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Arsenic mobility controlled by solid calcium arsenates: A case study in Mexico showcasing a potentially widespread environmental problem
2013
Martínez-Villegas, Nadia | Briones-Gallardo, Roberto | Ramos-Leal, José A. | Avalos-Borja, Miguel | Castañón-Sandoval, Alan D. | Razo-Flores, Elías | Villalobos, Mario
An As-contaminated perched aquifer under an urban area affected by mining was studied over a year to determine the contamination source species and the mechanism of As mobilization. Results show that the dissolution of calcium arsenates in residues disposed on an inactive smelter has caused high levels of As pollution in the adjoining downgradient 6-km perched aquifer, reaching up to 158 mg/L of dissolved As, and releasing a total of ca. 7.5 tons of As in a year. Furthermore, free calcium ion availability was found to control As mobility in the aquifer through the diagenetic precipitation of calcium arsenates (Ca5H2(AsO4)4·cH2O) preventing further mobilization of As. Results shown here represent a model for understanding a highly underreported mechanism of retention of arsenate species likely to dominate in calcium-rich environments, such as those in calcareous sediments and soils, where the commonly reported mechanism of adsorption to iron(III) oxyhydroxides is not the dominant process.
Показать больше [+] Меньше [-]Isosteric heats of sorption and desorption of phenanthrene in soils and carbonaceous materials
2013
Wang, Guohui | Grathwohl, Peter
Isosteric heats (ΔH) of sorption/desorption of phenanthrene were determined for carbonaceous materials (Pahokee peat, lignite, and high-volatile bituminous coal) and two soils based on reported equilibrium sorption/desorption isotherms at four different temperatures (4, 20, 46 and 77 °C). In addition, ΔH for desorption of native phenanthrene was determined to elucidate the “aging” effect by equilibrating samples with water at six temperatures (20, 40, 53, 61, 73, and 86 °C). Isosteric heats decreased with increasing solute concentration and were in a range of 19–35 kJ mol−1. Values higher than the heat of octanol–water phase transfer for phenanthrene (19 kJ mol−1) imply that both partitioning and adsorption processes are involved for these materials, where the sorptive contributions from both processes were estimated based on the phenanthrene thermodynamic data. Moreover, on the basis of ΔH values of desorption, release of native and spiked phenanthrene from our samples was similar.
Показать больше [+] Меньше [-]Protective role of fine silts for PAH in a former industrial soil
2013
Pernot, Audrey | Ouvrard, Stéphanie | Leglize, Pierre | Faure, Pierre
An original combined organic geochemistry and soil science approach was used to elucidate PAH availability controlling factors in a multi-contaminated industrial soil. Water granulodensimetric fractionation was applied to obtain five water-stable material fractions. These were characterized by elemental, molecular and mineral analysis, and microscopic observations. Among the different fractions, fine silts distinguished themselves by higher carbon and nitrogen contents, lower C/N ratio, an enrichment in total PAH and especially high molecular weight compounds, a coal tar signature and the lowest PAH availability. This fine silt fraction seemed to play a protective role for PAH that might be explained by its size and/or its specific reactivity. The mineral phases present in this fraction were proposed to explain the protection of organic matter. This led to a specific molecular signature of OM, having higher sorption properties both processes (sorption and mineral-bound protection) resulting in a lower PAH availability.
Показать больше [+] Меньше [-]Influence of contact time and sediment composition on the bioavailability of Cd in sediments
2013
Zhong, Huan | Kraemer, Lisa | Evans, Douglas
Stable isotope 111Cd was spiked into sediments of different organic content levels for 3 days to 2 months. Bioavailability of spiked Cd to deposit-feeders, assessed by in vitro Cd solubilization, generally decreased with contact time but became comparable with that of background Cd after 2 months. This could be explained by the gradual transfer of Cd from the more mobile geochemical phase (carbonate associated phase) to more refractory phases (Fe–Mn oxide associated phase, and organic associated phase) within 2 months. The sedimentary organic content had a weak effect on Cd solubilization, while the distribution of Cd in carbonate or Fe–Mn oxide associated phase could have a larger influence on the solubilization of sedimentary Cd and its change with contact time. The observations in this study emphasize the need to consider Cd sequestration over time in sediments of various compositions, which would be useful in risk assessment of contaminated sediments.
Показать больше [+] Меньше [-]Sorption of humic acid to functionalized multi-walled carbon nanotubes
2013
Wang, Fei | Yao, Jun | Chen, Huilun | Yi, Zhengji | Xing, Baoshan
The environmental behavior of carbon nanotubes (CNTs) and humic acid (HA) is a prominent concern, but effect of functionalities on their sorption is not clear yet. Functionalized multi-walled CNTs (MCNT15) and HA were used to study their sorption behavior. Sorption rate of HA to MCNTs was dominantly controlled by its diffusion from liquid-MCNT boundary to MCNT surfaces. The sorption is in the sequence of MCNT15 > MCNT15-NH2 > MCNT15-OH > MCNT15-COOH > MCNT15-Ni, which was dependent on their surface area and meso- and macro-pore volume. The functionalities of MCNTs regulated the sorption by affecting their interaction mechanisms (i.e., H-bonding, π–π, and hydrophobic interaction). Additionally, the amount of these functionalities on the MCNT surface reduced indirectly the sorption sites due to the steric hindrance. Electrostatic repulsion deceased the sorption of HA by MCNTs with increasing pH. This study demonstrated the importance of functionalities on the MCNTs for the sorption of HA.
