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The Use of Metal Nanoparticle-Embedded Poly(ethyleneimine) Composite Microgel in the Reduction of Nitrophenols
2015
Demirci, Sahin | Sahiner, Nurettin
Metal nanoparticles such as Ni, Cu, and Co were prepared within polyethyleneimine (PEI) microgels and were used in the reduction of 4-nitrophenol (4-NP) and 2-nitrophenol (2-NP) to 4-aminophenol (4-AP) and 2-aminophenol (2-AP). The metal nanoparticle content of the prepared PEI-M composite catalyst system (M = Co, Ni, and Cu) was increased by multiple loading and reduction cycles into PEI microgels to provide faster and better reduction of 4-NP and 2-NP. The TOF value increased to 1.48 from 0.353 (mol 4-NP (mol catalyst min)⁻¹) for 4-NP reduction catalyzed by PEI-Ni after three cycles of metal loading and reduction. The effect of temperature on 4-NP and 2-NP reductions catalyzed by PEI-M illustrated that higher temperature resulted in very fast reductions, e.g., at 70 °C 4-NP and 2-NP reduction by PEI-Ni resulted in very fast reduction times of 1.2 and 0.67 min to 4-AP and 2-AP, respectively. The activation parameters, such as energy, entropy, and enthalpy, were also calculated and mild activation energies of 38.8 and 46.0 kJ mol⁻¹for 4-NP and 2-NP catalyzed by PEI-Ni were found, respectively, in comparison to similar studies in the literature. Moreover, it was demonstrated that PEI-Ni microgels are reusable five times consecutively, with almost 100 % conversion and 100 % of their catalytic activity.
Afficher plus [+] Moins [-]Identification of Dust Hot Spots from Multi-Resolution Remotely Sensed Data in Eastern China and Mongolia
2015
Zhang, Baolin | Tsunekawa, Atsushi | Tsubo, M. (Mitsuru)
Aeolian dust from hot spots in eastern China and Mongolia can be carried downwind to provinces in China, neighboring countries, the Pacific islands, and cities far beyond the source region. Although dust sources of huge extent have been identified in several countries, few effective countermeasures are available to combat dust emissions in arid regions. We analyzed Moderate Resolution Imaging Spectroradiometer (MODIS) images (1 km spatial resolution) that captured dust emission and dispersion during 2000–2013 to determine dust sources in eastern China and Mongolia. MODIS level 1B data and the brightness temperature difference (BTD) algorithm provided efficient discrimination of dust in this study. The derived dust information, in conjunction with the MODIS land cover product (1 km spatial resolution) and high-resolution Landsat data (30 m spatial resolution; Landsat 8, Operational Land Imager sensor) were used to identify the locations and specific sources of dust. Dust emissions appear to be sporadic in time and space, controlled by both environmental factors and human activity, although past studies have indicated that many dust emissions are from consistently active hot spots. Analysis of MODIS data indicated that three subregions of the eastern China and Mongolia source region are the dominant sources of dust: Horqin Sandy Land, Otintag Sandy Land, and the southeastern Mongolian Gobi; each of these subregions contains dust emission hot spots. We identified the locations of consistent hot spots and verified that some individual dust emissions originated from those hot spots. Our data also indicated that hot spots in southeastern Mongolia have migrated northward since 2006. Our study showed that hot spots such as dry lakes, river beds, mines, and croplands contribute to dust emissions in the eastern China and Mongolia source region. Dust hot spots coincide with regions of expanding industry in Otintag Sandy Land and in some areas of the Mongolian Gobi and with agricultural areas in Horqin Sandy Land and in some parts of the Mongolian Gobi. In Horqin and Otintag sandy lands, dust sources are associated with ephemeral water bodies. Water conservation can be an important countermeasure for initial dust emissions in the Horqin Sandy Land. In the Otintag Sandy Land, attention should be paid to human activities, for example, minimizing the effects of mining disturbances, improving dust suppression in industrial areas, and controlling water use by industry. In Mongolia, protective farming techniques and water conservation in dust emitting basins, and dust suppression and water resource protection in mining zones, must be considered to combat dust emission. MODIS level 1B data can be used to locate dust hot spots and to identify future sources of dust entrainment. Dust hot spots identified from MODIS level 1B data provide small-scale information about dust emission that can be used to locate pollution hot spots, increase understanding of the global dust cycle, and improve dust modeling.
