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Sorption mechanisms of sulfamethazine to soil humin and its subfractions after sequential treatments
2016
Guo, Xiaoying | Shen, Xiaofang | Zhang, Meng | Zhang, Haiyun | Chen, Weixiao | Wang, Hui | Koelmans, A.A. | Cornelissen, Gerard | Tao, Shu | Wang, Xilong
Sorption mechanisms of an antibiotic sulfamethazine (SMT) to humin (HM) isolated from a peat soil and its subfractions after sequential treatments were examined. The treatments of HM included removal of ash, O-alkyl carbon, lipid, and lignin components. The HF/HCl de-ashing treatment removed a large amount of minerals (mainly silicates), releasing a fraction of hydrophobic carbon sorption domains that previously were blocked, increasing the sorption of SMT by 33.3%. The de-O-alkyl carbon treatment through acid hydrolysis greatly reduced polarity of HM samples, thus weakening the interaction between sorbents with water at the interfaces via H-bonding, leaving more effective sorption sites. Sorption of SMT via mechanisms such as van der Waals forces and π-π interactions was enhanced by factors of 2.04–2.50. After removing the lipid/lignin component with the improved Soxhlet extraction/acid hydrolysis, the organic carbon content-normalized sorption enhancement index Eoc was calculated. The results demonstrated that the Eoc-lipid for SMT (16.9%) was higher than Eoc-lignin (10.1%), implying that removal of unit organic carbon mass of lipid led to a higher increase in sorption strength than that of lignin. As each component was progressively removed from HM, the sorption strength and isotherm nonlinearity of the residual HM samples for SMT were gradually enhanced. The Koc values of SMT by HM samples were positively correlated with their aromatic carbon contents, implying that π-π electron donor-acceptor interactions between the benzene ring of sorbate and the aromatic domains in HM played a significant role in their interactions.
Показать больше [+] Меньше [-]Seasonality in size-segregated ionic composition of ambient particulate pollutants over the Indo-Gangetic Plain: Source apportionment using PMF
2016
Singh, Atinderpal | Rastogi, Neeraj | Patel, Anil | Darashana Siṅgha,
Size-segregated particulate pollutants (PM<0.95, PM0.95–1.5, PM1.5–3.0, PM3.0–7.2 and PM>7.2) were collected over Patiala (30.33°N, 76.40°E; 250 m amsl), a semi-urban city located in northwestern Indo-Gangetic Plain (IGP), during October, 2012 to September, 2013. Mass concentration of total suspended particulates (TSP), derived by summation of particulate (aerosol) mass in different size range, varied from 88 to 387 μg m−3 with highest mass concentration (∼55% of total mass) in submicron size (PM<0.95) during the entire study period, which broadly reflects relative higher contribution of various anthropogenic sources (emissions from biomass and bio-fuel burning, vehicles, thermal power plants, etc) to ambient particles. Concentration of SO42−, NO3−, NH4+, K+ and Ca2+ exhibited large variability ranging from 0.52 to 40, 0.20 to 19, 0.14 to 12, 0.06 to 5.3 and 0.08 to 5.6 μg m−3, respectively, in different size ranges with varying size distribution for most of the species, except NH4+. A strong linear correlation (r = 0.97) between (SO42− + NO3−) and (K+ + NH4+) concentrations has been observed in submicron particles collected in different seasons, suggesting the formation of secondary inorganic salts. However, relatively poor correlation is observed in higher size ranges where significant correlation between (SO42− + NO3−) and (Ca2+ + Mg2+) has been observed. These observations indicate the acid neutralization by dust in coarser modes of particles. Chemical composition of submicron particulates (PM<0.95) in different seasons as well as for whole year was used to identify PM sources through the application of Positive Matrix Factorization (PMF, version 5.0) model. Based on annual data, PMF analyses suggests that six source factors namely biomass burning emission (24%), vehicular emission (22%), secondary organic aerosols (20%), power plant emission (13%), secondary inorganic aerosols (12%) and mineral dust (9%) contribute to PM<0.95 loading over the study region. Such studies are important in dispersion modeling, health impact assessment, and planning of pollution mitigation strategies.
