[Pollution Characteristics and Sources of Wintertime Atmospheric Brown Carbon at a Background Site of the Yangtze River Delta Region in China].

To investigate the pollution characteristics and sources of atmospheric brown carbon (BrC) in Chongming Island, a background site of the Yangtze River Delta (YRD) region in China, PM2.5 samples collected from December 2018 to January 2019 were analyzed to determine their chemical compositions and optical properties. The results showed that the light absorption coefficient (Abs365,M) of BrC extracted by methanol at 365 nm was (5.39±3.33) M-1·m-1, which was 1.3 times of the water extracted BrC. Both increased significantly with the increase of pH values, suggesting that less acidic conditions can enhance the light absorption ability of BrC. In winter, both Abs365 and MAE365 (mass absorption efficiency) were higher in the nighttime than in the daytime. A strong linear correlation observed between Abs365 and levoglucosan (R2=0.72) indicated that many light absorbing substances in Chongming Island were derived from biomass burning emissions. During the campaign, nitro-aromatic compounds (NACs) and PAHs accounted for (1.5±1.1) ng·m-3 and (8.3±4.7) ng·m-3, respectively, contributing to 0.1% and 0.067% of the absorption of the total BrC at 365 nm, respectively. Positive matrix factorization (PMF) analysis further showed that biomass and fossil fuel combustions were the main sources of BrC in Chongming Island in winter, accounting for 56% of the total BrC, followed by secondary formation, accounting for 24% of the total BrC, with road dust contributing only 6%.

[Pollution Characteristics and Source Apportionment of n-Alkanes and PAHs in Summertime PM2.5 at Background Site of Yangtze River Delta].

To investigate the pollution characteristics and sources of organic aerosols at a background site of the Yangtze River Delta, day- and night- PM2.5 samples were collected from May 30th to August 15th, 2018 in Chongming Island, China and measured for their normal alkanes (n-alkanes) and polycyclic aromatic hydrocarbons (PAHs) content employing a GC-MS technique. Concentrations of PM2.5, n-alkanes, and PAHs during the entire sampling period were (33±21) µg·m-3, (26±44) ng·m-3, and (0.76±1.0) ng·m-3, respectively. During the entire campaign, 35% of the collected PM2.5 samples were of a particle loading larger than the first grade of the China National Air Quality Standard (35 µg·m-3), suggesting that further mitigation with respect to air pollution in Chongming Island remains imperative. In the period with a PM2.5 concentration higher than 35 µg·m-3, which was classified as the pollution period, concentrations of n-alkanes and PAHs were one order of magnitude higher than those in the period with PM2.5 less than 15 µg·m-3, which was classified as the clean period. During the entire campaign, OC was higher in the daytime than in the nighttime, mainly due to the daytime photooxidation that enhanced the formation of secondary organic aerosols. During the pollution period, concentrations of EC and other pollutants were higher in the nighttime than in daytime, mainly due to the transport of the inland pollutants by the nighttime land breeze. Such a diurnal difference was not observed for the pollutants in clean periods, mainly due to the relatively clean breeze from East China Sea that diluted the air pollution. Diagnostic ratios showed that 67% of n-alkanes in PM2.5 was derived from fossil fuel combustion. PMF analysis further showed that during the pollution period, vehicle exhausts and industrial emissions were the largest sources of PAHs, both accounting for 51% of the total in PM2.5. In contrast, during the clean periods ship emissions were the largest source, contributing about 45% of the total PAHs, exceeding the sum (38%) of vehicle and industrial emissions.

Evolution of aerosol chemistry in Xi'an during the spring dust storm periods: Implications for heterogeneous formation of secondary organic aerosols on the dust surface.

TSP and 9-stage size-segregated samples were simultaneously collected in Xi'an during the spring of 2013 and analyzed for organic aerosols (OA) on a molecular level. n-Alkanes were the dominant compound class during the whole campaign, followed by fatty acids. High molecular weight (HMW) n-alkanes and fatty acids dominated in the coarse mode particles (>1.1 µm) during the dust event, indicating they were mostly originated from surface soil and plants in the upwind regions. Low-volatile anthropogenic compounds such as benzo(e)pyrene (BeP) and bisphenol A (BPA) dominated in the fine mode particles during the whole campaign. In contrast, semi-volatile anthropogenic compounds such as phenanthrene (Phe) and di-n-butyl phthalates (DBP) showed a bimodal size distribution with a significant increase in the coarse mode during the dust event due to their vaporization from the fine mode particles and the subsequent adsorption on the dust surface. Secondary organic aerosols (SOA) in Xi'an during the dust storm period were predominantly enriched on the coarse particles, which can be ascribed to the adsorption and subsequent oxidation of gas-phase hydrophilic organics on the aqueous-phase of hygroscopic dust surface (e.g., mirabilite). Our work suggested an important role of multiphase reaction in evolution of aerosol chemistry during the dust long-range transport process.

