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An intensive investigation of carbonaceous PM2.5 and TSP (total suspended particles) from Pudong (China) was conducted as part of the MIRAGE-Shanghai (Megacities Impact on Regional and Global Environment) experiment in 2009. Data for organic and elemental carbon (OC and EC), organic species, including C17 to C40 n-alkanes and 17 polycyclic aromatic hydrocarbons (PAHs), and stable carbon isotopes OC (δ13COC) and EC (δ13CEC) were used to evaluate the aerosols' temporal variations and identify presumptive sources. High OC/EC ratios indicated a large fraction of secondary organic aerosol (SOA); high char/soot ratios indicated stronger contributions to EC from motor vehicles and coal combustion than biomass burning. Diagnostic ratios of PAHs indicated that much of the SOA was produced via coal combustion. Isotope abundances (δ13COC = −24.5 ± 0.8‰ and δ13CEC = −25.1 ± 0.6‰) indicated that fossil fuels were the most important source for carbonaceous PM2.5 (particulate matter less than 2.5 micrometers in diameter), with lesser impacts from biomass burning and natural sources. An EC tracer system and isotope mass balance calculations showed that the relative contributions to total carbon from coal combustion, motor vehicle exhaust, and SOA were 41%, 21%, and 31%; other primary sources such as marine, soil and biogenic emissions contributed 7%. Combined analyses of OC and EC, n-alkanes and PAHs, and stable carbon isotopes provide a new way to apportion the sources of carbonaceous particles.

During winter 2013, extremely high concentrations (i.e., 4–20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including Xi'an, Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set from elemental carbon (EC), organic carbon (OC), 14C and biomass-burning marker measurements using Latin hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. Based on 14C measurements of EC fractions (six samples each city), we found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% across all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC), respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8, 48 ± 18, 53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass-burning emissions. For each site, we also compared samples from moderately to heavily polluted days according to particulate matter mass. Despite a significant increase of the absolute mass concentrations of primary emissions from both fossil and non-fossil sources during the heavily polluted events, their relative contribution to TC was even decreased, whereas the portion of SOC was consistently increased at all sites. This observation indicates that SOC was an important fraction in the increment of carbonaceous aerosols during the haze episode in China.

China has experienced considerable economic losses from a severe deterioration in air quality. To solve this, a comprehensive understanding of the impacts and sources of air pollution is necessary. This study aimed to quantify the environmental and human health impacts of PM2.5 and O3 pollution from the six major emission-producing sectors in China. We utilized a chemical transport model to simulate the air quality impacts engendered by sectoral emissions. The consequent impacts on public health and crop production, as well as the corresponding collateral economic costs, were quantified by concentration-response functions. The results show that the sectoral emissions in 2010 caused approximately 1 143 000 (95% confidence interval (CI): 168 000-1 796 000) premature mortalities and a 20 035 (95% CI: 6776-32 166) Gg crop production loss. Of the six sectors, the industrial sector was the largest contributor of air pollution, accounting for 36% of the total impact on health, as well as 41% of crop production loss due to O3 exposure. The impacts attributable to sectoral emissions in China were estimated to cost ∼267 (95% CI: 180-360) billion yuan (0.66% of the annual GDP). Our findings suggest an urgent need to reduce anthropogenic emissions in China, particularly those of the industrial sector. The varying characteristics of impact due to emissions of various sectors highlight the importance of evaluating cobenefits when formulating emission control policies.

