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Enhanced adsorption of oxytetracycline to weathered microplastic polystyrene: Kinetics, isotherms and influencing factors
2018
Zhang, Haibo | Wang, Jiaqing | Zhou, Bianying | Zhou, Yang | Dai, Zhenfei | Zhou, Qian | Chriestie, Peter | Luo, Yongming
Microplastic polystyrene foam has been found widely in the environment and is readily transported by wind or water. Beached and virgin foams of size 0.45–1 mm were prepared as sorbents to study oxytetracycline sorption. Enhanced adsorption were found in the beached foams compared to the virgin foams, corresponding to the higher specific surface area, micropore area and the degree of oxidation of the former. The Freundlich Kf value was 894 ± 84 ((mg kg⁻¹) (mg L⁻¹)¹/ⁿ) for oxytetracycline adsorption on the beached foams, approximately twice as high as on the virgin foams. Effects of solution pH on adsorption to the beached foams were more pronounced to the virgin foams. Maximum adsorption occurred at pH 5 at which electrostatic repulsion between the microplastic surface and the oxytetracycline zwitterion was minimal, indicating that electrostatic interaction may have regulated adsorption. Moreover, H-bonding and multivalent cationic bridging mechanisms may also have affected the adsorption of oxytetracycline to the beached foams as reflected by the ionic effects. Adsorption was promoted more in the presence of humic acid than of fulvic acid, perhaps owing to π-π conjugation between the humic acid and the microplastic surface which led to enhanced electrostatic attraction for oxytetracycline. This study suggests that weathered polystyrene foams may act as carriers of antibiotics in the environment and their potential risks to ecosystem and human health merit further investigation.
Show more [+] Less [-]Aging shapes the distribution of copper in soil aggregate size fractions
2018
Li, Qi | Du, Huihui | Chen, Wenli | Hao, Jialong | Huang, Qiaoyun | Cai, Peng | Feng, Xionghan
Soil aggregates are often considered the basic structural elements of soils. Aggregates of different size vary in their ability to retain or transfer heavy metals in the environment. Here, after incubation of a sieved (<2 mm) topsoil with copper, bulk soil was separated into four aggregate-size fractions and their adsorption characteristics for Cu were determined. By combining nano-scale secondary ion mass spectrometry and C-1s Near Edge X-ray Absorption Fine Structure Spectroscopy, we found that copper tends to bind onto organic matter in the <2 μm and 20–63 μm aggregates. Surprisingly, Cu correlated with carboxyl-C in the <2 μm aggregates but with alkyl-C in the 20–63 μm aggregates. This is the first attempt to visualize the spatial distribution of copper in aggregate size fractions. These direct observations can help improve the understanding of interactions between heavy metals and various soil components.
Show more [+] Less [-]Recent advances in layered double hydroxide-based nanomaterials for the removal of radionuclides from aqueous solution
2018
Gu, Pengcheng | Zhang, Sai | Li, Xing | Wang, Xiangxue | Wen, Tao | Jehan, Riffat | Alsaedi, Ahmed | Hayat, Tasawar | Wang, Xiangke
Layered double hydroxides (LDHs), one of the most important two-dimensional layered compounds, have enabled massive developments in effective pollution treatments. Their derivative materials have also attracted multidisciplinary attention owing to the intrinsic advantages of their moderate chemiostability, low cost and nontoxicity. Over the past few decades, significant advances have been made in the synthesis of novel LDH-based composites and the optimization of characterization techniques. In this review, we give an overview of the recent advances in LDH-based nanomaterials, from a brief introduction to their preparation and modification methods to an overview of their application in the removal of radionuclides and an exploration of their underlying adsorption mechanisms. In the end, a summary and outlook are also briefly addressed. This review intends to provide deep insight into the design of high-performance LDH-based materials for the potential elimination of radionuclides from aqueous solutions during environmental pollution cleanup.
Show more [+] Less [-]Selective binding behavior of humic acid removal by aluminum coagulation
2018
Jin, Pengkang | Song, Jina | Yang, Lei | Jin, Xin | Wang, Xiaochang C.