[Vertical Distributional Characteristics of Inorganic Ions of PM2.5 at Mt. Huashan, Inland China].

PM2.5 was simultaneously collected using a high-volume sampler at 4 h intervals from the mountainside and the foot of the mountain in the Mt. Huashan region, inland China, during the summer of 2016, and the samples were analyzed for inorganic ions, to investigate the chemical characteristics and vertical distribution of the fine particles in the region. The results showed that the concentrations of PM2.5 were (46.9±38.2) µg·m-3 and (76.0±44.3) µg·m-3 on the mountainside and at the foot of Mt. Huashan, respectively. The concentrations of inorganic ions in PM2.5 was higher at the foot of the mountain than on the mountainside, with the order of the mass concentrations of the major ionic species being SO42- > NO3- > NH4+ > Ca2+. Among all the inorganic ions, SO42-, NO3-, and NH4+ are the dominant species, accounting for 89% and 85% of the total, on the mountainside and at the foot, respectively. The fine particulate NH4+ existed mostly in the forms of (NH4)2SO4 and NH4NO3 on the mountainside, and in the forms of NH4HSO4 and NH4NO3 at the foot of the mountain. Mass concentrations of PM2.5 and its major components on the mountainside showed clear diurnal variations, with maximums between 12:00-16:00, mainly due to the transport of the pollutants from the ground surface by the planetary boundary layer height variation and the valley breeze. In contrast, the diurnal variations of PM2.5 and its major components at the foot are characterized with two maxima, peaking between 08:00-12:00 in the daytime and 00:00-04:00 in the nighttime, respectively, mainly due to the increased emissions from both the morning rush-hour traffic and the nighttime on-road heavy-duty vehicles. Acidity of the fine particles was estimated by using the equivalent ratio of anions to cations and the thermodynamic equilibrium model ISORROPIA Ⅱ. Both methods showed that the acidity of PM2.5 at the ground surface site is stronger than that on the mountainside in the Mt. Huashan region.

[Analysis of Different Particle Sizes, Pollution Characteristics, and Sources of Atmospheric Aerosols During the Spring Dust Period in Beijing].

To understand the evolution of the physical and chemical properties of dust aerosols in the atmosphere, the concentrations and chemical compositions of differently sized particles were continuously observed and analyzed using an ion chromatograph and carbonaceous analyzer during the outbreak of dust in May 2017 in Beijing. The concentrations of total suspended particulate (TSP), water-soluble organic carbon (WSOC), elemental carbon (EC), OC, and water-soluble inorganic ions were (2237.59±681.49), (29.90±18.05), (1.46±3.05), (67.35±29.07), and (136.75±46.38) µg·m-3 during the dust period, respectively, and significantly exceeded that of the non-dust period, except for EC. The Na+, NH4+, K+, Mg2+, Ca2+, Cl-, NO3-, SO42-, and WSOC concentrations during the dust storm period were 11.55, 3.00, 14.88, 14.89, 9.40, 4.60, 2.40, 3.91, and 1.83 times higher than that during the non-dust period. The growth of crustal ions, such as Ca2+ and K+, was notably the largest and NH4+ and NO3- were minimal. The size distribution indicates that crustal ions primarily occur in the coarse mode during the whole sampling campaign. The SO42- and NO3- ions are slightly bimodal during the dust storm, with a dominant peak in the coarse mode at 4.7-5.8 µm and a very minor peak in the fine mode with a size range of 0.43-0.65 µm. During the non-dust period, SO42- is the dominant mode in the fine mode, while NO3- changes little compared with that during the dust period, which indicates that heterogeneous reaction with crustal ions is the main formation mechanism of NO3- in the coarse mode. A significant positive correlation was observed between SO42- and the sum of crustal ions during the dust period, indicating that the source of SO42- during the dust period is remote transmission of the dust storm. During the non-dust period, the positive correlation of SO42- with NH4+ indicates that secondary formation is the main source of SO42-. Based on correlation analysis of NO3- with crustal ions and NH4+, both remote transmission and secondary formation are the sources of NO3- during the dust storm and heterogeneous reactions are predominant during the non-dust period.

