Fossil and Nonfossil Sources of Winter Organic Aerosols in the Regional Background Atmosphere of China.

Carbonaceous aerosols (CA) from anthropogenic emissions have been significantly reduced in urban China in recent years. However, the relative contributions of fossil and nonfossil sources to CA in rural and background regions of China remain unclear. In this study, the sources of different carbonaceous fractions in fine aerosols (PM2.5) from five background sites of the China Meteorological Administration Atmosphere Watch Network during the winter of 2019 and 2020 were quantified using radiocarbon (14C) and organic markers. The results showed that nonfossil sources contributed 44-69% to total carbon at these five background sites. Fossil fuel combustion was the predominant source of elemental carbon at all sites (73 ± 12%). Nonfossil sources dominated organic carbon (OC) in these background regions (61 ± 13%), with biomass burning or biogenic-derived secondary organic carbon (SOC) as the most important contributors. However, the relative fossil fuel source to OC in China (39 ± 13%) still exceeds those at other regional/background sites in Asia, Europe, and the USA. SOC dominated the fossil fuel-derived OC, highlighting the impact of regional transport from anthropogenic sources on background aerosol levels. It is therefore imperative to develop and implement aerosol reduction policies and technologies tailored to both the anthropogenic and biogenic emissions to mitigate the environmental and health risks of aerosol pollution across China.

Is biomass burning always a dominant contributor of fine aerosols in upper northern Thailand?

Biomass burning (BB) is an important contributor to the air pollution in Southeast Asia (SEA), but the emission sources remain great uncertainty. In this study, PM2.5 samples were collected from an urban (Chiang Mai University, CMU) and a rural (Nong Tao village, NT) site in Chiang Mai, Thailand from February to April (high BB season, HBB) and from June to September (low BB season, LBB) in 2018. Source apportionment of carbonaceous aerosols was carried out by Latin Hypercube Sampling (LHS) method incorporating the radiocarbon (14C) and organic markers (e.g., dehydrated sugars, aromatic acids, etc.). Thereby, carbonaceous aerosols were divided into the fossil-derived elemental carbon (ECf), BB-derived EC (ECbb), fossil-derived primary and secondary organic carbon (POCf, SOCf), BB-derived OC (OCbb) and the remaining OC (OCnf, other). The fractions of ECbb generally prevailed over ECf throughout the year. OCbb was the dominant contributor to total carbon with a clear seasonal trend (65.5 ± 5.8 % at CMU and 79.9 ± 7.6 % at NT in HBB, and 39.1 ± 7.9 % and 42.8 ± 4.6 % in LBB). The distribution of POCf showed a spatial difference with a higher contribution at CMU, while SOCf displayed a temporal variation with a greater fraction in LBB. OCnf, other was originated from biogenic secondary aerosols, cooking emissions and bioaerosols as resolved by the principal component analysis with multiple liner regression model. The OCnf, other contributed within a narrow range of 6.6 %-14.4 %, despite 34.9 ± 7.9 % at NT in LBB. Our results highlight the dominance of BB-derived fractions in carbonaceous aerosols in HBB, and call the attention to the higher production of SOC in LBB.

[Changes in Carbonaceous Aerosol in the Northern Suburbs of Nanjing from 2015 to 2019].

