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Long-term aging of a CeO2 based nanocomposite used for wood protection
2014
Auffan, Melanie | Masion, Armand | Labille, Jerome | Diot, Marie-Ange | Liu, Wei | Olivi, Luca | Proux, Olivier | Ziarelli, Fabio | Chaurand, Perrine | Geantet, Christophe | Bottero, Jean-Yves | Rose, Jerome
A multi-scale methodology was used to characterize the long-term behavior and chemical stability of a CeO2-based nanocomposite used as UV filter in wood stains. ATR-FTIR and 13C NMR demonstrated that the citrate coated chelates with Ce(IV) through its central carboxyl- and its α-hydroxyl- groups at the surface of the unaged nanocomposite. After 42 days under artificial daylight, the citrate completely disappeared and small amount of degradation products remained attached to the surface even after 112 days. Moreover, the release/desorption of the citrate layer led to a surface reorganization of the nano-sized CeO2 core observed by XANES (Ce L3-edge). Such a surface and structural transformation of the commercialized nanocomposite could have implications in term of fate, transport, and potential impacts towards the environment.
Показать больше [+] Меньше [-]Explaining PAH desorption from sediments using Rock Eval analysis
2014
Poot, Anton | Jonker, M.T.O. | Gillissen, Frits | Koelmans, Albert A.
Here, we provide Rock Eval and black carbon (BC) characteristics and polycyclic aromatic hydrocarbon (PAH) distribution coefficients (KD) for sediments from the Danube, Elbe, Ebro, and Meuse river basins. PAH desorption kinetic parameters were determined using sequential Tenax extractions. We show that residual carbon (RC) from Rock Eval analysis is an adequate predictor of fast, slow, and very slow desorbing fractions of 4-ring PAHs. RC correlated better than BC, the latter constituting only 7% of RC. A dual domain sorption model was statistically superior to a single domain model in explaining KD for low molecular weight PAHs, whereas the opposite was observed for high molecular weight PAHs. Because particularly the 4-ring PAHs are bioavailable and relevant from a risk assessment perspective and because their fast desorbing fractions correlate best with RC, we recommend RC as a relevant characteristic for river sediments.
Показать больше [+] Меньше [-]Mechanism of and relation between the sorption and desorption of nonylphenol on black carbon-inclusive sediment
2014
Liping, Lou | Guanghuan, Cheng | Jingyou, Deng | Mingyang, Sun | Huanyu, Chen | Qiang, Yang | Xinhua, Xu
Correlation between the sorption and desorption of nonylphenol (NP) and binary linear regression were conducted to reveal the underlying mechanism of and relation between sorption domains and desorption sites in black carbon (BC)-amended sediment. The sorption and desorption data could be fitted well using dual-mode (R2 = 0.971–0.996) and modified two-domain model (R2 = 0.986–0.995), respectively, and there were good correlations between these two parts of parameters (R2 = 0.884–0.939, P < 0.01). The NP percentage in desorbable fraction was almost equal to that of the partition fraction, suggesting the desorbed NP came from linear partition domain, whereas the resistant desorption NP was segregated in nonlinear adsorption sites, which were dominated by pores in BC-amended sediment. Our investigation refined theory about the relation between sorption domains and desorption sites in sediment and could be used to predict the release risk of NP using sorption data when BC is used for NP pollution control.
Показать больше [+] Меньше [-]Sorption affinities of sulfamethoxazole and carbamazepine to two sorbents under co-sorption systems
2014
Wang, Chi | Li, Hao | Liao, Shaohua | Zhang, Di | Wu, Min | Pan, Bo | Xing, Baoshan
The Kd of sulfamethoxazole (SMX) on activated carbon (AC) was larger than that of SMX on single-walled carbon nanotubes (SC), but the competition of SMX with carbamazepine (CBZ) for adsorption sites was weaker on AC than SC. Thus, a large Kd value does not necessarily reflect a high affinity. The analysis of the apparent sorption, competition, desorption hysteresis, and the sorption thermodynamics for SMX and CBZ did not provide sufficient information to distinguish their sorption affinities. The release of the adsorbed CBZ was not altered with SMX as the competitor, but SMX release increased significantly after CBZ addition. The higher sorption affinity of CBZ may be explained by the interactions of the CBZ benzene rings with the aromatic structures of the adsorbents. Although the thermodynamic meaning cannot be described, the release ratio of the adsorbed pollutants provides useful information for understanding pollutant sorption strength and associated risks.
Показать больше [+] Меньше [-]Species-dependent effects of biochar amendment on bioaccumulation of atrazine in earthworms
2014
Wang, Fang | Ji, Rong | Jiang, Zhongwei | Chen, Wei
We observed that at a contamination level of 4.25 mg-atrazine/kg-soil, the biota–soil accumulation factor (BSAF) for the anecic M. guillelmi is approximately 5 times that for the epigeic E. foetida. This is attributable to the fact that bio-uptake by E. foetida is mainly through dermal absorption, whereas bio-uptake by M. guillelmi is largely affected by the gut processes, through which the physical grinding and surfactant-like materials facilitate the desorption of atrazine from soil. Strikingly, biochar amendment resulted in much greater reduction in BSAF for M. guillelmi than for E. foetida. At a biochar dose of 0.5% (wt:wt) the difference in BSAF between the two species became much smaller, and at a dose of 2% no statistical difference was observed. A likely explanation is that gut processes by M. guillelmi were much less effective in extracting atrazine from the biochar (the predominant phase wherein atrazine resided) than from soil particles.
