3 ± 1.3% to 108.4 ± 1.6% for these tracers. All the parameters related to LC and MS/MS have been optimized to ensure good identification and pronounced intensity for each compound. A series of rigorous validation steps have been conducted. This newly developed analytical method using ultrasonication and HPLC-MS/MS has been successfully applied to environmental aerosol samples of different pollution levels for the simultaneous measurement of the above mentioned five organic tracers from biomass burning and fungal spores.

[Characteristics and Source Analysis of Atmospheric Carbonaceous Aerosols in the Cities of Hangzhou and Ningbo].

To investigate the seasonal variations and sources of carbonaceous aerosols in the cities of Hangzhou and Ningbo, field PM2.5 sampling was conducted at four representative sites (two urban, one suburban, and one rural) in this region from December 2014 to November 2015. A thermal/optical carbon analyzer was employed to analyze both organic carbon (OC) and elemental carbon (EC) contents in PM2.5 by identifying eight different carbon fractions, including OC1, OC2, OC3, OC4+OPC, EC1-OPC, EC2, and EC3. Based on these fractions, OC and EC were defined as OC1+OC2+OC3+OC4+OPC and EC1+EC2+EC3-OPC, respectively; total carbon (TC) was calculated as the sum of OC and EC; and total carbonaceous aerosols (TCAs) were quantified via the sum of organic aerosols (OAs; converted from OC) and EC. The results showed the following. ①The annual average level of TC in this region was (14.3±4.1) µg·m-3, accounting for (26.2±6.5)% of the annual average PM2.5 concentration. The annual average OC and EC concentrations were (11.3±3.4) µg·m-3 and (3.0±0.9) µg·m-3, respectively. The highest TC level was observed in winter among the four seasons. ②The annual average TCA concentration in this region was (25.6±7.5) µg·m-3, contributing (42.2±10.0)% of PM2.5. In addition, secondary organic carbon (SOC) was also estimated by the commonly applied EC method. It was found that SOC contributed (41.1±5.5)% to OC on an annual average basis. ③The sources of carbonaceous aerosols were determined using the correlation between OC and EC, OC/EC mass ratio, and different carbon fraction characteristics. The annual average OC/EC ratio in this region was 4.7±1.7, which falls in the diagnostic ratio range for vehicular emissions, coal combustion, and biomass burning, indicating these sources are probably the major contributors of the regional carbonaceous aerosols. Moreover, a higher char-EC/soot-EC ratio was observed during winter and autumn at all sites, possibly implying the enhanced biomass burning activities during these two seasons.

Temporal and spatial variation in major ion chemistry and source identification of secondary inorganic aerosols in Northern Zhejiang Province, China.

To investigate the seasonal and spatial variations of ion chemistry of fine particles in Northern Zhejiang Province (NZP), China, one year-long field sampling was conducted at four representative sites (two urban, one suburb, and one rural sites) in both cities of Hangzhou and Ningbo from December 2014 to November 2015. Twelve water soluble inorganic ions (WSII) were characterized in this comprehensive study. The annual average of PM2.5 concentration in NZP as overall was 66.2 ± 37.7 µg m-3, and urban sites in NZP were observed with more severe PM2.5 pollution than the suburban and rural sites. The annual average concentration of total WSII at four sampling sites in NZP was 29.1 ± 19.9 µg m-3, dominated by SO42- (10.3 µg m-3), and followed by NO3- (8.9 µg m-3), NH4+ (6.6 µg m-3), Cl- (1.3 µg m-3) and K+ (0.7 µg m-3). Among all cations, NH4+ was the predominant neutralizing ion with the highest neutralization factor (NF), while the remaining cations showed limited neutralization capacity. The highest and lowest sulfur oxidation ratio (SOR) values in this region were found in summer and winter, respectively; while the seasonal patterns for nitrogen oxidation ratio (NOR) were opposite to that of SOR. Principal component analysis (PCA) showed that the significant sources of WSII in NZP were industrial emissions, biomass burning, and formation of secondary inorganic aerosols. In addition, contribution from transboundary transport of polluted aerosols was also confirmed from the assessment through air mass backward trajectory analysis.