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Comparison of arsenic fractions and health risks in PM2.5 before and after coal-gas replacement 全文
2020
Xie, Jiao-Jiao | Yuan, Chun-Gang | Xie, Jin | Niu, Xiao-Dong | Zhang, Xu-Rui | Zhang, Ke-Gang | Xu, Pei-Yao | Ma, Xiao-Ying | Lv, Xiang-Bing
Coal-Gas replacement project has been implemented to decrease haze pollution in China in recent years. Airborne arsenic (As) mostly originates from coal burning processes. It is noteworthy to compare the distribution of arsenic fraction in PM₂.₅ before and after coal-gas replacement. Eighty PM₂.₅ samples were collected in Baoding in December 2016 (coal dominated year) and December 2017 (gas dominated year) at different functional areas including residential area (RA), industrial area (IA), suburb (SB), roadside (ST) and Botanical Garden Park (BG). The fraction, bioavailability and health risk of As in the PM₂.₅ samples were investigated and compared between these two years. Arsenic was mainly distributed in the non-specifically sorbed fraction (F1) and the residual fraction (F5). However, the proportion of F1 to the total As in 2017 was higher than that in 2016, while the proportion of As in the amorphous and poorly-crystalline hydrous oxides of Fe and Al fraction (F3) in 2017 was lower. The distributions of fraction and bioavailability showed temporal and spatial characteristics. The total concentration and bioavailability of As in SB and IA were significantly higher than those in RA, ST and BG. The BF (Bioavailability Factor) values of As ranged from 0.30 to 0.61. Health risk assessment indicated that the hazard quotient (HQ) and carcinogenic risk (CR) of As in PM₂.₅ significantly decreased after coal-gas replacement.
显示更多 [+] 显示较少 [-]Vertical distribution of smoke aerosols over upper Indo-Gangetic Plain 全文
2020
Attenuated backscatter profiles retrieved by the space borne active lidar CALIOP on-board CALIPSO satellite were used to measure the vertical distribution of smoke aerosols and to compare it against the ECMWF planetary boundary layer height (PBLH) over the smoke dominated region of Indo-Gangetic Plain (IGP), South Asia. Initially, the relative abundance of smoke aerosols was investigated considering multiple satellite retrieved aerosol optical properties. Only the upper IGP was selectively considered for CALIPSO retrieval based on prevalence of smoke aerosols. Smoke extinction was found to contribute 2–50% of the total aerosol extinction, with strong seasonal and altitudinal attributes. During winter (DJF), smoke aerosols contribute almost 50% of total aerosol extinction only near to the surface while in post-monsoon (ON) and monsoon (JJAS), relative contribution of smoke aerosols to total extinction was highest at about 8 km height. There was strong diurnal variation in smoke extinction, evident throughout the year, with frequent abundance of smoke particles at lower height (<4 km) during daytime compared to higher height during night (>4 km). Smoke injection height also varied considerably during rice (ON: 0.71 ± 0.65 km) and wheat (AM: 2.34 ± 1.34 km) residue burning period having a significant positive correlation with prevailing PBLH. Partitioning smoke AOD against PBLH into the free troposphere (FT) and boundary layer (BL) yield interesting results. BL contribute 36% (16%) of smoke AOD during daytime (nighttime) and the BL-FT distinction increased particularly at night. There was evidence that despite travelling efficiently to FT, major proportion of smoke AOD (50–80%) continue to remain close to the surface (<3 km) thereby, may have greater implications on regional climate, air quality, smoke transport and AOD-particulate modelling.
显示更多 [+] 显示较少 [-]Light absorption of organic carbon and its sources at a southeastern U.S. location in summer 全文
2019
Xie, Mingjie | Chen, Xi | Holder, Amara L. | Hays, Michael D. | Lewandowski, Michael | Offenberg, John H. | Kleindienst, Tadeusz E. | Jaoui, Mohammed | Hannigan, Michael P.
Light-absorbing organic carbon (OC), also referred to as “brown carbon” (BrC), has been intensively investigated in atmospheres impacted by biomass burning. However, other BrC sources (e.g., secondary formation in the atmosphere) are rarely studied in ambient aerosols. In the current work, forty-five PM₂.₅ filter samples were collected in Research Triangle Park (RTP), NC, USA from June 1st to July 15th, 2013. The bulk carbonaceous components, including OC, elemental carbon (EC), water soluble OC (WSOC), and an array of organic molecular markers were measured; an ultraviolet/visible spectrometer was used to measure the light absorption of methanol extractable OC and WSOC. The average light absorption per OC and WSOC mass of PM₂.₅ samples in summer RTP are 0.36 ± 0.16 m² gC⁻¹ and 0.29 ± 0.13 m² gC⁻¹, respectively, lower than the ambient aerosol samples impacted by biomass burning and/or fossil fuel combustion (0.7–1.6 m² gC⁻¹) from other places. Less than 1% of the aqueous extracts absorption is attributed to the light-absorbing chromophores (nitroaromatic compounds) identified in this work. To identify the major sources of BrC absorption in RTP in the summer, Positive Matrix Factorization (PMF) was applied to a dataset containing optical properties and chemical compositions of carbonaceous components in PM₂.₅. The results suggest that the formation of biogenic secondary organic aerosol (SOA) containing organosulfates is an important BrC source, contributing up to half of the BrC absorption in RTP during the summertime.