Показать больше [+] Меньше [-]Tracking aquaculture-derived fluoroquinolones in a mangrove wetland, South China
2016
Liu, Xiao | Liu, Yu | Xu, Jian-Rong | Ren, Ke-Jun | Meng, Xiang-Zhou
Aquaculture in mangrove wetlands has been developed rapidly, causing various environmental problems (e.g., antibiotic residue). In the present study, the levels and distributions of a well-known class of antibiotics (fluoroquinolones; FQs), including norfloxacin (NOR), ciprofloxacin (CIP), and enrofloxacin (ENR), were examined in sediment and mangrove plant (Aegiceras corniculatum) from a mangrove wetland in the Zhanjiang Mangrove National Nature Reserve, South China. NOR and CIP were detected in all sediment samples, with concentrations ranging from 4.3 to 64.2 ng/g and from 7.62 to 68.5 ng/g on a basis of dry weight (dw), respectively, whereas ENR was found with relatively lower frequency (<78%) and lower concentrations (<19.3 ng/g). Sediments in mangrove rhizosphere area contained considerably higher concentrations of all FQs (except for ENR). FQs were largely varied in mangrove plant tissues; NOR and ENR were not detected in leaf and root samples, respectively. CIP featured an increasing tendency from the root to the upper parts of plants, whereas a decreasing trend was found for NOR. Three bioconcentration factors (BCFs) of FQs, including BCFs for roots (BCFr), branches (BCFb), and leaves (BCFl) were calculated, and most of them exceeded 1. Especially for NOR, its BCFr can reach up to 9.9, indicating that Aegiceras corniculatum has a strong ability to accumulate FQs from sediment and/or surrounding environment. For NOR and CIP, strong positive relationships were observed between BCFr and concentrations in root, but no significant correlations were observed between BCFr and root lipid of mangrove plant. More studies are needed to investigate the uptake mechanism of antibiotics in mangrove plants.
Показать больше [+] Меньше [-]Shipboard and ground measurements of atmospheric particulate mercury and total mercury in precipitation over the Yellow Sea region
2016
Nguyen, Duc Luong | Kim, Jin Young | Shim, Shang-gyoo | Ghim, Young Sung | Zhang, Xiao-Shan
The first ever shipboard measurements for atmospheric particulate mercury (Hg(p)) over the Yellow Sea and ground measurements for atmospheric Hg(p) and total mercury (THg) in precipitation at the remote sites (Deokjeok and Chengshantou) and the urban sites (Seoul and Ningbo) surrounding the Yellow Sea were carried out during 2007–2008. The Hg(p) regional background concentration of 56.3 ± 55.6 pg m−3 over the Yellow Sea region is much higher than the typical background concentrations of Hg(p) in terrestrial environments (<25 pg m−3) which implies significant impact of anthropogenic mercury emission sources from East Asia. The episodes of highly elevated Hg(p) concentrations at the Korean remote site were influenced through long-range transport from source regions in the Liaoning Province - one of China's most mercury-polluted regions and in the western region of North Korea. Interestingly, wet scavenging of atmospheric Hg(p) is the predominant mechanism regulating concentration of THg in precipitation at the Chinese sites; whereas, wet scavenging of gaseous oxidized mercury (GOM) might play the more important role than that of Hg(p) at the Korean sites. The highest annual wet and dry deposition fluxes of Hg were found at the Ningbo site. The comparison between wet and dry deposition fluxes suggested that dry deposition might play the more important role than wet deposition in Chinese urban areas (source regions); whereas, wet deposition is more important in Korean areas (downwind regions).
Показать больше [+] Меньше [-]Transportation and transformation of mercury in a calcine profile in the Wanshan Mercury Mine, SW China
2016
Yin, Runsheng | Gu, Chunhao | Feng, Xinbin | Zheng, Lirong | Hu, Ningning
Calcination of Hg ores has resulted in serious contamination of mercury (Hg) in the environment. To understand the mobilization of Hg in the calcine pile, the speciation of Hg in a profile of a large calcine pile in the Wanshan Mercury Mine, SW China was investigated using the X-ray absorption spectroscopy (XANES), to understand the mobilization of Hg in the calcine pile. Higher concentrations of Hg were observed at the 30–50 cm depth of the profile, corresponding to a cemented layer. This layer is observed in the entire pile, and was formed due to cementation of calcines. Hg species in calcines include cinnabar (α-HgS), metacinnabar (β-HgS), elemental Hg(0), and minor mercuric chloride (HgCl2), but these Hg species show dramatic changes in the profile. Variations in Hg speciation suggest that extensive mobilization of Hg can occur during weathering processes. We show that the cemented layer can prevent the leaching of Hg and the emission of Hg(0) from the pile. High MeHg concentrations were found near the cemented layer, indicating Hg methylation occurs. This study provides important insights into the environmental risk of Hg in mining areas.