Characteristics of polycyclic aromatic hydrocarbons in PM2.5 emitted from different cooking activities in China.

Nineteen polycyclic aromatic hydrocarbons (PAHs) in PM2.5 emitted from five different cooking activities were characterized, and their influencing factors were determined. The total quantified particle-bounded PAH concentrations (ΣPAHs) in the airs from the cooking activities were 4.2-36.5-fold higher than those in corresponding backgrounds. The highest ΣPAHs were seen in cafeteria frying (783 ± 499 ng/m3), followed by meat roasting (420 ± 191 ng/m3), fish roasting (210 ± 105 ng/m3), snack-street boiling (202 ± 230 ng/m3), and cafeteria boiling (150 ± 65 ng/m3). The main influencing factors on the PAH emissions were cooking methods, fat contents in raw materials, and oil consumptions. Four- to six-ringed PAHs had the highest contributions to the ΣPAHs (avg. 87.5%). Diagnostic ratios of individual PAH were similar between the two charbroiling and other three conventional Chinese cooking methods, respectively, demonstrating the dominance of cooking methods in the PAH emissions. Remarkably high benzo(b)fluoranthene/benzo(k)fluoranthene (BbF/BkF) ratio (8.31) was seen in the snack-street boiling, attributed to the coal combustion as cooking fuel. Both fluoranthene/(fluoranthene + pyrene) [FLT/(FLT + PYR)] and benzo(a)anthracene/(benzo(a)anthracene + chrysene) [BaA/(BaA + CHR)] ratios were higher for the oil-based cooking than those from the water-based ones. In addition, two ratios of indeno(1,2,3-cd)pyrene/(indeno(1,2,3-cd)pyrene + benzo(g,h,i)perylene) [IPY/(IPY + BPE)] and benzo(a)pyrene/(benzo(a)pyrene + benzo(g,h,i)perylene) [BaP/(BaP + BPE)] were higher for two charbroiling than the three conventional Chinese cooking methods. The characterization work in this study is particularly important since cooking is a potential contributor of atmospheric PAHs in urban China. Carcinogenic potencies of PAHs were assessed by comparison with the air quality guideline and health risk estimation. The BaP and BaP equivalent were higher for the oil-based than the water-based cooking activities.

Characterization and seasonal variations of levoglucosan in fine particulate matter in Xi'an, China.

PM2.5 (particulate matter with an aerodynamic diameter <2.5 microm) samples (n = 58) collected every sixth day in Xi'an, China, from 5 July 2008 to 27 June 2009 are analyzed for levoglucosan (1,6-anhydro-beta-D-glucopyranose) to evaluate the impacts of biomass combustion on ambient concentrations. Twenty-four-hour levoglucosan concentrations displayed clear summer minima and winter maxima that ranged from 46 to 1889 ng m(-3), with an average of 428 +/- 399 ng m(-3). Besides agricultural burning, biomass/biofuel combustion for household heating with straws and branches appears to be of regional importance during the heating season in northwestern China. Good correlations (0.70 < R < 0.91) were found between levoglucosan relative to water- soluble K+, Cl-, organic carbon (OC), elemental carbon (EC), and glyoxal. The highest levoglucosan/OC ratio of2.3% wasfound in winter, followed by autumn (1.5%). Biomass burning contributed to 5.1-43.8% of OC (with an average of 17.6 +/- 8.4%).

[Characteristics of water-soluble organic nitrogen of PM2.5 in Xi'an during wintertime non-haze and haze periods].