Carbonaceous aerosol is an important component of atmospheric fine particles that has an important impact on air quality, human health, and climate change. In order to explore the long-term changes in carbonaceous aerosol under the background of emission reduction, this study measured the mass concentrations of organic carbon (OC) and elemental carbon (EC) of PM2.5, which collected in the northern suburbs of Nanjing for five years (December 17, 2014 to January 5, 2020). The results showed that the five-year average ρ(OC) and ρ(EC) were (10.2±5.3) µg·m-3 and (1.6±1.1) µg·m-3, accounting for 31.1% and 5.2% of PM2.5, respectively. OC and EC concentrations were both high in winter and low in summer. According to the nonparametric Mann-Kendall test and Sen's slope, the mass concentrations of OC and PM2.5 decreased significantly[OC:P<0.0001, -0.79 µg·(m3·a)-1, -0.29%·a-1; PM2.5:P<0.0001, -4.59 µg·(m3·a)-1, -1.58%·a-1]. Although EC had an upward trend, the significance and range of change were not obvious[P=0.02, 0.05 µg·(m3·a)-1, 0.02%·a-1]. OC and EC decreased significantly during winter from 2014 to 2019[OC:P<0.0001, -2.05 µg·(m3·a)-1, -0.74%·a-1; EC:P=0.001, -0.15 µg·(m3·a)-1, -0.05%·a-1], and the decline was more obvious than the whole. The correlation between OC and EC showed that the sources in winter and summer were more complex than those in spring and autumn. According to the characteristic ratio of OC and EC, the contribution of coal combustion and biomass burning decreased from 2015 to 2019, whereas the impact of industrial sources and vehicle emissions became more significant. Corresponding to this was the obvious decline in OC and the slight recovery of EC. The OC/EC ratio was over 2.0, indicating that there was secondary pollution in the study area. Further calculation revealed that the variation in SOC was consistent with that in OC, showing a significant decrease[P<0.0001, -0.47 µg·(m3·a)-1, -0.17%·a-1]. The average mass concentration of SOC was (5.0±3.5) µg·m-3, accounting for 49.2% of OC. These changes indicate clear effects of the prevention and control of air pollution in Nanjing in recent years. Furthermore, future control can focus on the emissions of VOCs to reduce secondary pollution.

[Distribution Characteristics and Source of Black Carbon Aerosols in the Northern Suburbs of Nanjing].

Black carbon (BC) is an important component of atmospheric particulate matter (PM) emitted during the combustion process. Light absorption and scattering exhibited by BC affect the exchange of solar energy on Earth. In this study, continuous measurements of atmospheric particulate BC were carried out, using a BC analyzer (AE33) in the suburban area of Nanjing from January 2019 to May 2019, to realize the diurnal variations of BC during the different seasons and potential sources of BC during the clean (CD, PM2.5<35 µg ·m-3) and haze days (PD, PM2.5>75 µg ·m-3). The results showed that the average concentration of BC was (3.8±2.3) µg ·m-3; a higher average BC concentration value of (4.3±2.6) µg ·m-3 was observed during the winter, exceeding that during the spring period by a factor of 1.3. The higher BC concentrations during the winter was attributed to the stagnant weather conditions and additional emissions. Significant diurnal cycles of BC were observed with higher BC concentrations during rush hours of traffic, suggesting traffic origins. The Ångström exponent were 1.32 and 1.30 during the spring and winter periods, respectively, indicating that the BC was mainly produced from the traffic emissions during both the seasons. This hypothesis was also supported by the average BC/CO ratio of 0.005, which was similar to that of BC derived by traffic emissions. Moreover, we discovered that the contributions of traffic emissions to BC were 68%-87% and 72%-86% during the haze and clean periods, respectively. This indicated enhanced contributions of coal combustion and biomass burning to BC in Nanjing during the haze events. Finally, using the potential source contribution function (PSCF) and concentration weighted trajectory (CWT) analysis, we highlighted that the BC at the receptor site was mainly from the local emissions in the surrounding areas of Nanjing.

Specific sources of health risks caused by size-resolved PM-bound metals in a typical coal-burning city of northern China during the winter haze event.