Показать больше [+] Меньше [-]Evergreen or deciduous trees for capturing PAHs from ambient air? A case study
2016
De Nicola, Flavia | Concha Graña, Estefanía | López Mahía, Purificación | Muniategui Lorenzo, Soledad | Prada Rodríguez, Darío | Retuerto, Rubén | Carballeira, Alejo | Aboal, Jesús R. | Fernández, J Ángel
Tree canopies play a key role in the cycling of polycyclic aromatic hydrocarbons (PAHs) in terrestrial ecosystems, as leaves can capture PAHs from the air. In this study, accumulation of PAHs was compared in an evergreen species, P. pinaster, and in a deciduous species, Q. robur, in relation to some physio-morphological characteristics. For this purpose, pine needles and oak leaves collected from different sites across Galicia (NW Spain) were analysed to determine PAH contents, specific leaf area, stomatal density and conductance.Leaves and needles contained similar total amounts of PAHs. The major contribution of particle-bound PAHs in oak (the concentrations of 4- and 5-ring PAHs were two times higher, and those of 6-ring PAHs five times higher in oak than in pine) may be related to the higher specific leaf area (13 and 4 cm2 g−1 dry mass in respectively oak and pine). However, the major contribution of vapor-phase PAHs in pines may be affected by the stomatal conductance (two times higher in pine than in oak). Moreover, an increase in the diameter at breast height of trees led to an increase in accumulation of PAHs, with pine capturing higher amounts of low and medium molecular weight PAHs. The study findings underline the potential role of trees in improving air quality, taking into account the canopy biomass and life cycle.
Показать больше [+] Меньше [-]Depth-resolved microbial community analyses in two contrasting soil cores contaminated by antimony and arsenic
2016
Xiao, Enzong | Krumins, Valdis | Xiao, Tangfu | Dong, Yiran | Tang, Song | Ning, Zengping | Huang, Zhengyu | Sun, Weimin
Investigation of microbial communities of soils contaminated by antimony (Sb) and arsenic (As) is necessary to obtain knowledge for their bioremediation. However, little is known about the depth profiles of microbial community composition and structure in Sb and As contaminated soils. Our previous studies have suggested that historical factors (i.e., soil and sediment) play important roles in governing microbial community structure and composition. Here, we selected two different types of soil (flooded paddy soil versus dry corn field soil) with co-contamination of Sb and As to study interactions between these metalloids, geochemical parameters and the soil microbiota as well as microbial metabolism in response to Sb and As contamination. Comprehensive geochemical analyses and 16S rRNA amplicon sequencing were used to shed light on the interactions of the microbial communities with their environments. A wide diversity of taxonomical groups was present in both soil cores, and many were significantly correlated with geochemical parameters. Canonical correspondence analysis (CCA) and co-occurrence networks further elucidated the impact of geochemical parameters (including Sb and As contamination fractions and sulfate, TOC, Eh, and pH) on vertical distribution of soil microbial communities. Metagenomes predicted from the 16S data using PICRUSt included arsenic metabolism genes such as arsenate reductase (ArsC), arsenite oxidase small subunit (AoxA and AoxB), and arsenite transporter (ArsA and ACR3). In addition, predicted abundances of arsenate reductase (ArsC) and arsenite oxidase (AoxA and AoxB) genes were significantly correlated with Sb contamination fractions, These results suggest potential As biogeochemical cycling in both soil cores and potentially dynamic Sb biogeochemical cycling as well.
Показать больше [+] Меньше [-]Predicting total dissolved solids release from central Appalachian coal mine spoils
2016
Daniels, W. L. | Zipper, C. E. | Orndorff, Z. W. | Skousen, J. | Barton, C. D. | McDonald, L. M. | Beck, M. A.