The reactivity characteristics of humic acid (HA) with aluminium coagulants at different pH values was investigated. It revealed that the linear complexation reaction occurred between aluminum and humic acid at pH < 7, and the reaction rate increased as the pH increased from 2 to 6. While at pH = 7, most of the dosed aluminum existed in the form of free aluminum and remained unreacted in the presence of HA until the concentration reached to trigger Al(OH)₃₍ₛ₎ formation. Differentiating the change of functional groups of HA by ¹H nuclear magnetic resonance spectroscopy and X-ray photoelectron spectra analysis, it elucidated that there was a selective complexation between HA and Al with lower Al dosage at pH 5, which was probably due to coordination of the activated functional groups onto aluminium. While almost all components were removed proportionally by sweep adsorption without selectivity at pH 7, as well as that with higher Al dosage at pH 5. This study provided a promising pathway to analyse the mechanism of the interaction between HA and metal coagulants in future.
Show more [+] Less [-]Oral bioaccessibility of silver nanoparticles and ions in natural soils: Importance of soil properties
2018
Dang, Fei | Jiang, Yuanyuan | Li, Min | Zhong, Huan | Peijnenburg, WillieJ.G.M. | Shi, Weilin | Zhou, Dongmei
The abundance of silver nanoparticles (AgNPs) in consumer products has led to their environmental release and therefore to concern about their impact on human health. The ingestion of AgNP-contaminated soil from urban sites is an important exposure pathway, especially for children. Given the limited information on oral bioaccessibility of soil Ag, we used a physiologically based extraction test (PBET) to evaluate the bioaccessibility of AgNPs and AgNO₃ from soil digestion. The AgNPs underwent several biochemical transformations, including their simultaneous dissolution and agglomeration in gastric fluid followed by the disintegration in the intestinal fluid of the agglomerates into NPs containing silver and chlorine. Therefore, Ag-containing soil exposed the intestine to nanoparticulate Ag in forms that were structurally different from the original forms. The bioaccessibility of AgNPs (0.5 ± 0.05%–10.9 ± 0.7%) was significantly lower than that of AgNO₃ (4.7 ± 0.6%–14.4 ± 0.1%), as a result of the lower adsorption of nanoparticles to soil residues during the digestive process. For the soils tested, the bioaccessibility of AgNPs increased with decreasing clay contents and lower pH. By identifying the soil properties that control AgNP bioaccessibility, a more efficient and accurate screening can be performed of soil types that pose the greatest health risk associated with AgNP exposure.
Show more [+] Less [-]Adsorption of perfluoroalkyl substances on microplastics under environmental conditions
2018
Llorca, Marta | Schirinzi, Gabriella | Martinez, Monica | Barceló, Damià | Farré, Marinella
Plastic debris has become an environmental problem during recent years. Among the plastic debris, microplastics (<5 mm; MPLs) imply an extra problem due to their capacity to enter into the fauna through ingestion. In this work, we study the capacity of three MPLs, that include high-density polyethylene (HDPE), polystyrene (PS) and polystyrene carboxylate (PS-COOH), to sorb 18 perfluoroalkyl substances (PFASs; including carboxylic acids, sulphonates and one sulphonamide) from the surrounding waters (freshwater and seawater).Conclusions drawn from the results are that perfluoro sulphonates and sulphonamides have more tendency to be sorbed onto MPLs. In addition, PS and PS-COOH have more affinity for PFASs than HDPE. Finally, the increment of conductivity and pH of the water decreases the exposure time that is necessary to reach equilibrium. However, the presence of salts decreases the tendency of PFASs to be sorbed onto plastic surfaces. These results highlight the problem associated with the presence of MPLs in inland and marine waters since toxic compounds can be sorbed onto surrounding plastics that could be ingested by aquatic fauna.