We calculated the organic matter to organic carbon mass ratios (OM/OC mass ratios) in PM2.5 collected from 14 Chinese cities during summer and winter of 2003 and analyzed the causes for their seasonal and spatial variability. The OM/OC mass ratios were calculated two ways. Using a mass balance method, the calculated OM/OC mass ratios averaged 1.92 ± 0.39 year-round, with no significant seasonal or spatial variation. The second calculation was based on chemical species analyses of the organic compounds extracted from the PM2.5 samples using dichloromethane/methanol and water. The calculated OM/OC mass ratio in summer was relatively high (1.75 ± 0.13) and spatially-invariant due to vigorous photochemistry and secondary organic aerosol (OA) production throughout the country. The calculated OM/OC mass ratio in winter (1.59 ± 0.18) was significantly lower than that in summer, with lower values in northern cities (1.51 ± 0.07) than in southern cities (1.65 ± 0.15). This likely reflects the wider usage of coal for heating purposes in northern China in winter, in contrast to the larger contributions from biofuel and biomass burning in southern China in winter. On average, organic matter constituted 36% and 34% of Chinese urban PM2.5 mass in summer and winter, respectively. We report, for the first time, a high regional correlation between Zn and oxalic acid in Chinese urban aerosols in summer. This is consistent with the formation of stable Zn oxalate complex in the aerosol phase previously proposed by Furukawa and Takahashi (2011). We found that many other dicarboxylic acids were also highly correlated with Zn in the summer Chinese urban aerosol samples, suggesting that they may also form stable organic complexes with Zn. Such formation may have profound implications for the atmospheric abundance and hygroscopic properties of aerosol dicarboxylic acids.

Ground‐based studies of PM2.5 were conducted for determination of 30 water‐soluble organic species, including dicarboxylic acids, ketocarboxylic acids and dicarbonyls, nine fatty acids, and benzoic acid, during the Campaign of Air Quality Research in Beijing 2006 (CAREBeijing‐2006; 21 August to 4 September 2006) at urban (Peking University, PKU) and suburban (Yufa) sites of Beijing. Molecular distributions of dicarboxylic acids demonstrated that oxalic acid (C2) was the most abundant species, followed by phthalic acid (Ph) and succinic acid (C4) at both sites. The sum of three dicarboxylic acids accounted for 71% and 74% of total quantified water‐soluble organics (327–1552 and 329–1124 ng m−3) in PKU and Yufa, respectively. Positive correlation was found between total quantified water‐soluble species and water‐soluble organic compounds (WSOC). On a carbon basis, total quantified dicarboxylic acids and ketocarboxylic acids and dicarbonyls account for up to 14.2% and 30.4% of the WSOC in PKU and Yufa, respectively, suggesting that they are the major WSOC fractions in Beijing. The distributions of fatty acids are characterized by a strong even carbon number predominance with maximum at hexadecanoic acid (C16:0). The ratio of octadecanoic acid (C18:0) to hexadecanoic acid (C16:0) (0.39–0.85, with an average of 0.36) suggests that in addition to vehicular emissions, an input from cooking emissions is important, as is biogenic emission. Benzoic acid that has been proposed as a primary pollutant from vehicular exhaust and a secondary product from photochemical reactions was found to be abundant: 72.2 ± 58.1 ng m−3 in PKU and 78.0 ± 47.3 ng m−3 in Yufa. According to the 72 hour back trajectory analysis, when the air mass passed over the southern or southeastern part of Beijing (24–25 August and 1–2 September), the highest concentrations of organic compounds were observed. On the contrary, when the clean air masses came straight from the north during 3–4 September, the lowest levels of organic compounds were recorded. This study demonstrates that pollution episodes in Beijing were strongly controlled by wind direction; that is, air quality in Beijing is good when air masses originate from the north and northwest, whereas it deteriorates when the air mass originates from the south and southeast.

