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Soil aggregate-associated distribution of DDTs and HCHs in farmland and bareland soils in the Danjiangkou Reservoir Area of China
2018
Wang, Li | Xue, Cheng | Zhang, Yushu | Li, Zhiguo | Liu, Zhuang | Pan, Xia | Chen, Fang | Liu, Yi
Soil organic matter (SOM) is the principal aggregating agent for soil aggregation and also the main adsorbent for organochlorine pesticides (OCPs) such as dichlorodiphenyltrichloroethane (DDT) and hexachlorocyclohexane (HCH), which may thereby affect OCP distribution in soils subjected to different land use types. However, the potential effects of land use on SOM and OCP distribution patterns in soil aggregates are not well understood. In this study, soils from farmlands and barelands in the Danjiangkou Reservoir area were analyzed to determine the influence of land use on OCP distribution and composition in different aggregate fractions (>3, 1–3, 0.25–1, and <0.25 mm). The results showed that the levels of ∑DDTs ranged from 9.01 to 27.48 with a mean of 14.40 ng g⁻¹, and ∑HCHs ranged from 2.06 to 4.66 with a mean of 3.19 ng g⁻¹ in farmland soils. In comparison, bareland soils were less contaminated, with total DDTs and HCHs fell in the range of 0.75–5.01 ng g⁻¹ and not detected (n.d.)-1.40 ng g⁻¹ respectively. In regard to the distribution patterns in soil aggregates, the residual levels of ∑DDTs and ∑HCHs tended to a certain degree to enrich in microaggregates (<0.25 mm) relative to bulk soils. A further analysis revealed that the enrichment of ∑DDTs and ∑HCHs in microaggregates were mainly attributed to the accumulation of p,p'-DDE and β-HCH. Moreover, SOM was found also enriched in microaggregates. The enrichment of SOM was significantly and positively correlated with these of ∑DDTs, ∑HCHs, and the dominant metabolites (i.e., DDE and β-HCH) in both land use types. Such results indicated that the variations in behavior of OCPs could be linked to the processes of soil aggregate turnover. These findings may help to enrich the theory of soil OCPs sequestration and establish targeted strategies to mitigate their health risks in the environment.
اظهر المزيد [+] اقل [-]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.
اظهر المزيد [+] اقل [-]Defective magnesium ferrite nano-platelets for the adsorption of As(V): The role of surface hydroxyl groups
2018
Wu, Can | Tu, Jingwei | Tian, Chen | Geng, Junjie | Lin, Zhang | Dang, Zhi
In this work, magnesium ferrite (MgFe₂O₄) nano-platelets with rich defects and abundant surface hydroxyl groups were synthesized, and used for the removal of low concentration As(V) in aqueous solution. Results from scanning electron microscopy (SEM) showed that the as-synthesized MgFe₂O₄ nano-platelets were consisted of many individual nanospheres. Rietveld refinement of X-ray diffraction (XRD) data indicated that the Mg²⁺ ions substituted the Fe³⁺ ions at both the octahedral and the tetrahedral sites of the crystal structure. Batch adsorption experiment showed that the equilibrium concentration of As(V) could be reduced down to 4.9 μg·L⁻¹ when the initial concentration of As(V) is 1 mg·L⁻¹, which complied with the drinking water standard of WHO (10 μg·L⁻¹). The adsorption capacity of synthesized MgFe₂O₄ towards As(V) was higher than commonly used iron oxide adsorbents (Fe₃O₄, γ-Fe₂O₃ and α-Fe₂O₃). Mechanistic studies proved that the superior adsorption capacity was attributed to: (1) increased amount of surface hydroxyl groups that resulted from the surface defects. (2) formation of tridentate hexanuclear surface complexes instead of bidentate binuclear complexes, and (3) formation of excess Mg-OH surface hydroxyl groups and As-Mg monodentate mononuclear surface complexes. This work disclosed the correlation of the superior As(V) adsorption ability with the surface hydroxyl groups in defective MgFe₂O₄, and propose MgFe₂O₄ as a potential candidate for the remediation of As-contaminated water.