显示更多 [+] 显示较少 [-]Biomass burning source identification through molecular markers in cryoconites over the Tibetan Plateau 全文
2019
Li, Quanlian | Wang, Ninglian | Barbante, Carlo | Kang, Shichang | Callegaro, Alice | Battistel, Dario | Argiriadis, Elena | Wan, Xin | Yao, Ping | Pu, Tao | Wu, Xiaobo | Han, Yu | Huai, Yanping
Cryoconite is a dark, dusty aggregate of mineral particles, organic matter, and microorganisms transported by wind and deposited on glacier surfaces. It can accelerate glacier melting and alter glacier mass balances by reducing the surface albedo of glaciers. Biomass burning in the Tibetan Plateau, especially in the glacier cryoconites, is poorly understood. Retene, levoglucosan, mannosan and galactosan can be generated by the local fires or transported from the biomass burning regions over long distances. In the present study, we analyzed these four molecular markers in cryoconites of seven glaciers from the northern to southern Tibetan Plateau. The highest levels of levoglucosan and retene were found in cryoconites of the Yulong Snow Mountain and Tienshan glaciers with 171.4 ± 159.4 ng g⁻¹ and 47.0 ± 10.5 ng g⁻¹ dry weight (d.w.), respectively. The Muztag glacier in the central Tibetan Plateau contained the lowest levels of levoglucosan and retene with mean values of 59.8 ng g⁻¹ and 0.4 ± 0.1 ng g⁻¹ d.w., respectively. In addition, the vegetation changes and the ratios of levoglucosan to mannosan and retene indicate that combustion of conifers significantly contributes to biomass burning of the cryoconites in the Yulong Snow Mountain and Tienshan glacier. Conversely, biomass burning tracers in cryoconites of Dongkemadi, Yuzhufeng, Muztag, Qiyi and Laohugou glaciers are derived from the combustion of different types of biomass including softwood, hardwood and grass.
显示更多 [+] 显示较少 [-]Spatiotemporal distribution, source apportionment and ecological risk assessment of PBDEs and PAHs in the Guanlan River from rapidly urbanizing areas of Shenzhen, China 全文
2019
Liang, Xinxiu | Junaid, Muhammad | Wang, Zhifen | Li, Tianhong | Xu, Nan
In this study, nine congeners of polybrominated diphenyl ethers (PBDEs) and sixteen congeners of polycyclic aromatic hydrocarbons (PAHs) were measured in water samples to elucidate their spatial distribution, congener profiles, sources and ecological risks in the Guanlan River during both the dry season (DS) and the wet season (WS). The concentration of Σ9PBDE ranged from 58.40 to 186.35 ng/L with an average of 115.72 ng/L in the DS, and from 8.20 to 37.80 ng/L with an average of 22.15 ng/L in the WS. Meanwhile, the concentration of Σ16PAHs was ranged from 121.80 to 8371.70 ng/L with an average of 3271.18 ng/L in the DS and from 1.85 to 7124.25 ng/L with an average of 908.11 ng/L in the WS. The concentrations of PBDEs and PAHs in the DS were significantly higher than those in the WS, probably due to the dilution of the river during the rainy season. Moreover, the spatial distribution of pollutants revealed decreasing trend in the concentration from upstream to downstream and almost identical pattern was observed during both seasons. The source apportionment suggested that penta-BDE and to some extent octa-BDE commercial products were major sources of PBDEs in the study area. However, the sources of PAHs were mainly comprised of fossil fuels and biomass burning, followed by the petroleum products and their mixtures. The results of the ecological risk assessment indicated PBDEs contamination posed high ecological risks, while PAHs exhibited low or no ecological risks in the study area. Consistent with the environmental levels, the ecological risks of pollutants were relatively lower in the WS, compared to that in the DS. The results from this study would provide valuable baseline data and technical support for policy makers to protect the ecological environment of the Guanlan River.