Ground-based PM2.5 samples collected at four different sites in Pearl River Delta region (PRD) during winter and summer (from 14 December 2006 to 28 January 2007 in winter and from 4 July to 9 August 2007 in summer) were analyzed for 30 water-soluble organic species, including dicarboxylic acids, ketocarboxylic acids and dicarbonyls, nine fatty acids, and benzoic acid. Molecular distributions of dicarboxylic acids demonstrated that oxalic acid (C2 ) was the most abundant species followed by phthalic acid (Ph) in PRD region. The concentrations of total dicarboxylic acids ranged from 99 to 1340 ng m-3 , with an average of 438 ± 267 ng m-3 in PRD. The concentrations of total ketocarboxylic acids ranged from 0.6 to 207 ng m-3 (43 ± 48 ng m-3 on average) while the concentrations of total α-dicarbonyls, including glyoxal and methylglyoxal, ranged from 0.2 to 89 ng m-3 , with an average of 11 ± 18 ng m-3 in PRD. The total quantified water-soluble compounds (TQWOC) (organic carbon) accounted for 3.4 ± 2.2% of OC and 14.3 ± 10.3% of water-soluble OC (WSOC). Hexadecanoic acid (C16:0 ), octadecanoic acid (C18:0 ) and oleic acid (C18:1 ) were the three most abundant fatty acids in PRD. The distributions of fatty acids were characterized by a strong even carbon number predominance with a maximum (Cmax ) at hexadecanoic acid (C16:0 ). Ratio of C18:1 to C18:0 acts as an indicator for aerosol aging. In PRD, an average of C18:1 /C18:0 ratio was 0.53 ± 0.39, suggesting an enhanced photochemical degradation of unsaturated fatty acid. Moreover, the concentrations of benzoic acid ranged from 84 to 306 ng m-3 , (165 ± 48 ng m-3 on average), which can be emitted as primary pollutant from motor vehicles exhaust, or formed from photochemical degradation of aromatic hydrocarbons. Seasonal variations of the organic specie concentrations were found in the four sampling cities. Higher concentrations of TQWOC were observed in winter (598 ± 321 ng m-3 ) than in summer (372 ± 215 ng m-3 ). However, the abundances of TQWOC in OC mass were higher in summer (0.9-12.4%, 4.5 ± 2.7% on average) than in winter (1.1-5.7, 2.5 ± 1.2% on average), being consistent with enhanced secondary production of dicarboxylic acids in warmer weather. Spatial variations of water-soluble dicarboxylic acids were characterized by higher concentrations in Hong Kong and lower concentrations in Guangzhou (GZ)/Zhaoqing (ZQ) during winter whereas the highest concentrations were observed in GZ/ZQ during summer. These spatial and seasonal distributions are consistent with photochemical production and the subsequent accumulation under different meteorological conditions.

In the urban area of Guangzhou, observations on aerosol light extinction effect were conducted at a monitoring site of the South China Institute of Environmental Sciences (SCIES) during April 2009, July 2009, October 2009 and January 2010. The main goal of these observations is to recognise the impact of relative humidity (RH) and particles number distribution on aerosol light extinction. PM2.5 was sampled by Model PQ200 air sampler; ions and OC/EC in PM2.5 were identified by the Dionex ion chromatography and the DRI model 2001 carbon analyser, respectively; particles number size distribution was measured by TSI 3321 APS, while total light scattering coefficient was measured by TSI 3563 Nephelometer. Chemical composition of PM2.5 was reconstructed by the model ISORROPIA II. As a result, possible major components in PM2.5 were (NH4)2SO4, Na2SO4, K2SO4, NH4NO3, HNO3, water, POM and EC. Regarding ambient RH, mass concentration of PM2.5 ranged from 26.1 to 279.1 μg m−3 and had an average of 94.8, 44.6, 95.4 and 130.8 μg m−3 in April, July, October and January, respectively. With regard to the total mass of PM2.5, inorganic species, water, POM, EC and the Residual accounted for 34–47%, 19–31%, 14–20%, 6–8% and 8–17%, respectively. Under the assumption of \"internal mixture\", optical properties of PM0.5–20 were estimated following the Mie Model. Optical refractive index, hygroscopic growth factor and the dry aerosol density required by the Mie Model were determined with an understanding of chemical composition of PM2.5. With these three parameters and the validated particles number size distribution of PM0.5–20, the temporal variation trend of optical property of PM0.5–20 was estimated with good accuracy. The highest average of bep,pm0.5–20 was 300 Mm−1 in April while the lowest one was 78.6 Mm−1 in July. Regarding size distribution of bep,pm0.5–20, peak value was almost located in the diameter range between 0.5 and 1.0 μm. Furthermore, hygroscopic growth of optical properties of PM0.5–20 largely depended on RH. As RH increased, bep,pm0.5–20 grew and favoured a more rapid growth when aerosol had a high content of inorganic water-soluble salts. Averagely, fbep,pm0.5–20 enlarged 1.76 times when RH increased from 20% to 90%. With regard to the temporal variation of ambient RH, fbep,pm0.5–20 was 1.29, 1.23, 1.14 and 1.26 on average in April, July, October and January, respectively.