اظهر المزيد [+] اقل [-]Abiotic and bioaugmented granular activated carbon for the treatment of 1,4-dioxane-contaminated water
2018
Myers, Michelle A. | Johnson, Nicholas W. | Marin, Erick Zerecero | Pornwongthong, Peerapong | Liu, Yun | Gedalanga, Phillip B. | Mahendra, Shaily
1,4-Dioxane is a probable human carcinogen and an emerging contaminant that has been detected in surface water and groundwater resources. Many conventional water treatment technologies are not effective for the removal of 1,4-dioxane due to its high water solubility and chemical stability. Biological degradation is a potentially low-cost, energy-efficient approach to treat 1,4-dioxane-contaminated waters. Two bacterial strains, Pseudonocardia dioxanivorans CB1190 (CB1190) and Mycobacterium austroafricanum JOB5 (JOB5), have been previously demonstrated to break down 1,4-dioxane through metabolic and co-metabolic pathways, respectively. However, both CB1190 and JOB5 have been primarily studied in laboratory planktonic cultures, while most environmental microbes grow in biofilms on surfaces. Another treatment technology, adsorption, has not historically been considered an effective means of removing 1,4-dioxane due to the contaminant's low Koc and Kow values. We report that the granular activated carbon (GAC), Norit 1240, is an adsorbent with high affinity for 1,4-dioxane as well as physical dimensions conducive to attached bacterial growth. In abiotic batch reactor studies, 1,4-dioxane adsorption was reversible to a large extent. By bioaugmenting GAC with 1,4-dioxane-degrading microbes, the adsorption reversibility was minimized while achieving greater 1,4-dioxane removal when compared with abiotic GAC (95–98% reduction of initial 1,4-dioxane as compared to an 85–89% reduction of initial 1,4-dioxane, respectively). Bacterial attachment and viability was visualized using fluorescence microscopy and confirmed by amplification of taxonomic genes by quantitative polymerase chain reaction (qPCR) and an ATP assay. Filtered samples of industrial wastewater and contaminated groundwater were also tested in the bioaugmented GAC reactors. Both CB1190 and JOB5 demonstrated 1,4-dioxane removal greater than that of the abiotic adsorbent controls. This study suggests that bioaugmented adsorbents could be an effective technology for 1,4-dioxane removal from contaminated water resources.
اظهر المزيد [+] اقل [-]Removal of ciprofloxacin from aqueous solutions by ionic surfactant-modified carbon nanotubes
2018
Li, Haibo | Wu, Wenhao | Hao, Xiangxiang | Wang, Shuai | You, Mengyang | Han, Xiaozeng | Zhao, Qing | Xing, Baoshan
Ionic surfactants may impact removal efficiency of organic contaminants from aqueous solution, but research regarding the adsorption mechanisms on surfactant-modified carbon nanotubes (CNTs) was limited. In this study, three multi-walled and one single-walled CNTs were used as adsorbents to investigate the adsorption behavior and mechanisms of ciprofloxacin (CIP) on CNTs modified by ionic surfactants (cationic CTAB (Cetyltrimethylamnonium bromide) or anionic SDS (Sodium dodecyl sulfate)). More than 80% (82–88%) of the total removed CIP on CTAB-modified CNTs occurred within the first 6 h, much higher than that on SDS-modified CNTs (57–78%). Modeling adsorption kinetics demonstrated that CIP adsorption on surfactant-modified CNTs was controlled by multiple and faster processes, and both external mass transfer and intraparticle diffusion are limiting factors. Relative to SDS, CTAB was significantly (P < 0.001) concentration-dependent in suppressing CIP removal. Besides, the increase in 1/n values of Freundlich model with increasing CTAB concentration suggested that CTAB could be a stronger competitor for CIP adsorption. Hydrophobic interactions predominated zwitterionic CIP adsorption on all CNTs tested, while electrostatic interactions could help control ionizable CIP adsorption on surfactant-modified CNTs depending upon pH. CIP adsorption on modified SWCNTs significantly declined with increasing ionic strength from 1 mM to 100 mM relative to those multi-walled CNTs because the more favorable aggregation of SWCNTs reduced the CIP adsorption, irrespective of which surfactant was added. Significant desorption hysteresis of adsorbed CIP released by SDS and water was observed, but not by CTAB, by which 32.6–54.4% of adsorbed CIP were removed. For SDS-modified CNTs, the mean release ratio (RR) followed an order of MWCNTs (0.075) > MHCNTs (0.058) > SWCNTs (0.057) > MCCNTs (0.049), significantly (P < 0.001) lower than CTAB-CNTs (0.37–0.56). It can be predicted that the tested surfactants co-existing with CNTs depress removal efficiency of diverse contaminants similar to CIP in aqueous systems.