Показать больше [+] Меньше [-]The effects of surfactants and solution chemistry on the transport of multiwalled carbon nanotubes in quartz sand-packed columns
2013
Lu, Yinying | Xu, Xiaopan | Yang, Kun | Lin, Daohui
The effect of different surfactants on the transport of multiwalled carbon nanotubes (MWCNTs) in quartz sand-packed columns was firstly investigated under various conditions. The stable plateau values (Cmax) of the breakthrough curves (BTCs), critical PVs (the number of pore volumes of infusions needed to reach the Cmax), maximum transport distances (Lmax), deposition rate coefficients (kd) and retention rates were calculated to compare the transport and retention of MWCNTs under various conditions. Stability of the MWCNT suspensions as a function of the influencing factors was examined to reveal the underlying mechanism of the MWCNT retention. Results showed that MWCNTs suspended by different surfactants presented different BTCs; the MWCNT transport increased with increasing sand size and MWCNT concentration; high flow velocity was favorable for the MWCNT transport, while high Ca2+ concentration and low pH were unfavorable for the transport; hetero-aggregation, straining and site blocking occurred during the transport.
Показать больше [+] Меньше [-]Contribution of a submerged membrane bioreactor in the treatment of synthetic effluent contaminated by Bisphenol-A: Mechanism of BPA removal and membrane fouling
2013
Seyhi, Brahima | Drogui, Patrick | Buelna, Gerardo | Azaïs, Antonin | Heran, Marc
A submerged membrane bioreactor has been operated at the laboratory scale for the treatment of a synthetic effluent containing Bisphenol-A (BPA). COD, NH4–N, PO4–P and BPA were eliminated respectively, at 99%, 99%, 61% and 99%. The increase of volumetric loading rate from 0 to 21.6 g/m3/d did not affect the performance of the MBR system. However, the removal rate decreased rapidly when the BPA loading rate increased above 21.6 g/m3/d. The adsorption process of BPA on the biomass was very well described by Freundlich and Langmuir isotherms. Subsequently, biodegradation of BPA occurred and followed the first order kinetic reaction, with a constant rate of 1.13 ± 0.22 h−1. During treatment, membrane fouling was reversible in the first 84 h of filtration, and then became irreversible. The membrane fouling was mainly due to the accumulation of suspended solid and development of biofilm on the membrane surface.
Показать больше [+] Меньше [-]Enhancement of water solubility and mobility of phenanthrene by natural soil nanoparticles
2013
Li, Wenyan | Zhu, Xinyu | He, Yan | Xing, Baoshan | Xu, Jianming | Brookes, Philip C.
Nanoparticles (NPs) in soils may participate in essential ecological services, since they have special characteristics arising from their nanoscale sizes and large surface areas. We did aqueous solubility enhancement experiments to derive the partition coefficients of phenanthrene between water and six natural soil NPs. The coefficients were approximately exponentially reduced with increasing concentrations of NPs, low concentrations of NPs (50 mg L−1) had significant high adsorption capacities for phenanthrene. Further experiments based on dynamic light scattering technique and column tests were performed to examine the aggregation and mobility of soil NPs and how they influence phenanthrene mobility in porous media. NPs have high and reversible adsorption on surfaces of porous media with aggregation taking place during their transport and they largely control the mobility of phenanthrene in sand columns.
Показать больше [+] Меньше [-]Enhanced PCBs sorption on biochars as affected by environmental factors: Humic acid and metal cations
2013
Wang, Yu | Wang, Lei | Fang, Guodong | Herath, H.M.S.K. | Wang, Yujun | Cang, Long | Xie, Zubin | Zhou, Dongmei
Biochar plays an important role in the behaviors of organic pollutants in the soil environment. The role of humic acid (HA) and metal cations on the adsorption affinity of polychlorinated biphenyls (PCBs) to the biochars in an aqueous medium and an extracted solution from a PCBs-contaminated soil was studied using batch experiments. Biochars were produced with pine needles and wheat straw at 350 °C and 550 °C under anaerobic condition. The results showed that the biochars had high adsorption affinity for PCBs. Pine needle chars adsorbed less nonplanar PCBs than planar ones due to dispersive interactions and separation. Coexistence of HA and metal cations increased PCBs sorption on the biochars accounted for HA adsorption and cation complexation. The results will aid in a better understanding of biochar sorption mechanism of contaminants in the environment.
Показать больше [+] Меньше [-]An intermediate complexity dynamic model for predicting accumulation of atmospherically-deposited metals (Ni, Cu, Zn, Cd, Pb) in catchment soils: 1400 to present
2013
The Intermediate Dynamic Model for Metals (IDMM) is a model for prediction of the pools of metals (Ni, Cu, Zn, Cd, Pb) in topsoils of catchments resulting from deposition of metals from the atmosphere. We used the model to simulate soil metal pools from 1400 onwards in ten UK catchments comprising semi-natural habitats, and compared the results with present day observations of soil metal pools. Generally the model performed well in simulating present day pools, and further improvements were made to simulations of Ni, Cu, Zn and Cd by adjusting the strength of metal adsorption to the soils. Some discrepancies between observation and prediction for Pb appeared to be due either to underestimation of cumulative deposition, or to overestimation of the metal pool under ‘pristine’, pre-industrial conditions. The IDMM provides a potential basis for large scale assessment of metal dynamics in topsoils.
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