显示更多 [+] 显示较少 [-]Baseline investigation on plasticizers, bisphenol A, polycyclic aromatic hydrocarbons and heavy metals in the surface soil of the informal electronic waste recycling workshops and nearby open dumpsites in Indian metropolitan cities 全文
2019
Chakraborty, Paromita | Sampath, Srimurali | Mukhopadhyay, Moitraiyee | Sakthivel, S. | Bharat, Girija K. | Nizzetto, Luca
Electronic waste (e-waste) has emerged as a global environmental problem because of its massive production volume and un-structured management policy. Since the rate of e-waste accumulation is startling and the combinatorial effects of toxicants are complex, we have investigated six phthalic acid esters (PAEs), bis (2-ethylhexyl) adipate (DEHA)), bisphenol A (BPA), sixteen polycyclic aromatic hydrocarbons (PAHs) and eight heavy metals (HMs) in the surface soil of e-waste recycling workshops and nearby open dumpsites in four metropolitan cities of India viz., New Delhi (north), Kolkata (east), Mumbai (west) and Chennai (south). Average concentration of ∑₁₆PAHs (1259 ng/g), ∑₆PAEs (396 ng/g), BPA (140 ng/g) and ∑₈HM (1288 mg/kg) in the informal e-waste recycling sites were higher than ∑₁₆PAHs (1029 ng/g), ∑₆PAEs (93 ng/g), BPA (121 ng/g) and ∑₈HM (675 mg/kg) in dumpsites. Almost 50–90% of BPA, bis (2-ethylhexyl) phthalate (DEHP), ∑₇cₐᵣcPAHs and copper (Cu) were from e-waste sites predominantly from metal recovery sites (EWR). Extensive combustion of e-waste particularly in the EWR sites at New Moore market and Pudupet in Chennai and Wire Lane, Kurla of Mumbai can explain the segregation of diethyl phthalate (DEP), benzyl butyl phthalate (BBP) and carcinogenic PAHs in the first principal component (PC-1). Copper and lead along with highly abundant plasticizers like DEHP, dibutyl phthalate (DBP) and BPA were loaded in PC-2. Combined impact of burning the plastic cables in e-waste and acid leaching process especially at Mandoli in New Delhi might have driven this result. Loading of chrysene, DEHA and low molecular weight (LMW) PAHs mostly in dumpsite soil might have resulted from incomplete combustion of dumped e-waste. Copper was found to exhibit the highest pollution estimated by geo-accumulation index (Igeo). Maximum estimated carcinogenic risk for adults via dermal contact was due to copper, followed by chromium, lead and nickel.
显示更多 [+] 显示较少 [-]Assessment of forest fire impacts on carbonaceous aerosols using complementary molecular marker receptor models at two urban locations in California's San Joaquin Valley 全文
2019
Bae, Min-Suk | Skiles, Matthew J. | Lai, Alexandra M. | Olson, Michael R. | de Foy, Benjamin | Schauer, James J.
Two hundred sixty-three fine particulate matter (PM₂.₅) samples were collected over fourteen months in Fresno and Bakersfield, California. Samples were analyzed for organic carbon (OC), elemental carbon (EC), water soluble organic carbon (WSOC), and 160 organic molecular markers. Chemical Mass Balance (CMB) and Positive Matrix Factorization (PMF) source apportionment models were applied to the results in order to understand monthly and seasonal source contributions to PM₂.₅ OC. Similar source categories were found from the results of the CMB and PMF models to PM₂.₅ OC across the sites. Six source categories with reasonably stable profiles, including biomass burning, mobile, food cooking, two different secondary organic aerosols (SOAs) (i.e., winter and summer), and forest fires were investigated. Both the CMB and the PMF models showed a strong seasonality in contributions of some sources, as well as dependence on wind transport for both sites. The overall relative source contributions to OC were 24% CMB wood smoke, 19% CMB mobile sources, 5% PMF food cooking, 2% CMB vegetative detritus, 17% PMF SOA summer, 22% PMF SOA winter, and 12% PMF forest fire. Back-trajectories using the Weather Research and Forecasting model combined with the FLEXible PARTicle dispersion model (WRF-FLEXPART) were used to further characterize wind transport. Clustering of the trajectories revealed dominant wind patterns associated with varying concentrations of the different source categories. The Comprehensive Air Quality Model with eXtensions (CAMx) was used to simulate aerosol transport from forest fires and thus confirm the impacts of individual fires, such as the Rough Fire, at the measurement sites.