High particulate matter (PM) pollution frequently occurs in winter over northern China , resulting in threats to human health. To date, there are limited studies to link source apportionments and health risk assessments in the different size-resolved PM samples during high PM events. In this study, size-segregated PM samples were collected in Linfen, a typical coal-burning city, in northern China during a wintertime haze pollution. In addition to water-soluble ions and carbon contents, metallic elements in the different size-segregated PM samples were also determined for health risk assessments by inhalation of PM. During the sampling period, the average concentration of PM10 was 274 ±â€¯57 µg m-3 with a major fraction (73%) of organic material and secondary-related aerosols, and an insignificant portion of trace elements (TEs, ~ 3%). The size distribution showed that As and Se, markers of coal combustion, exhibited a mono-modal distribution with a major peak at 0.4-0.7 µm and the others mostly possessed mono-/bi-modal patterns with a major peak at 3.3-5.8 µm. The cancer risk (CR) resulted from PM10 metals by inhalation was estimated to be 2.91 × 10-5 for children and 7.75 × 10-5 for adults while non-cancer risk (NCR) was 2.10 for children and 0.70 for adults. Chromium (Cr) was the dominant species (~89%) of cancer risk in PM10. Road dust was a major fraction (~65%) to total metals in coarse PM (dp > 3.3 µm) whereas coal combustion was a dominant source (~55%) in submicron (dp < 1.1 µm) PM metals. However, traffic emissions (40%) and coal combustion (36%) were the dominant sources of CR since both emissions contributed major fractions (74%) to Cr, especially in submicron PM which exhibited high deposition efficiency of TEs into respiratory tracts, resulting in high CR in Linfen City.

High Time- and Size-Resolved Measurements of PM and Chemical Composition from Coal Combustion: Implications for the EC Formation Process.

Inefficient coal combustion is a significant source of elemental carbon (EC) air pollution in China, but there is a limited understanding of EC's formation processes. In this study, high time-resolved particle number size distributions (PNSDs) and size-resolved chemical compositions were obtained from the combustion of four bituminous coals burned in a quartz tube furnace at 500 and 800 °C. Based on the distinct characteristics of PNSD, the flaming stage was divided into the first-flaming stage (with a PNSD peak at 0.3-0.4 µm) and the second-flaming stage (with a PNSD peak at 0.1-0.15 µm). For the size-segregated EC and OC measurements, more soot-EC was observed in particles larger than 0.3 µm, whereas the smaller ones possessed more char-EC. The results indicated that gas-phase and direct-conversion EC generation mechanisms dominate different burning stages. The analysis of 16 parent PAHs showed more high-molecular-weight PAHs in the second-flaming stage particles, which supports the idea of different formation processes for char-EC and soot-EC. For all four coals, the PNSD and chemical compositions shared a similar trend, confirming that the different formation processes of EC in different flaming stages were common. This study provides novel information concerning EC formation.

Chemical characteristics of dicarboxylic acids and related organic compounds in PM2.5 during biomass-burning and non-biomass-burning seasons at a rural site of Northeast China.

Fine particulate matter (PM2.5) samples were collected using a high-volume air sampler and pre-combusted quartz filters during May 2013 to January 2014 at a background rural site (47∘35 N, 133∘31 E) in Sanjiang Plain, Northeast China. A homologous series of dicarboxylic acids (C2-C11) and related compounds (oxoacids, α-dicarbonyls and fatty acids) were analyzed by using a gas chromatography (GC) and GC-MS method employing a dibutyl ester derivatization technique. Intensively open biomass-burning (BB) episodes during the harvest season in fall were characterized by high mass concentrations of PM2.5, dicarboxylic acids and levoglucosan. During the BB period, mass concentrations of dicarboxylic acids and related compounds were increased by up to >20 times with different factors for different organic compounds (i.e., succinic (C4) acid > oxalic (C2) acid > malonic (C3) acid). High concentrations were also found for their possible precursors such as glyoxylic acid (ωC2), 4-oxobutanoic acid, pyruvic acid, glyoxal, and methylglyoxal as well as fatty acids. Levoglucosan showed strong correlations with carbonaceous aerosols (OC, EC, WSOC) and dicarboxylic acids although such good correlations were not observed during non-biomass-burning seasons. Our results clearly demonstrate biomass burning emissions are very important contributors to dicarboxylic acids and related compounds. The selected ratios (e.g., C3/C4, maleic acid/fumaric acid, C2/ωC2, and C2/levoglucosan) were used as tracers for secondary formation of organic aerosols and their aging process. Our results indicate that organic aerosols from biomass burning in this study are fresh without substantial aging or secondary production. The present chemical characteristics of organic compounds in biomass-burning emissions are very important for better understanding the impacts of biomass burning on the atmosphere aerosols.