Appalachian USA surface coal mines face public and regulatory pressure to reduce total dissolved solids (TDS) in discharge waters, primarily due to effects on sensitive macroinvertebrates. Specific conductance (SC) is an accurate surrogate for TDS and relatively low levels of SC (300–500 μS cm−1) have been proposed as regulatory benchmarks for instream water quality. Discharge levels of TDS from regional coal mines are frequently >1000 μS cm−1. The primary objectives of this study were to (a) determine the effect of rock type and weathering status on SC leaching potentials for a wide range of regional mine spoils; (b) to relate leachate SC from laboratory columns to actual measured discharge SC from field sites; and (c) determine effective rapid lab analyses for SC prediction of overburden materials. We correlated laboratory unsaturated column leaching results for 39 overburden materials with a range of static lab parameters such as total-S, saturated paste SC, and neutralization potential. We also compared column data with available field leaching and valley fill discharge SC data. Leachate SC is strongly related to rock type and pre-disturbance weathering. Fine-textured and non-weathered strata generally produced higher SC and pose greater TDS risk. High-S black shales produced the highest leachate SC. Lab columns generated similar range and overall SC decay response to field observations within 5–10 leaching cycles, while actual reduction in SC in the field occurs over years to decades. Initial peak SC can be reliably predicted (R2 > 0.850; p < 0.001) by simple lab saturated paste or 1:2 spoil:water SC procedures, but predictions of longer-term SC levels are less reliable and deserve further study. Overall TDS release risk can be accurately predicted by a combination of rock type + S content, weathering extent, and simple rapid SC lab measurements.
Показать больше [+] Меньше [-]Bioaccumulation and metabolomics responses in oysters Crassostrea hongkongensis impacted by different levels of metal pollution
2016
Cao, Chen | Wang, Wen-Xiong
Jiulong River Estuary, located in southern China, was heavily contaminated by metal pollution. In this study, the estuarine oysters Crassostrea hongkongensis were transplanted to two sites with similar hydrological conditions but different levels of metal pollution in Jiulong River Estuary over a six-month period. We characterized the time-series change of metal bioaccumulation and final metabolomics responses of oysters. Following transplantation, all metals (Cd, Cu, Cr, Ni, Pb, and Zn) in the oyster digestive glands had elevated concentrations over time. By the end of six-month exposure, Cu, Zn and Cd were the main metals significantly differentiating the two sites. Using 1H NMR metabolite approach, we further demonstrated the disturbance in osmotic regulation, energy metabolism, and glycerophospholipid metabolism induced by metal contaminations. Six months later, the oysters transplanted in the two sites showed a similar metabolite variation pattern when compared with the initial oysters regardless of different metal levels in the tissues. Interestingly, by comparing the oysters from two sites, the more severely polluted oysters accumulated significantly higher amounts of osmolytes (betaine and homarine) and lower energy storage compounds (glycogen) than the less polluted oysters; these changes could be the potential biomarkers for different levels of metal pollution. Our study demonstrated the complexity of biological effects under field conditions, and NMR metabolomics provides an important approach to detect sensitive variation of oyster inner status.
Показать больше [+] Меньше [-]An extended study on historical mercury accumulation in lake sediment of Shanghai: The contribution of socioeconomic driver
2016
Yang, Jing | Chen, Ling | Steele, Joshua Caleb | Chen, Rui-Shan | Meng, Xiang-Zhou
Rapid industrialization and urbanization has caused large emission and potential contamination of mercury (Hg) in urban environment. However, little is known about the impact of socioeconomic factor on Hg accumulation in sediment. In the present study, historical record of anthropogenic Hg deposition of Shanghai was reconstructed by using three sediment cores from three park lakes (C1: Luxun Park; C2: Fuxing island Park; C3: Xinjiangwan Park). Meanwhile, the influence of socioeconomic factor to Hg emissions and sedimentary record was calculated based on an extended STIRPAT (stochastic impacts by regression on population, affluence and technology) model. The profiles of Hg levels and fluxes in the three sediment cores showed that Shanghai has recently undergone urbanization. The anthropogenic Hg fluxes exhibited fluctuant increases from ∼1900 to present and accelerated after the establishment of the People’s Republic of China in 1949 and the implementation of reform and opening up policy in 1978. The mean flux ratios of Hg in post-2000 were 2.2, 12, and 2.7 in the C1, C2 and C3 cores, respectively. The extended STIRPAT model was constructed based on strong positive relationships between socioeconomic factors and Hg fluxes, revealing that the proportion of coal consumption, the urbanization rate, and the proportion of heavy industry were the three most important driving factors for Hg accumulations in urban sediment of Shanghai.
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