显示更多 [+] 显示较少 [-]Characterization of the chemical components and bioreactivity of fine particulate matter produced during crop-residue burning in China 全文
2019
Chuang, Hsiao-Chi | Sun, Jian | Ni, Haiyan | Tian, Jie | Lui, Ka Hei | Han, Yongming | Cao, Junji | Huang, Ru-Jin | Shen, Zhenxing | Ho, Kin-Fai
Five types of crop residue (rice, wheat, corn, sorghum, and sugarcane) collected from different provinces in China were used to characterize the chemical components and bioreactivity properties of fine particulate matter (PM2.5) emissions during open-burning scenarios. Organic carbon (OC) and elemental carbon (EC) were the most abundant components, contributing 41.7%–54.9% of PM2.5 emissions. The OC/EC ratio ranged from 8.8 to 31.2, indicating that organic matter was the dominant component of emissions. Potassium and chloride were the most abundant components in the portion of PM2.5 composed of water-soluble ions. The coefficient of divergence ranged from 0.27 to 0.51 among various emissions profiles. All samples exposed to a high PM2.5 concentration (150 μg/mL) exhibited a significant reduction in cell viability (A549 lung alveolar epithelial cells) and increase in lactic dehydrogenase (LDH) and interleukin 6 levels compared with those exposed to 20 or 0 μg/mL. Higher bioreactivity (determined according to LDH and interleukin 6 level) was observed for the rice, wheat, and corn samples than for the sorghum straw samples. Pearson's correlation analysis suggested that OC, heavy metals (chromium, manganese, iron, nickel, copper, zinc, tin, and barium), and water-soluble ions (fluoride, calcium, and sulfate) are the components potentially associated with LDH production.
显示更多 [+] 显示较少 [-]Response of aerosol chemistry to clean air action in Beijing, China: Insights from two-year ACSM measurements and model simulations 全文
2019
Zhou, Wei | Gao, Meng | He, Yao | Wang, Qingqing | Xie, Conghui | Xu, Weiqi | Zhao, Jian | Du, Wei | Qiu, Yanmei | Lei, Lu | Fu, Pingqing | Wang, Zifa | Worsnop, Douglas R. | Zhang, Qiang | Sun, Yele
Despite substantial mitigation of particulate matter (PM) pollution during the past decade in Beijing, the response of aerosol chemistry to clean air action and meteorology remains less understood. Here we characterized the changes in aerosol composition as responses to emission reductions by using two-year long-term measurements in 2011/2012 and 2017/2018, and WRF-Chem model. Our results showed substantial decreases for all aerosol species except nitrate from 2011/2012 to 2017/2018. Chloride exhibited the largest decrease by 65–89% followed by organics (37–70%), mainly due to reductions in coal combustion emissions in winter and agriculture burning in June. Primary and secondary organic aerosol (SOA) showed comparable decreases by 61–70% in fall and winter, and 34–63% in spring and summer, suggesting that reductions in primary emissions might also suppress SOA formation. The changes in nitrate were negligible and even showed increases due to less reductions in NOₓ emissions and increased formation potential from N₂O₅ heterogeneous reactions. As a result, nitrate exceeded sulfate and became the major secondary inorganic aerosol species in PM with the contribution increasing from 14–21% to 22–32%. Further analysis indicated that the reductions in aerosol species from 2011/2012 to 2017/2018 were mainly caused by the decreases of severely polluted events (PM₁ > 100 μg m⁻³). WRF-Chem simulations suggested that the decreases in OA and sulfate in fall and winter were mainly resulted from emission reductions (27–36% and 25–43%) and favorable meteorology (4–10% and 19–30%), while they were dominantly contributed by emission changes in spring and summer. Comparatively, the changes in nitrate were mainly associated with meteorological variations while the contributions of emissions changes were relatively small. Our results highlight different chemical responses of aerosol species to emission changes and meteorology, suggesting that future mitigation of air pollution in China needs species-targeted control policy.
显示更多 [+] 显示较少 [-]Perchlorate behavior in the context of black carbon and metal cogeneration following fireworks emission at Oak Lake, Lincoln, Nebraska, USA 全文
2019
Manish Kumar, | Snow, Daniel D. | Li, Yusong | Shea, Patrick J.
The imprints of fireworks displays on the adjacent water body were investigated from the perspective of cogeneration of black carbon, metals and perchlorate (ClO₄⁻). In particular, the mixing and dissipation of ClO₄⁻ were studied at Oak Lake, Lincoln, Nebraska, following fireworks displays in 2015 and 2016. Following the display, ClO₄⁻ concentration in the water increased up to 4.3 μg/L and 4.0 μg/L in 2015 and 2016, respectively. A first-order model generally provided a good fit to the measured perchlorate concentrations from which the rate of dissipation was estimated as 0.07 d⁻¹ in 2015 and 0.43 d⁻¹ in 2016. SEM images show imprints of soot and metal particles in aerosol samples. EDS analysis of the lake sediment confirmed the presence of Si, K, Ca, Zn and Ba, most of which are components of fireworks. The δ¹³C range of −7.55‰ to −9.19‰ in the lake water system closely resembles fire-generated carbon. Cogeneration of black carbon and metal with perchlorate was established, indicating that ClO₄⁻ is an excellent marker of fireworks or a burning event over all other analyzed parameters. Future microcosmic, aggregation and column-based transport studies on black carbon in the presence of perchlorate and metals under different environmental conditions will help in developing transport and fate models for perchlorate and black carbon particles.
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