Afficher plus [+] Moins [-]Evaluation of VOC fluxes at the soil-air interface using different flux chambers and a quasi-analytical approach
2015
Cotel, Solenn | Schäfer, Gerhard | Traverse, Sylvie | Marzougui-Jaafar, Salsabil | Gay, Guillaume | Razakarisoa, Olivier
Dense nonaqueous-phase liquids (DNAPLs) spilled on the soil migrate vertically depending upon gravity and capillary forces through the unsaturated zone of the porous aquifer, forming a vapour plume. These volatile organic compounds (VOCs) can be transferred by advection-diffusion to the groundwater or to the atmosphere. Evaluating DNAPL vapour fluxes at the soil-air interface is one of the key challenges in the remediation of contaminated sites. This work discusses the results of a large-scale vapour plume experiment with a well-defined trichloroethylene (TCE) spill, including a sequential raising and lowering of the water table, where the TCE vapour fluxes at the soil surface were experimentally quantified in two ways: (i) directly, with measurements at the soil-air interface using different flux chambers at various operational modes under both transient and steady-state conditions of the vapour plume, and (ii) indirectly, using a quasi-analytical approach based on soil gas measurements. It was shown that upward displacement of the water-air front during the controlled raising of the water table (approximately 10 cm h⁻¹) increased the TCE vapour flux measured at the soil surface by factors of 4 to 10. Under steady-state transport conditions, TCE vapour fluxes measured using five types of flux chambers and three operational modes were similar. The effects of the flux chamber geometry, the accumulation of TCE vapours in the chamber headspace or the air recirculation at a low flow rate on the measured TCE vapour fluxes were low. At steady-state transport conditions, TCE vapour fluxes measured with the flux chambers and estimated using the quasi-analytical approach were of the same order of magnitude. However, under transient conditions of the vapour plume, the TCE vapour flux predicted by the quasi-analytical approach greatly underestimated or overestimated the real TCE vapour flux at the soil-air interface.
Afficher plus [+] Moins [-]Evaluation of Various Inorganic and Biological Extraction Techniques Suitability for Soil Mercury Phytoavailable Fraction Assessment
2015
Hlodák, Michal | Matúš, Peter | Urík, Martin | Kořenková, Lucia | Mikušová, Petra | Senila, Marin | Diviš, Pavel
This article evaluates various extraction techniques’ suitability for soil mercury phytoavailable fraction assessment, including DGT method and extraction with microscopic filamentous fungi metabolites, MgCl₂, rainwater, and EDTA. After mercury extraction from contaminated soils by these techniques, the obtained data were compared to mercury accumulation by shoots of barley (Hordeum vulgare L.). Comparison of these values showed that DGT method is able to separate soil mercury with the best agreement to total mercury concentration in shoots of barley. However, comparing mercury extraction efficiency of selected techniques to extraction efficiency of barley, statistical significance at 0.05 significance level was proved for fungal Cladosporium sp. and Alternaria alternata metabolites. Our results indicate that these extraction techniques are suitable for risk assessment of mercury phytoavailability in contaminated areas.
Afficher plus [+] Moins [-]Enhanced Electrokinetic Transport of Sulfate in Saline Soil
2015
Jo, SungUng | Shin, Yeon-Jun | Yang, Jung-Seok | Moon, Deok Hyun | Koutsospyros, Agamemnon | Baek, Kitae
The electrokinetic transport of sulfate was investigated as a means of treating and restoring a sulfate-accumulating saline soil. The electrokinetic treatment decreased the electrical conductivity of the soil, an indicator of soil salinity, to 58.6, 73.1, and 83.5 % for 7, 14, and 21 days, respectively. More than 96 % of the chloride and nitrate were removed within 7 days. However, the removal of sulfate was highly influenced by the anode material. An iron anode removed sulfate effectively, whereas sulfate was hyper-accumulated in the anodic region when an inert anode was used. The iron anode was oxidized in a sacrificial anodic reaction, which competed with the electrolysis reaction of water at the anode, and finally, the reaction prevented the severe acidification of the soil in the anodic region. However, the competing reactions produced hydrogen ions at the anode and the ions were transported toward the cathode, which, in turn, acidified the soil, especially in the anodic region. The acidification switched the surface charge of the soil from negative to positive, increasing the interaction between the soil surface and sulfate and thus inhibiting the transport of sulfate under the electric field. The zeta potential analysis of the soil provided an explanation. The results indicate that preventing severe acidification is an important factor which influences the transport of anions and iron anode for the enhanced removal of anionic pollutants by electrokinetic remediation.