High-volume PM2.5 samples were collected hourly from 4 December to 13 December 2012 at an urban site in Xi'an and analyzed for organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), water-soluble total nitrogen (WSTN), water-soluble organic nitrogen (WSON) and inorganic ions to investigate the sources and formation mechanism of WSON. The results showed that during the sampling period the averaged hourly concentration of WSON was (12 +/- 9.4) microg x m(-3) and maximized at 31 microg x m(-3), accounting for 47% +/- 9.8% of WSTN with NH4(+) -N and NO3(-) -N being 29% +/- 8.5% and 23% +/- 8.1%, respectively. WSON: WSOC (N: C) mass ratios ranged from 0.04 to 0.65 with an average of 0.31 +/- 0.13 during the observation period. WSON was (1.6 +/- 0.9) microg x m(-3), (6.5 +/- 3.9) microg x m(-3) and (23 +/- 4.7) microg x m(-3) in non-haze days (visibility > 10 km), light haze days (5 km < visibility < 10 km) and heavy haze days (visibility < 5 km), respectively. WSOC/OC mass ratio throughout the observation period showed no significant change, but WSON/WSOC(N: C) mass ratio increased significantly from a lower value of 0.2 +/- 0.1 in non-haze days to 0.3 +/- 0.1 on light haze days and 0.4 +/- 0.1 on heavy haze days, in consistence with the enhanced acidity of the fine particles. In addition, during the whole sampling period, WSON was strongly correlated with NH4(+), SO4(2-) and NO3(-) (R2 > 0.80), and negatively correlated with cation-anion equivalent ratio (R2 = 0.53). These phenomena can be mainly ascribed to a gas-particle conversion of gaseous water-soluble nitrogen-containing organic compounds like amines via acid-base reactions, which was sharply increased under the favorable meteorological conditions (e.g., low temperature and high humidity) during the heavy haze days.

[Study on pollution characteristics of carbonaceous aerosols in Xi'an City during the spring festival].

The samples of PM2.5 with 8 times periods were collected using Automated Cartridge Collection Unit (ACCU) of Rupprecht& Patashnick (R&P)Corporation, and monitored by R&P1400a instrument of TEOM series online during 2011 Spring Festival in Xi'an city. The organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and water-insoluble organic carbon (WIOC) contents of 3 h integrated PM2.5 were analyzed to evaluate the influence of firework display on the carbonaceous components in urban air. The mass concentration of PM2.5 was found increased significantly from 00:00 A. M. to 02:59 A. M. at the Chinese Lunar New Year's Eve than the non-firework periods, reaching 1514.8 microg.m-3 at 01:00 A. M. The mass concentrations of OC, EC, WSOC, and WIOC during the same time period were 123.3 microg.m-3, 18.6 microg.m-3, 66.7 microg.m-3, and 56.6 microg.m-3, about 1.7, 1.2, 1.4, and 2.2 times higher than the average in normal days, respectively. Correlation analysis among WSOC, OC, and EC contents in PM25 showed that firework emission was an obvious source of carbonaceous aerosol in the Spring Festival vacation. However, it only contributes to 9. 4% for aerosol in fireworks emission.

Winter and summer PM2.5 chemical compositions in fourteen Chinese cities.

UNLABELLED: PM2.5 in 14 of China's large cities achieves high concentrations in both winter and summer with averages > 100 microg m(-3) being common occurrences. A grand average of 15 microg m(-3) was found for all cities, with a minimum of 27 microg m(-3) measured at Qingdao during summer and a maximum of 356 microg m(-3) at Xi 'an during winter. Both primary and secondary PM2.5 are important contributors at all of the cities and during both winter and summer. While ammonium sulfate is a large contributor during both seasons, ammonium nitrate contributions are much larger during winter. Lead levels are still high in several cities, reaching an average of 1.68 microg m(-3) in Xi 'an. High correlations of lead with arsenic and sulfate concentrations indicate that much of it derives from coal combustion, rather than leaded fuels, which were phased out by calendar year 2000. Although limited fugitive dust markers were available, scaling of iron by its ratios in source profiles shows -20% of PM2.5 deriving from fugitive dust in most of the cities. Multipollutant control strategies will be needed that address incomplete combustion of coal and biomass, engine exhaust, and fugitive dust, as well as sulfur dioxide, oxides of nitrogen, and ammonia gaseous precursors for ammonium sulfate and ammonium nitrate. IMPLICATIONS: PM2.5 mass and chemical composition show large contributions from carbon, sulfate, nitrate, ammonium, and fugitive dust during winter and summer and across fourteen large cities. Multipollutant control strategies will be needed that address both primary PM2.5 emissions and gaseous precursors to attain China's recently adopted PM2.5 national air quality standards.