Seventeen airborne carbonyls including monocarbonyls and dicarbonyls were determined in urban and sub-urban sites of Xi’an, China in three seasons in 2010. In winter, acetone was the most abundant carbonyl in the urban site due to usage of organic solvents in constructions and laboratories and its slower atmospheric removal mechanisms by photolysis and reaction with hydroxyl radical than those of formaldehyde and acetaldehyde. In the sub-urban site, acetaldehyde was the most abundant carbonyl, followed by formaldehyde and acetone. During summer, however, formaldehyde was the most dominant carbonyl in both sites. The photooxidations of a wide range of volatile organic compounds (VOCs) yielded much more formaldehyde than other carbonyls under high solar radiation and temperature. In the urban site, the average concentrations of dicarbonyls (i.e., glyoxal and methyglyoxal) in spring and summer were higher than that in winter. Transformation of aromatic VOCs emitted from fuel evaporation leads to the formation of 1,2-dicarbonyls. A reverse trend was observed in sub-urban sites, as explained by the relatively low abundances and accumulations of VOC precursors in the rural atmosphere during warm seasons. Moreover, cumulative cancer risk based on measured outdoor carbonyls (formaldehyde and acetaldehyde) in Xi’an Jiaotong University and Heihe was estimated (8.82 × 10⁻⁵ and 4.96 × 10⁻⁵, respectively). This study provides a clear map on the abundances of carbonyls and their source interpretation in the largest and the most economic city in Northwestern China.

Background, aim, and scope Photochemical smog, characterized by high concentrations of O₃ and fine particles, is of great concern in the urban areas, in particular megacities and city clusters like the Pearl River Delta. Materials, methods, and results Ambient ozone (O₃) and its precursors were simultaneously measured at two sites in the Pearl River Delta, namely, Wan Qing Sha (WQS) in Guangzhou and Tung Chung (TC) in Hong Kong, from 23 October to 01 December 2007 in order to explore their potential relationship. Eight high O₃ episode days were identified at WQS and two at TC during the sampling campaign, indicating a more serious O₃ pollution in Guangzhou than in Hong Kong. An observation-based model was employed to determine the ozone-precursor relationship. At both sites, O₃ production was found to be volatile organic compound (VOC)-limited, which is consistent with previous observations. Anthropogenic hydrocarbons played a key role in O₃ production, while reducing nitric oxide emissions aided the buildup of O₃ concentrations. Among VOC species, the summed relative incremental reactivity (RIR) of the top 12 compounds accounted for 89% and 85% of the total RIR at WQS and TC, respectively, indicating that local photochemical O₃ formation can be mainly attributed to a small number of VOC species. Discussion and conclusions A large increment in both simulated HO₂ and O₃ concentrations was achieved with additional input of hourly carbonyl data. This suggested that apart from hydrocarbons, carbonyls might significantly contribute to the O₃ production in the Pearl River Delta.

In recent years low molecular weight alkylamines have been recognized to play an important role in particle formation and growth in the lower atmosphere. However, major uncertainties are associated with their atmospheric processes, sources and sinks, mostly due to the lack of ambient measurements and the difficulties in accurate quantification of alkylamines at trace level. In this study, we present the evaluation and optimization of two analytical approaches, i.e., gas chromatography–mass spectrometry (GC-MS) and ion chromatography (IC), for the determination of alkylamines in aerosol particles. Alkylamines were converted to carbamates through derivatization with isobutyl chloroformate for GC-MS determination. A set of parameters affecting the analytical performances of the GC-MS approach, including reagent amount, reaction time and pH value, was evaluated and optimized. The accuracy is 84.3–99.1%, and the limits of detection obtained are 1.8–3.9 pg (or 0.02–0.04 ng m−3). For the IC approach, a solid-phase extraction (SPE) column was used to separate alkylamines from interfering cations before IC analysis. 1–2% (v/v) of acetone (or 2–4% (v/v) of acetonitrile) was added to the eluent to improve the separation of alkylamines on the IC column. The limits of detection obtained are 2.1–15.9 ng (or 0.9–6.4 ng m−3), and the accuracy is 55.1-103.4%. The lower accuracy can be attributed to evaporation losses of amines during the sample concentration procedure. Measurements of ambient aerosol particle samples collected in Hong Kong show that the GC-MS approach is superior to the IC approach for the quantification of primary and secondary alkylamines due to its lower detection limits and higher accuracy.