Afficher plus [+] Moins [-]Arsenic Removal and Transformation by Pseudomonas sp. Strain GE-1-Induced Ferrihydrite: Co-precipitation Versus Adsorption
2015
Xiu, Wei | Guo, Huaming | Liu, Qiong | Liu, Zeyun | Zou, Yan’e | Zhang, Baogang
Hundreds of millions of people are at risk from drinking arsenic (As)-contaminated groundwater in the world, making As removal from aquatic systems of utmost importance. However, characteristics of As removal by bacteria-induced ferrihydrite and coupled with redox processes are still not clear. Two-line ferrihydrite was formed in the presence of aerobic Fe(II)-oxidizing bacterium, Pseudomonas sp. strain GE-1. Arsenic co-precipitation with and adsorption onto ferrihydrite induced by Pseudomonas sp. strain GE-1 and redox processes of As were investigated. Results demonstrated that co-precipitation performed better in As(V) removal than As(III) removal, while adsorption showed higher capacity for As(III) removal. X-ray absorption near-edge spectroscopy (XANES) indicated that As(III) oxidation occurred in solid phases during co-precipitation and adsorption. Detection of As species in solution showed that As(V) was reduced to As(III) during co-precipitation, although no As(V) reduction occurred during adsorption. Arsenic immobilization by Pseudomonas sp. strain GE-1-induced ferrihydrite in the presence of the strains may be applied as an alternative remediation strategy.
Afficher plus [+] Moins [-]Nitrate-Contaminated Water Remediation Supported by Solid Organic Carbon and ZVI-Combined System
2015
Wang, Z. | Wang, Q. | Li, R. H. | Zhang, Z. Q.
Solid organic carbon and zero-valent iron (ZVI) have been used separately as reactive media in permeable reactive barriers (PRBs) to degrade nitrate in groundwater, but few studies have examined the combination of the two materials in one system for nitrate remediation. In the present study, batch tests are conducted to evaluate three common solid organic carbons and their combination with ZVI for nitrate removal from water. The results show that the combined system achieves better denitrification efficiency than that measured with sawdust or cotton alone. However, no obvious difference is noted between the cornstalk alone and its mixture with ZVI treatment. When complete nitrate removal is achieved in the system that combined ZVI with sawdust or cotton, only 72 and 62.6 % of nitrate removal, respectively, are obtained in which the carbon (C) source is used alone. The results indicate that there are synergistic effects in the combined denitrification system, and the effects depend on the type of carbon material used. Sawdust is an alternative carbon source for nitrate removal in a C-ZVI-combined system. In a sawdust-ZVI system, the accumulation of nitrite and ammonium is affected greatly by nitrate concentration, C/N ratio, and Fe/N ratio.
Afficher plus [+] Moins [-]Characterization of Single-Walled Carbon Nanotubes and Adsorption of Perchlorate in Water
2015
Xu, Yongsen | Lou, Jie-Chung | Chou, Ming-Shean | Hsu, Kai-Lin | Han, Jia-Yun
The current study focuses on the removal of perchlorate in water using single-walled carbon nanotubes (SWCNTs) and granular ferric hydroxide as sorbents. The randomly distributed tubes were observed by scanning electron microscopy. The influence of temperature and content of natural humic acid on the perchlorate adsorption capacity was examined at pH 3. The adsorption data were fitted with three models: modified Freundlich, pseudo-first order, and pseudo-second order. The modified Freundlich model produced the best fit to describe the kinetic adsorption processes. The adsorption capacities of perchlorate measured at 25 °C and pH 3 using single-walled carbon nanotubes and granular ferric hydroxide were about 6 and 3 mg/g, respectively. The influence of natural humic acid on perchlorate adsorption by SWCNTs was examined. Natural humic acid was derived from raw water in Gao-Ping River in south Taiwan. Lower adsorption reaction rates of perchlorate were obtained at higher humic acid concentrations. High humic acid concentrations induce the compression of the electric double layer that consequently reduces the surface potential energy and electrostatic repulsion.