اظهر المزيد [+] اقل [-]Adsorption and regeneration of expanded graphite modified by CTAB-KBr/H3PO4 for marine oil pollution
2018
Xu, Congbin | Jiao, Chunlei | Yao, Ruihua | Lin, Aijun | Jiao, Wentao
The cleaning-up of viscous oil spilled in ocean is a global challenge, especially in Bohai, due to its slow current movement and poor self-purification capacity. Frequent oil-spill accidents not only cause severe and long-term damages to marine ecosystems, but also lead to a great loss of valuable resources. To eliminate the environmental pollution of oil spills, an efficient and environment-friendly oil-recovery approach is necessary. In this study,¹expanded graphite (EG) modified by CTAB-KBr/H₃PO₄ was synthesized via composite intercalation agents of CTAB-KBr and natural flake graphite, followed by the activation of phosphoric acid at low temperature. The resultant modified expanded graphite (M-EG) obtained an interconnected and continuous open microstructure with lower polarity surface, more and larger pores, and increased surface hydrophobicity. Due to these characteristics, M-EG exhibited a superior adsorption capacity towards marine oil. The saturated adsorption capacities of M-EG were as large as 7.44 g/g for engine oil, 6.12 g/g for crude oil, 5.34 g/g for diesel oil and 4.10 g/g for gasoline oil in 120min, exceeding the capacity of pristine EG. Furthermore, M-EG maintained good removal efficiency under different adsorption conditions, such as temperature, oil types, and sodium salt concentration. In addition, oils sorbed into M-EG could be recovered either by a simple compression or filtration-drying treatment with a recovery ratio of 58–83%. However, filtration-drying treatment shows better performance in preserving microstructures of M-EG, which ensures the adsorbents can be recycled several times. High removal capability, fast adsorption efficiency, excellent stability and good recycling performance make M-EG an ideal candidate for treating marine oil pollution in practical application.
اظهر المزيد [+] اقل [-]In-situ examination of graphene and graphene oxide impact on the depuration of phenanthrene and fluoranthene adsorbed onto spinach (Spinacia oleracea L.) leaf surfaces
2018
Sun, Haifeng | Feng, Ruijie | Nan, Yanli | Chen, Zhang | Sang, Nan
To further assess the human being's exposure to polycyclic aromatic hydrocarbons (PAHs) through the dietary pathway, understanding the partitioning of these chemicals co-existed with nanomaterials in edible vegetable systems deserves specific consideration. In this study, the fiber-optic fluorimetry was applied to in situ examine the effects of graphene (GNS) and graphene oxide (GO) nanosheets on the quantification and depuration of three-ringed phenanthrene (Phe) and four-ringed fluoranthene (Fla) adsorbed individually onto the living spinach (Spinacia oleracea L.) surfaces. When the GNS and GO dosages separately increased to the maximum values: a respective red-shift of 4–5 nm and blue-shift of 2–3 nm occurred for the optimal detection emission wavelengths (λem) of the two PAHs, indicating that individual GNS and GO resulted in different changes to the epicuticular wax (ECW) polarity; GNS-inducing fluorescence quenching for the PAHs was about two times greater than GO, owing to the stronger π-π interactions between PAH molecules and GNS relative to GO; the volatilization coefficients (kC1) were reduced by 31.1% versus 26.7% for Phe, and 51.6% versus 34.4% for Fla, mainly via providing an additional adsorbent and promoting the accessibility of the leaf cuticle; respective photolysis coefficients (kP2) of Phe and Fla decreased by 42.9% and 50.0% with GNS, primarily owing to the enhancement of the ECW light-adsorption capacity, but increased by 33.3% and 40.0% with GO due to its photocatalytic activities; overall, total depuration coefficients (kT1, kT2) of the two PAHs decreased by 11.1–55.6%. These findings demonstrate that GNS and GO significantly alter the depuration behavior of PAHs in vegetable systems, potentially posing a threat to the safety of edible vegetables.