Show more [+] Less [-]Multiwall carbon nanotubes modulate paraquat toxicity in Arabidopsis thaliana
2018
Fan, Xiaoji | Chui, Kawai | Lavoie, Michel | Peijnenburg, W.J.G.M. | Zhu, Youchao | Lu, Tao | Fu, Zhengwei | Zhu, Tingheng | Qian, Haifeng
Carbon nanotubes can be either toxic or beneficial to plant growth and can also modulate toxicity of organic contaminants through surface sorption. The complex interacting toxic effects of carbon nanotubes and organic contaminants in plants have received little attention in the literature to date. In this study, the toxicity of multiwall carbon nanotubes (MWCNT, 50 mg/L) and paraquat (MV, 0.82 mg/L), separately or in combination, were evaluated at the physiological and the proteomic level in Arabidopsis thaliana for 7–14 days. The results revealed that the exposure to MWCNT had no inhibitory effect on the growth of shoots and leaves. Rather, MWCNT stimulated the relative electron transport rate and the effective photochemical quantum yield of PSII value as compared to the control by around 12% and lateral root production up to nearly 4-fold as compared to the control. The protective effect of MWCNT on MV toxicity on the root surface area could be quantitatively explained by the extent of MV adsorption on MWCNT and was related to stimulation of photosynthesis, antioxidant protection and number and area of lateral roots which in turn helped nutrient assimilation. The influence of MWCNT and MV on photosynthesis and oxidative stress at the physiological level was consistent with the proteomics analysis, with various over-expressed photosynthesis-related proteins (by more than 2 folds) and various under-expressed oxidative stress related proteins (by about 2–3 folds). This study brings new insights into the interactive effects of two xenobiotics (MWCNT and MV) on the physiology of a model plant.
Show more [+] Less [-]Emission characteristics for gaseous- and size-segregated particulate PAHs in coal combustion flue gas from circulating fluidized bed (CFB) boiler
2018
Wang, Ruwei | Liu, Guijian | Sun, Ruoyu | Yousaf, Balal | Wang, Jizhong | Liu, Rongqiong | Zhang, Hong
The partitioning behavior of polycyclic aromatic hydrocarbons (PAHs) between gaseous and particulate phases from coal-fired power plants (CFPPs) is critically important to predict PAH removal by dust control devices. In this study, 16 US-EPA priority PAHs in gaseous and size-segregated particulate phases at the inlet and outlet of the fabric filter unit (FFs) of a circulating fluidized bed (CFB) boiler were analyzed. The partitioning mechanisms of PAHs between gaseous and particulate phases and in particles of different size classes were investigated. We found that the removal efficiencies of PAHs are 45.59% and 70.67–89.06% for gaseous and particulate phases, respectively. The gaseous phase mainly contains low molecular weight (LMW) PAHs (2- and 3-ring PAHs), which is quite different from the particulate phase that mainly contains medium and high molecular weight (MMW and HMW) PAHs (4- to 6-ring PAHs). The fractions of LMW PAHs show a declining trend with the decrease of particle size. The gas-particle partitioning of PAHs is primarily controlled by organic carbon absorption, in addition, it has a clear dependence on the particle sizes. Plot of log (TPAH/PM) against logDp shows that all slope values were below −1, suggesting that PAHs were mainly adsorbed to particulates. The adsorption effect of PAHs in size-segregated PMs for HMW PAHs is more evident than LMW PAHs. The particle size distributions (PSDs) of individual PAHs show that most of PAHs exhibit bi-model structures, with one mode peaking in the accumulation size range (2.1–1.1 μm) and another mode peaking in coarse size range (5.8–4.7 μm). The intensities of these two peaks vary in function of ring number of PAHs, which is likely attributed to Kelvin effect that the less volatile HMW PAH species preferentially condense onto the finer particulates. The emission factor of PAHs was calculated as 3.53 mg/kg of coal burned, with overall mean EFPAH of 0.55 and 2.98 mg/kg for gaseous and particulate phase, respectively. Moreover, the average emission amount of PAHs for the investigated CFPP was 1016.6 g/day and 371073.6 g/y, respectively.