Afficher plus [+] Moins [-]Mixed Agricultural Pollutant Mitigation Using Woodchip/Pea Gravel and Woodchip/Zeolite Permeable Reactive Interceptors
2015
Ibrahim, Tristan G. | Goutelle, Alexis | Healy, Mark G. | Brennan, Raymond | Tuohy, Patrick | Humphreys, James | Lanigan, Gary | Brechignac, Jade | Fenton, O. (Owen)
Dairy soiled water (DSW) is water from concreted areas, hard stand areas and holding areas for livestock that has become contaminated by livestock faeces or urine, chemical fertilisers and parlour washings. Losses of DSW occur as point (e.g. storage, pivot irrigators) and diffuse losses (e.g. during or shortly after land application). The concept of a permeable reactive interceptor (PRI), comprising a denitrifying bioreactor woodchip cell to convert nitrate (NO₃⁻) to dinitrogen (N₂) gas and an adsorptive media cell for phosphorus (P) and ammonium (NH₄⁺) mitigation, attempts to simultaneously treat mixed pollutants. This study is the first attempt to test this concept at laboratory-scale. Washing of woodchip media prior to PRI operation produced low NO₃⁻but high NH₄⁺, dissolved reactive P (DRP) and dissolved organic carbon losses. Dairy soiled water was then treated in replicated PRIs containing woodchip in combination with zeolite or gravel compartments. In general, all PRIs were highly efficient at reducing NO₃⁻, NH₄⁺, DRP, dissolved unreactive phosphorus (DUP) and dissolved organic nitrogen (DON) from an influent water replicating DSW. Longitudinal and hydrochemical PRI profiles, as well as zeolite batch experiments, showed that woodchip can both enhance NO₃⁻reduction and adsorb nutrients. Since woodchip is likely to become saturated, it is important to place the reactive media cell further into the sequence of treatment. Even though the majority of the dissolved nutrients were mitigated, the PRIs also emitted greenhouse gases, which would need further remediation sequences.
Afficher plus [+] Moins [-]Fate and Risk Assessment of Arsenic Compounds in Soil Amended with Poultry Litter Under Aerobic and Anaerobic Circumstances
2015
Xie, Haiyun | Han, Deming | Cheng Jinping, | Zhou, Pei | Wang, Wenhua
Poultry litter and bedding materials generated from laying chicken farm often contain high levels of arsenic when roxarsone is included in feed to combat disease and improve egg production. This study was conducted to determine the fate and ecological risk of arsenic species in poultry litter which applied to agricultural field. Three poultry litter application rates (0, 10, 60 % dry weight) were used to amend soil samples under anaerobic and aerobic circumstances, respectively, incubated at 30 % moisture content for 110 days. Experiment indicated that under anaerobic circumstance, As(V) and As(III) decreased in treatments applied 60 and 10 % rates within initial 7 days, subsequently methylated arsenic displayed increasing, suggesting biotic activity transformed inorganoarsenical to methylated arsenic species. In contrast, As(V) dropped in the first 7 days but increased thereafter under aerobic circumstances, with methylated arsenic increasing, implying abiotc and biotic activities enhanced arsenic speciation. Based on different arsenic species, we evaluated their ecological risk in poultry litter respectively. It was found that ecological risks under anaerobic circumstance were higher than under aerobic circumstance of the same poultry litter rates, and higher poultry litter rates applied to soil would bring about higher ecological risk. We suggest that poultry litter should be disposed at low rate (approximately 10 %) and applied to soil surface to create aerobic circumstance for the initial 2 months time, but should be buried into a deeper depth thereafter.
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