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Sorption of apolar and polar organic contaminants by waste tire rubber and its chars in single- and bi-solute systems
2011
Lian, Fei | Huang, Fang | Chen, Wei | Xing, Baoshan | Zhu, Lingyan
Single- and bi-solute sorption of organic compounds [1,3-dichlorbenzene (DCB), 1,3-dinitrobenzene (DNB) and 2,4-dichlorophenol (DCP)] on ground tire rubber and its chars was studied. The chars were prepared by pyrolyzing tire rubber at different temperatures (200–800 °C). Their surface area, aromaticity and hydrophobicity increase greatly with pyrolytic temperature, and the polymeric phase is partly converted into a condensed phase. The sorption of DNB and DCP increases with pyrolytic temperature and is characterized by a transition from a partition dominant to an adsorption dominant process. However, the sorption of DCB linearly decreases with the pyrolytic temperature. The enhanced adsorption of DNB and DCP on carbonized phase is primarily attributed to nonhydrophobic interactions such as π–π electron-donor–acceptor interactions and/or H bonding. The higher partition of DCB to polymeric phase is attributed to its high hydrophobicity. Competitive sorption between DCB and DCP on the tire chars is highly dependent on dissociation of the latter.
Afficher plus [+] Moins [-]XAFS study of starch-stabilized magnetite nanoparticles and surface speciation of arsenate
2011
Zhang, Meiyi | Pan, Gang | Zhao, Dongye | He, Guangzhi
It has been shown that starch can effectively stabilize nanoscale magnetite particles, and starch-stabilized magnetite nanoparticles (SMNP) are promising for in situ remediation of arsenic-contaminated soils. However, a molecular level understanding has been lacking. Here, we carried out XAFS studies to bridge this knowledge gap. Fe K-edge XAFS spectra indicated that the Fe–O and Fe–Fe coordination numbers of SMNP were lower than those for bare magnetite particles, and these coordination numbers decreased with increasing starch concentration. The decrease in the average coordination number at elevated stabilizer concentration was attributed to the increase in the surface-to-volume ratio. Arsenic K-edge XAFS spectra indicated that adsorbed arsenate on SMNP consisted primarily of binuclear bidentate (BB) complexes and monodentate mononuclear (MM) complexes. More BB complexes (energetically more favorable) were observed at higher starch concentrations, indicating that SMNP not only offered greater adsorption surface area, but also stronger adsorption affinity toward arsenate.
Afficher plus [+] Moins [-]Effects of compositional heterogeneity and nanoporosity of raw and treated biomass-generated soot on adsorption and absorption of organic contaminants
2011
Chen, Baoliang | Huang, Wenhai
A biomass-generated soot was sequentially treated by HCl-HF solution, organic solvent, and oxidative acid to remove ash, extractable native organic matter (EOM), and amorphous carbon. The compositional heterogeneity and nano-structure of the untreated and treated soot samples were characterized by elemental analysis, thermal gravimetric analysis, BET-N₂ surface area, and electron microscopic analysis. Sorption properties of polar and nonpolar organic pollutants onto the soot samples were compared, and individual contributions of adsorption and absorption were quantified. The sorption isotherms for raw sample were practically linear, while were nonlinear for the pretreated-soot. The removal of EOM enhanced adsorption and reduced absorption, indicating that EOM served as a partitioning phase and simultaneously masked the adsorptive sites. By drastic-oxidation, the outer amorphous carbon and the inner disordered core of the soot particles were completely removed, and a fullerene-like nanoporous structure (aromatic shell) was created, which promoted additional π–π interaction between phenanthrene and the soot.
Afficher plus [+] Moins [-]Sorption of simazine to corn straw biochars prepared at different pyrolytic temperatures
2011
Zhang, Guixiang | Zhang, Qing | Sun, Ke | Liu, Xitao | Zheng, Wenjuan | Zhao, Ye
Simazine sorption to corn straw biochars prepared at various temperatures (100–600 °C) was examined to understand its sorption behavior as influenced by characteristics of biochars. Biochars were characterized via elemental analysis, BET-N₂ surface area (SA), FTIR and ¹³C NMR. Freundlich and dual-mode models described sorption isotherms well. Positive correlation between log Kₒc values and aromatic C contents and negative correlation between log Kₒc values and (O + N)/C ratios indicate aromatic-rich biochars have high binding affinity to simazine (charge transfer (π–π*) interactions) and hydrophobic binding may overwhelm H-bonding, respectively. Dual-mode model results suggest adsorption contribution to total sorption increases with carbonization degree. Positive correlation between amounts of adsorption (Qₐd) and SA indicates pore-filling mechanism. Comparison between our results and those obtained with other sorbents indicates corn straw biochars produced at higher temperature can effectively retain simazine. These observations will be helpful for designing biochars as engineered sorbents to remove triazine herbicides.
Afficher plus [+] Moins [-]Ecotoxicity of nanosized TiO₂. Review of in vivo data
2011
Menard, Anja | Drobne, Damjana | Jemec, Anita
This report presents an exhaustive literature review of data on the effect of nanoparticulate TiO₂ on algae, higher plants, aquatic and terrestrial invertebrates and freshwater fish. The aim, to identify the biologically important characteristics of the nanoparticles that have most biological significance, was unsuccessful, no discernable correlation between primary particle size and toxic effect being apparent. Secondary particle size and particle surface area may be relevant to biological potential of nanoparticles, but insufficient confirmatory data exist. The nanotoxicity data from thirteen studies fail to reveal the characteristics actually responsible for their biological reactivity because reported nanotoxicity studies rarely carry information on the physicochemical characteristics of the nanoparticles tested. A number of practical measures are suggested which should support the generation of reliable QSAR models and so overcome this data inadequacy.
Afficher plus [+] Moins [-]Ultrasonic Enhanced Desorption of DDT from Contaminated Soils
2011
Thangavadivel, Kandasamy | Megharaj, Mallavarapu | Smart, Roger St. C. | Lesniewski, Peter J. | Bates, Darren | Naidu, R.
In this study, using high-power low-frequency ultrasound, heated slurries with anionic surfactant sodium dodecyl sulfate (SDS) were treated to enhance desorption of DDT from soils with high clay, silt, and organic matter content and different pH (5.6–8.4). The results were compared with DDT extracted using a strong solvent combination as reference. Slurry ranges from 5 to 20Â wt.% were studied. For a soil slurry (10Â wt.%) at pHÂ 6.9 with 0.1% v/v SDS surfactant heated to 40°C for 30Â min, desorption was above 80% in 30Â s using 20Â kHz, 932 W/L ultrasonic intensity without solvent extraction. Other soils gave lower desorption efficiency in the range 40–60% after 30Â s ultrasonic treatment. The percentage of organic matter, dissolved organic carbon, soil surface area, clay and silt percentage, and soil pH level were the key parameters influencing variations in desorption of DDT in the three soils in similar experimental conditions. DDT dissolution in SDS and soil organic matter removal employing the ultrasonic-enhanced organic matter roll-up mechanism emerged as the two best possible methods of DDT desorption. The method offers a practical, potentially low-cost alternative to high volume, costly, hazardous solvent extraction of DDT.
Afficher plus [+] Moins [-]Natural Attenuation of Zn, Cu, Pb and Cd in Three Biosolids-Amended Soils of Contrasting pH Measured Using Rhizon Pore Water Samplers
2011
Murtaza, Ghulam | Haynes, R. J. | Naidu, Ravindra | Belyaeva, Oxana N. | Kim, Kwon-Rae | Lamb, Dane T. | Bolan, Nanthi S.
The effects of application of biosolids, at four rates, to an alkaline (pH 8.4), neutral (pH 7.0) and acidic (pH 4.0) soil on concentrations of Cu, Zn, Pb, Cd and dissolved organic C in soil solution were measured over a 170-day period in a laboratory incubation study using Rhizon pore water samplers. Applications of biosolids decreased solution pH in the alkaline soil, increased it in the acidic soil and had little effect in the neutral soil. In general, increasing application rates of biosolids progressively increased EC and concentrations of dissolved organic C (DOC), Cu, Zn, and to a lesser extent Cd and Pb, in soil solution. Concentrations of DOC and concentrations of solution Cu, Zn, and to a lesser extent solution Cd and Pb, decreased over the incubation period. In all three soils, concentrations of solution Cu and Zn were closely positively correlated with DOC concentrations and similar positive but weaker correlations were found for solution Cd and Pb. For the alkaline and neutral soils, concentrations of solution Cu, Zn, Cd and Pb were generally negatively correlated with solution pH but for the acidic soil, positive correlations for Cu and Zn were recorded. The percentage reduction in solution Cu and Zn, between 0 and 170 days incubation, increased with increasing rates of biosolids in the acid soil (where biosolids applications increased pH) but the reverse was the case for the alkaline soil (where pH fell following biosolids applications). Greatest percentage reduction in soluble Cu and Zn occurred in the neutral soil which had the greatest BET surface area, clay and organic matter contents and therefore the greatest capacity to adsorb heavy metal cations. It was concluded that solution pH, dissolved organic C and the intrinsic capacity of the soil to remove metals from solution, were the main factors interacting to regulate heavy metal cation solubility in the biosolids-amended soils.
Afficher plus [+] Moins [-]Metal and Metalloid Contaminants in Atmospheric Aerosols from Mining Operations
2011
Csavina, Janae | Landázuri, Andrea | Wonaschütz, Anna | Rine, Kyle | Rheinheimer, Paul | Barbaris, Brian | Conant, William | Sáez, Avelino Eduardo | Betterton, Eric A.
Mining operations are potential sources of airborne metal and metalloid contaminants through both direct smelter emissions and wind erosion of mine tailings. The warmer, drier conditions predicted for the Southwestern USA by climate models may make contaminated atmospheric dust and aerosols increasingly important, with potential deleterious effects on human health and ecology. Fine particulates such as those resulting from smelting operations may disperse more readily into the environment than coarser tailings dust. Fine particles also penetrate more deeply into the human respiratory system and may become more bioavailable due to their high specific surface area. In this work, we report the size-fractionated chemical characterization of atmospheric aerosols sampled over a period of a year near an active mining and smelting site in Arizona. Aerosols were characterized with a ten-stage (0.054 to 18Â μm aerodynamic diameter) multiple orifice uniform deposit impactor (MOUDI), a scanning mobility particle sizer (SMPS), and a total suspended particulate collector. The MOUDI results show that arsenic and lead concentrations follow a bimodal distribution, with maxima centered at approximately 0.3 and 7.0Â μm diameter. We hypothesize that the sub-micron arsenic and lead are the product of condensation and coagulation of smelting vapors. In the coarse size, contaminants are thought to originate as Aeolian dust from mine tailings and other sources. Observation of ultrafine particle number concentration (SMPS) show the highest readings when the wind comes from the general direction of the smelting operations site.
Afficher plus [+] Moins [-]Microstructures and Photocatalytic Properties of Fe3+/Ce 3+ Codoped Nanocrystalline TiO 2 Films
2011
Qu, Yan-zhen | Yao, Ming-ming | Li, Fang | Sun, Xiao-hu
Fe3+ and Ce3+ codoped titanium dioxide films with high photocatalytic activity were successfully obtained via the improved sol–gel process. The as-prepared specimens were characterized using X-ray diffraction (XRD), high-resolution field emission scanning electron microscopy (FE-SEM), X-ray energy dispersive spectroscopy, Brunauer–Emmett–Teller (BET) surface area, X-ray photoelectron spectroscopy, photoluminescence (PL) spectra, and UV–Vis diffuse reflectance spectroscopy. The photocatalytic activities of the films were evaluated by degradation of various organic dyes in aqueous solutions. The results of XRD, FE-SEM, and BET analyses indicated that the TiO2 film had nanostructure. With the codoping of Fe3+ and Ce3+, TiO2 photocatalysts with smaller crystal size, larger surface area, and larger pore volume were obtained. Moreover, codoped ions could obviously not only suppress the formation of brookite phase but also inhibit the transformation of anatase to rutile at high temperature. Compared with pure TiO2 film, Fe3+ doped or Ce3+ doped TiO2 film, the Fe3+/Ce3+ codoped TiO2 film exhibited excellent photocatalytic activity. It is believed that the surface microstructure of the films and the doping methods of the ions are responsible for improving the photocatalytic activity.
Afficher plus [+] Moins [-]Adsorption of Pb, Cd, Cu, Zn, and Ni to titanium dioxide nanoparticles: effect of particle size, solid concentration, and exhaustion
2011
Engates, Karen E | Shipley, Heather J
Purpose Adsorption of metals (Pb, Cd, Cu, Ni, Zn) to TiO₂ nanoparticles and bulk particles was examined for use as a contaminant removal substrate as a function of particle size, sorbent concentration, and exhaustion. Methods Adsorption experiments were conducted with 0.01, 0.1, and 0.5 g/L nanoparticles in a pH 8 solution and in spiked San Antonio tap water. Results When results were normalized by mass, nanoparticles adsorbed more than the bulk particles but when results were surface-area normalized, the opposite was observed. The adsorption data shows the ability of the TiO₂ nanoparticles to remove Pb, Cd, and Ni from solution with similar adsorption at 0.1 and 0.5 g/L. Adsorption kinetics for all metals tested was described by a modified first order rate equation with the nanoparticles having a faster rate of adsorption than the bulk particles. The nanoparticles were able to simultaneously removal multiple metals (Zn, Cd, Pb, Ni, Cu) from both pH 8 solution and spiked San Antonio tap water. Exhaustion experiments showed that both the nanoparticles and bulk particles were exhausted at pH 6 but at pH 8, exhaustion did not occur for the nanoparticles. Conclusion Comparison of K d, distribution coefficient, with other literature showed that the nanoparticles were better sorbents than other metal oxide nanoparticles and a commercial activated carbon.
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