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Organophosphorus flame retardants and plasticizers in the aquatic environment: A case study of the Elbe River, Germany
2015
Wolschke, Hendrik | Sühring, Roxana | Xie, Zhiyong | Ebinghaus, Ralf
This study reports the occurrence and distribution of organophosphorus flame retardants and plasticizers (OPEs) in the Elbe and Rhine rivers. A special focus of this investigation concerns the potential impacts of a major flood event in 2013 on the OPE patterns and levels in the Elbe River. In this river, 6 of 13 OPEs were detected, with tris-ethyl-phosphate (TEP, 168 ± 44 ng/L), tris-1,3-dichloro-2-propyl-phosphate (TDCPP, 155 ± 14 ng/L) and tris-1-chloro-2-propyl phosphate (TCPP, 126 ± 14 ng/L) identified as the dominant compounds. Relative to previous studies, an increase in the concentrations and relative contributions of TDCPP to the total level of OPEs was observed, which was likely caused by its increased use as a replacement for the technical pentaBDE formulation. During the flood event, the concentrations of OPEs were similar to the normal situation, but the mass fluxes increased by a factor of approximately ten (∼16 kg/d normal versus ∼160 kg/d flood peak). No input hotspots were identified along the transects of the Elbe and Rhine rivers, and the mass flux of OPEs appeared to be driven by water discharge.
Show more [+] Less [-]An assessment of the transport of southern California stormwater ocean discharges
2015
Rogowski, Peter A. | Terrill, Eric | Schiff, Kenneth | Kim, Sŭng-yŏng
The dominant source of coastal pollution adversely affecting the regional coastal water quality is the seasonally variable urban runoff discharged via southern California’s rivers. Here, we use a surface transport model of coastal circulation driven by current maps from high frequency radar to compute two-year hindcasts to assess the temporal and spatial statistics of 20 southern California stormwater discharges. These models provide a quantitative, statistical measure of the spatial extent of the discharge plumes in the coastal receiving waters, defined here as a discharge’s “exposure”. We use these exposure maps from this synthesis effort to (1) assess the probability of stormwater connectivity to nearby Marine Protected Areas, and (2) develop a methodology to estimate the mass transport of stormwater discharges. The results of the spatial and temporal analysis are found to be relevant to the hindcast assessment of coastal discharges and for use in forecasting transport of southern California discharges.
Show more [+] Less [-]Adsorption of Natural Organic Matter onto the Products of Water-Pipe Corrosion
2015
Świetlik, Joanna | Laskowski, Tomasz | Kozyatnyk, Ivan
Natural organic matter (NOM) interaction with corrosion sediments is important because it can adversely affect the behaviour of many organic and inorganic pollutants in drinking water distribution systems. NOM accumulation onto corrosion sediments can cause serious problems for water supply, such as bacteria regrowth and deterioration of water quality. Corrosion sediments have different structures from the well-known iron oxides. The interaction among corrosion sediments and water organic matter can also differ. The main goal of this work was to understand the adsorption mechanism of the processes of NOM interaction with corrosion sediments. Fulvic acid (FA) isotherms on corrosion sediments in logarithmic coordinates of the Freundlich equation have different segments with different slopes, representing the non-adsorbed and adsorbed conditional component of the FA. The formation of structures with a molecular weight higher than the initial FA was observed. FA adsorption on corrosion sediments depends on time. Almost 60–70 % of the FA was removed during the first 10 min of contact. Such rapid adsorption indicates that FA was accumulated onto corrosion sediments mainly due to physical-chemical interaction. The pseudo-second-order kinetics model was demonstrated to better describe the adsorption of FA onto corrosion sediments than the pseudo-first-order model. External mass transfer is the limiting stage of the process of FA adsorption onto corrosion sediments. This knowledge is useful for understanding of corrosion processes and biological regrowth in water supply pipes and thus further decrease of drinking water quality.
Show more [+] Less [-]Removal of Phosphate from Aqueous Solutions by Chemical- and Thermal-Modified Bentonite Clay
2015
Tanyol, Mehtap | Yonten, Vahap | Demir, Veysel
The study investigated phosphate adsorption from aqueous solutions using chemical- and thermal-modified bentonite in batch system. The adsorbent was characterized by SEM, BET, and FTIR spectroscopy. Contact time, beginning phosphate concentration, pH of the solution, and the effects of the temperature on phosphate adsorption capacity were determined by a series of experimental studies. In a wide pH range (3–10), high phosphate removal yields were obtained (between 94.23 and 92.26 %), and with the increase in temperature (from 25 to 45 °C), phosphate removal increased. Langmuir and Freundlich isotherms were used to determine the sorption equilibrium, and the results demonstrated that equilibrium data displayed better adjustment to Langmuir isotherm than the Freundlich isotherm. Phosphate sorption capacity, calculated using Langmuir equation, is 20.37 mg g⁻¹ at 45 °C temperature and pH 3. Mass transfer and kinetic models were applied to empirical findings to determine the mechanism of adsorption and the potential steps that control the reaction rate. Both external mass transfer and intra-particle diffusion played a significant role on the adsorption mechanism of phosphate, and adsorption kinetics followed the pseudo-second-order-type kinetic. Furthermore, thermodynamic parameters (ΔH°, ΔG°, ΔS°) which reveal that phosphate adsorption occur spontaneously and in endothermic nature were determined. The results of this study support that bentonite, which is found abundant in nature and modified as an inexpensive and effective adsorbent, could be used for phosphate removal from aqueous solutions.