Показать больше [+] Меньше [-]Changes in the adsorption of bisphenol A, 17 α-ethinyl estradiol, and phenanthrene on marine sediment in Hong Kong in relation to the simulated sediment organic matter decomposition
2014
Fei, Ying-heng | Xing, Baoshan | Li, Xiao-yan
Marine sediment with an input of particulate organic matter was incubated to simulate the early aging process. On the sediment after various incubation periods, adsorption and desorption tests were conducted for three selected organic micropollutants: bisphenol A (BPA), 17α-ethinyl estradiol (EE2), and phenanthrene (Phe). The results showed significant sediment organic matter (SOM) decomposition during the incubation, and the SOM decay and transformation had a profound impact on the adsorption of organic compounds by the sediment. An increasing-delay-increasing pattern of change was observed for the SOM normalized partition coefficients of EE2 and Phe. This change was accordant to the transformation of SOM from labile organics into active biomass and its microbial products, and finally into more condensed and humic-like substances. Comparison between the 3 model micropollutants indicates that the chemical adsorption behaviors were mostly affected by their hydrophobic properties.
Показать больше [+] Меньше [-]Titanium dioxide nanoparticles as carrier facilitate bioaccumulation of phenanthrene in marine bivalve, ark shell (Scapharca subcrenata)
2014
Tian, Shengyan | Zhang, Yaodan | Song, Chunzheng | Zhu, Xiaoshan | Xing, Baoshan
To evaluate the impact of titanium dioxide nanoparticles (nTiO2) on the uptake of hydrophobic organic chemicals by marine bivalves, we conducted a comparative bioaccumulation study by exposing clam, Scapharca subcrenata, to phenanthrene (Phe) in the presence and absence of nTiO2. The large surface area of nTiO2 resulted in adsorption of co-existing Phe in aqueous solution to form nTiO2-Phe complexes. Accumulation of nTiO2 was not observed in clams at exposed concentration (500 μg/L) in this study. However, enhanced uptake of Phe by clams was observed in the presence of nTiO2, with ku and BAFs values being 2 and 1.7 times higher than that of Phe alone, respectively. The enhanced uptake can be explained by ingestion of nTiO2-Phe complexes into the gut and subsequent desorption of Phe there. Therefore, nTiO2 as a carrier facilitated the uptake of Phe by marine bivalves.
Показать больше [+] Меньше [-]Effects of oil dispersant and oil on sorption and desorption of phenanthrene with Gulf Coast marine sediments
2014
Gong, Yanyan | Zhao, Xiao | O'Reilly, S.E. | Qian, Tianwei | Zhao, Dongye
Effects of a model oil dispersant (Corexit EC9500A) on sorption/desorption of phenanthrene were investigated with two marine sediments. Kinetic data revealed that the presence of the dispersant at 18 mg/L enhanced phenanthrene uptake by up to 7%, whereas the same dispersant during desorption reduced phenanthrene desorption by up to 5%. Sorption isotherms confirmed that at dispersant concentrations of 18 and 180 mg/L, phenanthrene uptake progressively increased for both sediments. Furthermore, the presence of the dispersant during desorption induced remarkable sorption hysteresis. The effects were attributed to added phenanthrene affinity and capacity due to sorption of the dispersant on the sediments. Dual-mode models adequately simulated sorption isotherms and kinetic data in the presence of the dispersant. Water accommodated oil (WAO) and dispersant-enhanced WAO increased phenanthrene sorption by up to 22%. This information is important for understanding roles of oil dispersants on the distribution and transport of petroleum PAHs in seawater-sediments.
Показать больше [+] Меньше [-]Sorption of phenanthrene and benzene on differently structural kerogen: Important role of micropore-filling
2014
Zhang, Yulong | Ma, Xiaoxuan | Ran, Yong
Shale was thermally treated to obtain a series of kerogen with varied maturation. Their chemical, structural and porous properties were related to the sorption and/or desorption behaviors of phenanthrene and benzene. As the treatment temperature increases, aliphatic and carbonyl carbon of the kerogen samples decrease, while their aromaticity and maturation increase. Meanwhile, the isothermal nonlinearity of phenanthrene and benzene increases whereas the sorption capacity and micropore adsorption volumes (Vo,d) initially increase and then decrease. The Vo,d of benzene is significantly correlated with, but higher than that of phenanthrene, suggesting similar micropore filling mechanism and molecular sieve effect. The benzene desorption exhibits hysteresis, which is related to the pore deformation of the kerogen and the entrapment of solute in the kerogen matrix. The Vo,d of phenanthrene and benzene on the kerogen samples accounts for 23–46% and 36–65% of the maximum sorption volumes, respectively, displaying the importance of the micropore filling.
Показать больше [+] Меньше [-]Use of passive samplers for improving oil toxicity and spill effects assessment
2014
Letinski, Daniel | Parkerton, Thomas | Redman, Aaron | Manning, Ryan | