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Heterologous spatial distribution of soil polycyclic aromatic hydrocarbons and the primary influencing factors in three industrial parks
2022
Ren, Helong | Su, Peixin | Kang, Wei | Ge, Xiang | Ma, Shengtao | Shen, Guofeng | Chen, Qiang | Yu, Yingxin | An, Taicheng
Soil polycyclic aromatic hydrocarbons (PAHs) generated from industrial processes are highly spatially heterologous, with limited quantitative studies on their main influencing factors. The present study evaluated the soil PAHs in three types of industrial parks (a petrochemical industrial park, a brominated flame retardant manufacturing park, and an e-waste dismantling park) and their surroundings. The total concentrations of 16 PAHs in the parks were 340–2.43 × 10³, 26.2–2.63 × 10³, and 394–2.01 × 10⁴ ng/g, which were significantly higher than those in the surrounding areas by 1–2 orders of magnitude, respectively. The highest soil PAH contamination was observed in the e-waste dismantling park. Nap can be considered as characteristic pollutant in the petrochemical industrial park, while Phe in the flame retardant manufacturing park and e-waste dismantling park. Low molecular weight PAHs (2–3 rings) predominated in the petrochemical industrial park (73.0%) and the surrounding area of brominated flame retardant manufacturing park (80.3%). However, high molecular weight PAHs (4–6 rings) were enriched in the other sampling sites, indicating distinct sources and determinants of soil PAHs. Source apportionment results suggested that PAHs in the parks were mainly derived from the leakage of petroleum products in the petroleum manufacturing process and pyrolysis or combustion of fossil fuels. Contrarily, the PAHs in the surrounding areas could have been derived from the historical coal combustion and traffic emissions. Source emissions, wind direction, and local topography influenced the PAH spatial distributions.
显示更多 [+] 显示较少 [-]Multi-spectroscopic investigation of the molecular weight distribution and copper binding ability of dissolved organic matter in Dongping Lake, China
2022
Fan, Tuantuan | Yao, Xin | Ren, Haoyu | Ma, Feiyang | Liu, Li | Huo, Xiaojia | Lin, Tong | Zhu, Haiyan | Zhang, Yinghao
The properties and metal-binding abilities of dissolved organic matter (DOM) rely on its molecular weight (MW) structure. In this study, the spatial differences of DOM in compositions, MW structures, and binding mechanisms with copper (Cu²⁺) in Dongping Lake were investigated by applying excitation-emission matrix combining parallel factor analysis (EEM-PARAFAC), synchronous fluorescence (SF) spectra, two-dimensional correlation spectra (2D-COS), and Fourier transform infrared (FTIR) spectra. The EDOM for the entrance of the Dawen River and PDOM for the macrophyte-dominated region were divided from DOM of Dongping Lake based on hierarchical clustering analysis (HCA) and principal component analysis (PCA) and were size-fractioned into MW < 500 kDa and <100 kDa fractions. According to EEM-PARAFAC, Dongping Lake was dominated by tryptophan-like substances with MW < 500 kDa. The concentration of PDOM was higher than that of EDOM (p < 0.05). 2D-COS showed that protein-like components preceded humic-like components binding to Cu²⁺ regardless of sample type (215 nm > 285 nm > 310–360 nm). The Cu²⁺ binding capacity of DOM exhibited specific differences in space, components, and molecular weights. The humic-like component 1 (C1) and tryptophan-like component 4 (C4) of PDOM showed stronger binding abilities than those of EDOM. Endogenous tryptophan-like component 4 (C4) had a higher binding affinity for Cu²⁺ than humic-like components (logKₐ: C4 > C1 > C2) in PDOM irrespective of MW. Humic-like components with MW < 500 kDa displayed higher binding potentials for Cu²⁺. FTIR spectra showed that the main participants of DOM-Cu complexation included aromatic hydrocarbons, aliphatic groups, amide Ⅰ bands, and carboxyl functional groups. This study provides spatial-scale insights into the molecular weight structure of DOM in influencing the behavior, fate, and bioavailability of heavy metals in lakes.
显示更多 [+] 显示较少 [-]Race-specific associations of urinary phenols and parabens with adipokines in midlife women: The Study of Women's Health Across the Nation (SWAN)
2022
Lee, Seulbi | Karvonen-Gutierrez, Carrie | Mukherjee, Bhramar | Herman, William H. | Park, Sung Kyun
Adipokines, cytokines secreted by adipose tissue, may contribute to obesity-related metabolic disease. The role of environmental phenols and parabens in racial difference in metabolic disease burden has been suggested, but there is limited evidence. We examined the cross-sectional associations of urinary phenols and parabens with adipokines and effect modification by race. Urinary concentrations of 6 phenols (bisphenol-A, bisphenol-F, 2,4-diclorophenol, 2,5-diclorophenol, triclosan, benzophenone-3) and 4 parabens (methyl-paraben, ethyl-paraben, propyl-paraben, butyl-paraben) were measured in 2002–2003 among 1200 women (mean age = 52.6) enrolled in the Study of Women's Health Across the Nation Multi-Pollutant Study. Serum adipokines included adiponectin, high molecular weight (HMW)-adiponectin, leptin, soluble leptin receptor (sOB-R). Linear regression models were used to estimate the adjusted percentage change in adipokines per inter-quantile range (IQR) increase in standardized and log-transformed levels of individual urinary phenols and parabens. Bayesian kernel machine regression (BKMR) was used to evaluate the joint effect of urinary phenols and parabens as mixtures. Participants included white (52.5%), black (19.3%), and Asian (28.1%) women. Urinary 2,4-dichlorophenol was associated with 6.02% (95% CI: 1.20%, 10.83%) higher HMW-adiponectin and urinary bisphenol-F was associated with 2.60% (0.48%, 4.71%) higher sOB-R. Urinary methyl-paraben was associated with lower leptin in all women but this association differed by race: 8.58% (−13.99%, −3.18%) lower leptin in white women but 11.68% (3.52%, 19.84%) higher leptin in black women (P interaction = 0.001). No significant associations were observed in Asian women. Additionally, we observed a significant positive overall effect of urinary phenols and parabens mixtures in relation to leptin levels in black, but not in white or Asian women. Urinary bisphenol-F, 2,4-dichlorophenol and methyl-paraben may be associated with favorable profiles of adipokines, but methyl-paraben, widely used in hair and personal care products, was associated with unfavorable leptin levels in black women. Future studies are needed to confirm this racial difference.
显示更多 [+] 显示较少 [-]Latitudinal difference in the molecular distributions of lipid compounds in the forest atmosphere in China
2022
Zhang, Donghuan | Ren, Hong | Hu, Wei | Wu, Libin | Ren, Lujie | Deng, Junjun | Zhang, Qiang | Sun, Yele | Wang, Zifa | Kawamura, Kimitaka | Fu, Pingqing
Lipids are important biogenic markers to indicate the sources and chemical process of aerosol particles in the atmosphere. To better understand the influences of biogenic and anthropogenic sources on forest aerosols, total suspended particles (TSP) were collected at Mt. Changbai, Shennongjia, and Xishuangbanna that are located at different climatic zones in northeastern, central and southwestern China. n-Alkanes, fatty acids and n-alcohols were detected in the forest aerosols based on gas chromatography-mass spectrometry. The total concentrations of aliphatic compounds ranged from 15.3 ng m⁻³ to 566 ng m⁻³, and fatty acids were the most abundant (44–95%) followed by n-alkanes and n-alcohols. Low molecular weight- (LFAs) and unsaturated fatty acids (UnFAs) showed diurnal variation with higher concentrations during the nighttime in summer, indicating the potential impact from microbial activities on forest aerosols. The differences of oleic acid (C₁₈:₁) and linoleic acid (C₁₈:₂) concentrations between daytime and nighttime increased at lower latitude, indicating more intense photochemical degradation occurred at lower latitude regions. High levels of n-alkanes during daytime in summer with higher values of carbon preference indexes, combining the strong odd carbon number predominance with a maximum at C₂₇ or C₂₉, implied the high contributions of biogenic sources, e.g., higher plant waxes. In contrast, higher concentrations of low molecular weight n-alkanes were detected in winter forest aerosols. Levoglucosan showed a positive correlation (R² > 0.57) with high- and low molecular weight aliphatic compounds in Mt. Changbai, but such a correlation was not observed in Shennongjia and Xishuangbanna. These results suggest the significant influence of biomass burning in Mt. Changbai, and fossil fuel combustion might be another important anthropogenic source of forest aerosols. This study adds useful information to the current understanding of forest organic aerosols at different geographical locations in China.
显示更多 [+] 显示较少 [-]The relationships between soil physicochemical properties, bacterial communities and polycyclic aromatic hydrocarbon concentrations in soils proximal to coking plants
2022
Du, Jingqi | Liu, Jinxian | Jia, Tong | Chai, Baofeng
Microbial degradation of polycyclic aromatic hydrocarbons (PAHs) is the major channel for their decontamination from different environments. Aerobic and anaerobic biodegradations of PAHs in batch reactors with single or multiple bacterial strains have been intensively studied, but the cooperative mechanism of functional PAH-degrading populations at the community level under field conditions remains to be explored. We determined the composition of PAH-degrading populations in the bacterial community and PAHs in farmland and wasteland soils contaminated by coking plants using high-throughput sequencing and high-performance liquid chromatography (HPLC), respectively. The results indicated that the PAH content of farmland was significantly lower than that of wasteland, which was attributed to the lower content of low molecular weight (LMW) PAHs and benzo [k]fluoranthene. The soil physicochemical properties were significantly different between farmland and wasteland. The naphthalene content was related to the soil organic carbon (SOC) and pH, while phenanthrene was related to the nitrate nitrogen (NO₃⁻-N) and water content (WC). The pH, nitrite (NO₂⁻-N), SOC, NO₃⁻-N and WC were correlated with the content of high molecular weight (HMW) PAHs and total PAHs. The relative abundances of the phyla Actinobacteria, Chloroflexi, Acidobacteria, and Firmicutes and the genera Nocardioides, Bacillus, Lysobacter, Mycobacterium, Streptomyces, and Steroidobacter in farmland soil were higher than those in wasteland soil. The soil physicochemical characteristics of farmland increased the diversities of the PAH degrader and total bacterial communities, which were significantly negatively related to the total PAHs and LMW PAHs. Subsequently, the connectivity and complexity of the network in farmland were lower than those in wasteland, while the module containing a module hub capable of degrading PAHs was identified in the network of farmland soil. Structural equation modelling (SEM) analysis showed that the soil characteristics and optimized abundance and diversity of the bacterial community in farmland were beneficial for the dissipation efficiency of PAHs.
显示更多 [+] 显示较少 [-]Inhibition of methylmercury uptake by freshwater phytoplankton in presence of algae-derived organic matter
2022
Li, Zhike | Chi, Jie | Shao, Bo | Wu, Zhengyu | He, Wei | Liu, Yiwen | Sun, Peizhe | Lin, Huiming | Wang, Xuejun | Zhao, Yingxin | Chen, Long | Tong, Yindong
As the first step of methylmercury (MeHg) entry into the aquatic food webs, MeHg uptake by phytoplankton is crucial in determining the final human MeHg exposure risks. MeHg availability to plankton is regulated by dissolved organic matter (DOM) in the water, while the extent of the impacts can vary largely based on the sources of DOM. Here, we investigated impacts of DOM sources on MeHg bioconcentration by three freshwater phytoplankton species (i.e. S. quadricauda, Chlorella sp., Microcystis elabens) in the laboratory system. We found that algae-derived DOM would prohibited the cellular MeHg bioconcentration by a percent up to 77–93%, while the soil-derived DOM didn't show similar inhibition effects. DOM characterization by the excitation‒emission matrices, Fourier transform infrared spectrum, ultra‒high performance liquid chromatography‒tandem quadrupole time of flight mass spectrometry shown that the molecular size of S-containing compound, rather than thiol concentration, has played a crucial role in regulating the MeHg uptake by phytoplankton. Climate change and increasing nutrient loadings from human activities may affect plankton growth in the freshwater, ultimately changing the DOM compositions. Impacts of these changes on cellular MeHg uptakes by phytoplankton should be emphasized when exploring the aquatic Hg cycling and evaluating their risks to human beings and wild life.
显示更多 [+] 显示较少 [-]Adsorptive removal of propranolol under fixed-bed column using magnetic tyre char: Effects of wastewater effluent organic matter and ball milling
2022
Feizi, Farzaneh | Sarmah, Ajit K. | Rangsivek, Ropru | Gobindlal, Kapish
We investigated the competitive effects of different fractions of wastewater treatment plant effluent organic matter (EfOM) on adsorption of an organic micro pollutant (OMP), propranolol (PRO), in a fixed bed column packed with magnetic tyre char (MTC). The results showed that the presence of EfOM inhibited PRO adsorption in wastewater leading to decreased PRO adsorption capacity from 5.86 to 2.03 mg/g due to competitive effects and pore blockage by smaller EfOM fractions. Characterization of EfOM using size exclusion chromatography (LC-OCD) showed that the principal factor controlling EfOM adsorption was pore size distribution. Low molecular weight neutrals had the highest adsorption onto MTC while humic substances were the least interfering fraction. Effect of important parameters such as contact time, linear velocity and bed height/diameter ratio on MTC performance was studied in large-lab scale columns. Linear velocity and contact time were found to be effective in increasing adsorption capacity of PRO on MTC and delaying breakthrough time. Increase in linear velocity from 0.64 cm/min to 1.29 cm/min increased mass transfer and dispersion, resulting in considerable rise of adsorbed amount (5.86 mg/g to 22.58 mg/g) and increase in breakthrough time (15.8–62.7 h). Efficiency of non-equilibrium Hydrus model considering dispersion and mass transfer mechanism was demonstrated for real wastewater and scale up purposes. Ball milling for degradation of adsorbed PRO and regeneration of MTC resulted in 79% degradation of PRO was achieved after 5 h milling (550 rpm), while the addition of quartz sand increased the efficiency to 92%.
显示更多 [+] 显示较少 [-]Size−resolved source apportionment of particulate matter from a megacity in northern China based on one-year measurement of inorganic and organic components
2021
Tian, Yingze | Harrison, Roy M. | Feng, Yinchang | Shi, Zongbo | Liang, Yongli | Li, Yixuan | Xue, Qianqian | Xu, Jingsha
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.
显示更多 [+] 显示较少 [-]Volatilization of polycyclic aromatic hydrocarbons (PAHs) over the North Pacific and adjacent Arctic Ocean: The impact of offshore oil drilling
2021
Chen, Afeng | Wu, Xiaoguo | Simonich, Staci L Massey | Kang, Hui | Xie, Zhouqing
Air and seawater samples were collected in 2016 over the North Pacific Ocean (NPO) and adjacent Arctic Ocean (AO), and Polycyclic Aromatic Hydrocarbons (PAHs) were quantified in them. Atmospheric concentrations of ∑₁₅ PAHs (gas + particle phase) were 0.44–7.0 ng m⁻³ (mean = 2.3 ng m⁻³), and concentrations of aqueous ∑₁₅ PAHs (dissolved phase) were 0.82–3.7 ng L⁻¹ (mean = 1.9 ng L⁻¹). Decreasing latitudinal trends were observed for atmospheric and aqueous PAHs. Results of diagnostic ratios suggested that gaseous and aqueous PAHs were most likely to be related to the pyrogenic and petrogenic sources, respectively. Three sources, volatilization, coal and fuel oil combustion, and biomass burning, were determined by the PMF model for gaseous PAHs, with percent contributions of 10%, 44%, and 46%, respectively. The 4- ring PAHs underwent net deposition during the cruise, while some 3- ring PAHs were strongly dominated by net volatilization, even in the high latitude Arctic region. Offshore oil/gas production activities might result in the sustained input of low molecular weight 3- ring PAHs to the survey region, and further lead to the volatilization of them. Compared to the gaseous exchange fluxes, fluxes of atmospheric dry deposition and gaseous degradation were negligible. According to the extrapolated results, the gaseous exchange of semivolatile aromatic-like compounds (SALCs) may have a significant influence on the carbon cycling in the low latitude oceans, but not for the high latitude oceans.
显示更多 [+] 显示较少 [-]Simultaneous changes of exogenous dissolved organic matter treated by ozonation in properties and interaction behavior with sulfonamides
2021
Lai, Chaochao | He, Caiwen | Han, Fengxia | Xu, Huayu | Huang, Bin | Dionysiou, Dionysios D. | Pan, Xuejun
Effluent is often treated with ozone before being discharged into a natural water environment. This process will change the interaction between effluent organic matter and pollutants in aquatic environment. The impact of ozonation on complexation between dissolved organic matter in such wastewater and sulfadimidine often found in natural water was studied in laboratory experiments using four types of real wastewater. Ozonation was found to decrease the proportion of organic matter with a molecular weight greater than 5 kDa as well as protein-like, fulvic-like and humic-like components, but except the proportion of hydrophilic components. The aromaticity of the dissolved organic matter was also reduced after ozonation. The complexation of tryptophan and tyrosine with sulfadimidine mainly depends on their hydrophobicity and large molecular weight. Ozonation of fulvic and humic acid tends to produce small and medium molecular weight hydrophilics. The complexation of humic and fulvic acids with sulfadimidine was enhanced by ozonation. Dissolved organic matter, with or without oxidation, were found to weaken sulfadimidine’s inhibition of microbial growth, especially for Aeromonas and Acinetobacter species. This finding will expand our understanding about the impact of advanced treatment processes on the dissolved organic matters’ properties in effluent.
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