Show more [+] Less [-]Enhanced Adsorptive Removal of Methylene Blue from Aqueous Solution by Alkali-Activated Palygorskite
2015
Wang, Wenbo | Wang, Fangfang | Kang, Yuru | Wang, Aiqin
Silicate clay materials are promising natural adsorbents with abundant, low cost, stable, and eco-friendly advantages, but the limited adsorption capacity restricts their applications in many fields. Herein, palygorskite (PAL) was facilely activated with alkali to enhance its adsorptive removal capability for methylene blue (MB). The effects of alkali activation on the microstructure, physicochemical, and adsorption properties of PAL for MB were intensively investigated. It was found that the moderate alkali activation can partially remove the metal cations (i.e., Al³⁺, Mg²⁺) and Si in the crystal backbone of PAL by which new “adsorption sites” were created and the surface negative charges increased. The adsorption capacity and rate of PAL for MB were evidently enhanced due to the effective activation. The adsorption isotherms were described by Freundlich isotherm model very well, and the adsorption kinetics can be accurately presented by a pseudo-second-order model. It can be inferred from the fitting results that the overall adsorption process was controlled by external mass transfer and intra-particle diffusion (the dominant role). The multiple adsorption interactions (hydrogen bonding, electrostatic interactions, mesopore filling, and complexing) were turned out to be the dominant factors to improve the adsorption properties. It was revealed that the activated PAL could be used as a potential adsorption candidate for environmental applications.
Show more [+] Less [-]Sorption behavior and modeling of endocrine-disrupting chemicals on natural sediments: role of biofilm covered on surface
2015
The surfaces of natural sediments are ubiquitously coated by biofilms that increase the content of organic matter in sediments. However, it is less understood whether the biofilms act as a sorbent or a barrier of mass transfer from water column to sediment phase. This study focused on the role of biofilms coverage on sediments in the sorption of bisphenol A (BPA), 17α-ethinyl estradiol (EE2), and 4-nonylphenols (4-NP) as model compounds for endocrine-disrupting chemicals (EDCs). The OC-normalized distribution coefficients (kOC) for BPA, EE2 and 4-NP ranged from 10¹.⁸⁷to 10³.⁰⁹ l/kg, the kOCof EE2 was slightly higher (10².²³ l/kg) for sediment after H₂O₂oxidation than before (10¹.⁹³ l/kg). A two-stage model with a fast section and slow section was employed to describe the sorption process (r² > 0.95). The model results showed that the fast sorption section played a main role in the sorption process, while the slow section determined the extent of the reaction (the second-phase partition coefficient (kₚ₂) ranged from 11.7 to 118.9 l/kg). The ratios of the mass transfer rate constant of the two stages for the natural sediment ranged from 6.0 to 7.2, which were somewhat lower than those for soil samples. These results indicated that the biofilm coverage on sediment may act as a barrier in mass transfer from water to sediment and scarcely increased the sorption capacity of sediments.
Show more [+] Less [-]Using live algae at the anode of a microbial fuel cell to generate electricity
2015
Xu, Chang | Poon, Karen | Choi, Martin M. F. | Wang, Ruihua
Live green microalgae Chlorella pyrenoidosa was introduced in the anode of a microbial fuel cell (MFC) to act as an electron donor. By controlling the oxygen content, light intensity, and algal cell density at the anode, microalgae would generate electricity without requiring externally added substrates. Two models of algal microbial fuel cells (MFCs) were constructed with graphite/carbon electrodes and no mediator. Model 1 algal MFC has live microalgae grown at the anode and potassium ferricyanide at the cathode, while model 2 algal MFC had live microalgae in both the anode and cathode in different growth conditions. Results indicated that a higher current produced in model 1 algal MFC was obtained at low light intensity of 2500 lx and algal cell density of 5 × 10⁶ cells/ml, in which high algal density would limit the electricity generation, probably by increasing oxygen level and mass transfer problem. The maximum power density per unit anode volume obtained in model 1 algal MFC was relatively high at 6030 mW/m², while the maximum power density at 30.15 mW/m² was comparable with that of previous reported bacteria-driven MFC with graphite/carbon electrodes. A much smaller power density at 2.5 mW/m² was observed in model 2 algal MFC. Increasing the algal cell permeability by 4-nitroaniline would increase the open circuit voltage, while the mitochondrial acting and proton leak promoting agents resveratrol and 2,4-dinitrophenol would increase the electric current production in algal MFC.
Show more [+] Less [-]Feasibility of treating aged polycyclic aromatic hydrocarbons (PAHs)-contaminated soils using ethyl lactate-based Fenton treatment via parametric and kinetic studies
2015
Yap, Chiew Lin | Gan, Suyin | Ng, Hoon Kiat
This study focuses on the feasibility of treating aged polycyclic aromatic hydrocarbons (PAHs)-contaminated soils using ethyl lactate (EL)-based Fenton treatment via a combination of parametric and kinetic studies. An optimised operating condition was observed at 66.7 M H₂O₂ with H₂O₂/Fe²⁺ of 40:1 for low soil organic carbon (SOC) content and mildly acidic soil (pH 6.2), and 10:1 for high SOC and very acidic soil (pH 4.4) with no soil pH adjustment. The desorption kinetic was only mildly shifted from single equilibrium to dual equilibrium of the first-order kinetic model upon ageing. Pretreatment with EL f c = 0.60 greatly reduced the mass transfer coefficient especially for the slow desorbed fraction (k ₛₗₒw) of high molecular weight (HMW) PAHs, largely contributed by the concentration gradient created by EL-enhanced solubility. As the major desorption obstacle was almost fully overcome by the pretreatment, the pseudo-first-order kinetic reaction rate constant of PAHs degradation of aged soils was statistically discernible from that of freshly contaminated soils but slightly reduced in high SOC and high acidity soil. Stabilisation of H₂O₂ by EL addition in combination with reduced Fe²⁺ catalyst were able to slow the decomposition rate of H₂O₂ even at higher soil pH.
Show more [+] Less [-]Solar photocatalytic gas-phase degradation of n-decane—a comparative study using cellulose acetate monoliths coated with P25 or sol-gel TiO2 films
2015
Miranda, Sandra M. | Lopes, Filipe V. S. | Rodrigues-Silva, Caio | Martins, Susana D. S. | Silva, Adrián M. T. | Faria, Joaquim L. | Boaventura, Rui A. R. | Vilar, Vítor J. P.
Cellulose acetate monoliths (CAM) were used as the substrate for the deposition of TiO₂films to produce honeycombed photoactive structures to fill a tubular photoreactor equipped with a compound parabolic collector. By using such a setup, an efficient single-pass gas-phase conversion was achieved in the degradation of n-decane, a model volatile organic compound. The CAM three-dimensional, gas-permeable transparent structure with a rugged surface enables a good adhesion of the catalytic coating. It also provides a rigid structure for packing the tubular photoreactor, and maximizing the illuminated catalyst surface. The efficiency of the photocatalytic oxidation (PCO) process on n-decane degradation was evaluated under different operating conditions, such as feeding concentration (73 and 146 ppm), gas stream flow rate (73, 150, and 300 mL min⁻¹), relative humidity (3 and 25 %), and UV irradiance (18.9, 29.1, and 38.4 WUVm⁻²). The results show that n-decane degradation by neat photolysis is negligible, but mineralization efficiencies of 86 and 82 % were achieved with P25-CAM and SG-CAM, respectively, for parent pollutant conversions above 95 %, under steady-state conditions. A mass transfer model, considering the mass balance to the plug-flow packed photoreactor, and PCO reaction given by a Langmuir-Hinshelwood bimolecular non-competitive two types of sites equation, was able to predict well the PCO kinetics under steady-state conditions, considering all the operational parameters tested. Overall, the performance of P25-CAM was superior taking into account mineralization efficiency, cost of preparation, surface roughness, and robustness of the deposited film.
Show more [+] Less [-]Enhanced adsorptive removal of selected pharmaceutical antibiotics from aqueous solution by activated graphene
2015
Yu, Fei | Ma, Jie | Bi, Dongsu
Activated graphene adsorbents (G-KOH) were synthesized by a one-step alkali-activated method, with a high specific surface area (SSA) and a large number of micropores. As a result, the SSA of the final product greatly increases to ∼512.6 m²/g from ∼138.20 m²/g. The resulting G-KOH was used firstly as an adsorbent for the removal of ciprofloxacin (CIP) in aqueous solutions. Experimental results indicated that G-KOH has excellent adsorption capacity (∼194.6 mg/g). The alkali-activation treatment introduced oxygen-containing functional groups on the surface of G-KOH, which would be beneficial to improving the adsorption affinity of G-KOH for the removal of CIP. Kinetic regression results showed that the adsorption kinetic was more accurately represented by a pseudo-second-order model. The overall adsorption process was jointly controlled by external mass transfer and intra-particle diffusion, and intra-particle diffusion played a dominant role. A Langmuir isotherm model showed a better fit with adsorption data than a Freundlich isotherm model for the adsorption of CIP on G-KOH. The remarkable adsorption capacity of CIP onto G-KOH can be attributed to the multiple adsorption interaction mechanisms (hydrogen bonding, π–π electron donor–acceptor interactions, and electrostatic interactions). Results of this work are of great significance for environmental applications of activated graphene with higher SSA as a promising adsorbent for organic pollutants from aqueous solutions.
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