اظهر المزيد [+] اقل [-]Selective detection of chloramphenicol based on molecularly imprinted solid-phase extraction in seawater from Jiaozhou Bay, China
2018
Lian, Ziru | Wang, Jiangtao
This study highlights an efficient sample pre-treatment method for preconcentration and detection of chloramphenicol in marine water using molecularly imprinted solid-phase extraction (MISPE). Chloramphenicol molecularly imprinted microspheres were prepared and evaluated on the base of morphology, capacity and selectivity. The imprinted microspheres exhibited specific recognition and high retention capability to chloramphenicol and were applied as special solid-phase extraction adsorbents. An off-line MISPE protocol has been optimized and a creative analytical method coupled to HPLC-DAD was successfully developed for the cleanup and determination of chloramphenicol in seawater samples. Method performance was satisfactory with recoveries ranging from 81 to 90% and relative standard deviation (RSD) was <4.93% (n = 3). Accuracy of the method was assessed at three spiking concentration levels and the limit of detection was 5 ng L⁻¹. Finally, five seawater samples from Jiaozhou Bay of China were determined and the results showed that there was no chloramphenicol detected.
اظهر المزيد [+] اقل [-]Silver@ graphene oxide nanocomposite: synthesize and application in removal of imidacloprid from contaminated waters
2018
Keshvardoostchokami, Mina | Bigverdi, Parastoo | Zamani, Abbasali | Parizanganeh, Abdolhosein | Piri, Farideh
Silver@graphene oxide nanocomposite was synthesized through an efficient approach, characterized by FTIR, EDX, and TEM instruments and then was used as adsorbent for imidacloprid removal from water in batch procedure. Effective variants such as contact time, pH, adsorbent dosage, and initial concentration of imidacloprid on procedure by two methods, one at a time and experimental design methods, were studied. Results in optimum conditions based on one at a time experiments is removal of 63% of the pesticide from 50 mL water containing 10 mg/L of imidacloprid by 0.03 g of the adsorbent at pH = 6.6 after 60 min while, experimental design method predict similarity results, 66% uptake of the poison by 0.06 g of the adsorbent in pH = 8. Kinetics and isotherm for adsorption processes follows Freundlich and pseudo-second-order models. Results confirm that Ag@graphene oxide nanocomposite can be applicable for removal of imidacloprid from real polluted water.
اظهر المزيد [+] اقل [-]Graphene Oxide/Alginate Quasi-Cryogels for Removal of Methylene Blue
2018
Balkız, Gizem | Pingo, Evridiki | Kahya, Nilay | Kaygusuz, Hakan | Bedia Erim, F.
Quasi-cryogelation technique is a simple yet effective technique for improving the adsorptive efficiency of biopolymer-based adsorbent materials. In this work, a biopolymer-based adsorbent material, graphene oxide alginate quasi-cryogel beads are reported. Alginate biopolymer was crosslinked and frozen at − 21 °C in order to obtain a gel with cryogel-like microstructure. Graphene oxide was included in the bead formulation in order to enhance the adsorptive characteristics. Beads were characterized using Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and swelling experiments. Removal of the model cationic dye, methylene blue, was studied by batch adsorption method. It is found that the adsorption follows the Freundlich isotherm model and pseudo-first order kinetics with reaching an adsorption capacity of 122.26 mg/g in 60 min. Results indicate that the physisorption might be due to the π–π interactions between graphene oxide and methylene blue, in addition to electrostatic interactions. Moreover, quasi-cryogelation technique significantly improved the dye removal properties.
اظهر المزيد [+] اقل [-]