Show more [+] Less [-]Correlations and adsorption mechanisms of aromatic compounds on biochars produced from various biomass at 700 °C
2018
Yang, Kun | Jiang, Yuan | Yang, Jingjing | Lin, Daohui
Knowledge of adsorption behavior of organic contaminants on high heat temperature treated biochars is essential for application of biochars as adsorbents in wastewater treatment and soil remediation. In this study, isotherms of 25 aromatic compounds adsorption on biochars pyrolyzed at 700 °C from biomass including wood chips, rice straw, bamboo chips, cellulose, lignin and chitin were investigated to establish correlations between adsorption behavior and physicochemical properties of biochars. Isotherms were well fitted by Polanyi theory-based Dubinin-Ashtakhov (DA) model with three parameters, i.e., adsorption capacity (Q⁰) and adsorption affinity (E and b). Besides the negative correlation of Q⁰ with molecular maximum cross-sectional areas (σ) of organic compounds, positive correlations of Q⁰ with total pore volume (Vₜₒₜₐₗ) and average diameter of micropore (D) of biochars were observed, indicating that adsorption by biochars is captured by the pore-filling mechanism with molecular sieving effect in biochar pores. Linear solvation energy relationships (LSERs) of adsorption affinity (E) with solvatochromic parameters of organic compounds (i. e., αₘ and π∗) were established, suggesting that hydrophobic effect, π-π interaction and hydrogen-bonding interaction are the main forces responsible for adsorption. The regression coefficient (π₁) and intercept (C) of obtained LSERs are correlated with biochar H/C and Rₘᵢcᵣₒ, respectively, implying that biochars with higher aromaticity and more micropores have stronger π-π bonding potential and hydrophobic effect potential with aromatic molecule, respectively. However, hydrogen-bonding potential of biochars for organic molecules is not changed significantly with properties of biochars. A negative correlation of b with biochar H/C is also obtained. These correlations could be used to predict the adsorption behavior of organic compounds on high heat temperature treated biochars from various biomass for the application of biochars as sorbents and for the estimating of environmental risks of organic compounds in the present of biochars.
Show more [+] Less [-]Diverse mechanisms drive fluoride enrichment in groundwater in two neighboring sites in northern China
2018
Li, Danni | Gao, Xubo | Wang, Yanxin | Luo, Wenting
Excessive amounts of fluoride in drinking groundwater are harmful to human health, but the mechanisms responsible for fluoride enrichment in groundwater are not fully understood. Samples from two neighboring areas with endemic fluorosis were collected to test the hypothesis that there are distinctly different mechanisms responsible for the enrichment of fluoride in these groundwater. Hydrochemistry, stable isotopes and geochemical simulation were conducted together to investigate the fluoride spatial distribution and the diversity of responsible mechanisms. Our results showed that the spatial distributions of fluoride are different: I) high [F] in fresh shallow groundwater (SGQJ) and II) medium [F] in fresh to brackish deep groundwater (DGQJ) in the Qiji area; and III) medium [F] in brackish shallow groundwater (SGYH) and IV) low [F] in fresh deep groundwater (DGYH) in the Yanhu area. We also found that the fluoride concentration in groundwater is primarily controlled by the dissolution equilibrium of fluorite, as suggested by the correlation between [F] and [Ca]. However, there are other significant mechanisms: 1) for SGQJ, fluoride-bearing minerals (such as fluorite) dissolution, along with moderate evaporation, cation exchange and the more alkaline conditions are the driving factors; 2) for SGYH, the contributing factors are strong evaporation, the salt effect, dissolution of evaporites, gypsum and dolomite, bicarbonate-fluoride competition and anthropogenic activity; 3) for DGQJ, cation exchange, alkaline conditions and competitive adsorption are major factors; and 4) dolomite dissolution promotes the [F] increase in DGYH. Our findings suggest that the hydrogeochemical conditions play key roles in the enrichment of fluoride and that caution should be taken in the future when evaluating fluoride occurrence in groundwater, even in nearby areas.
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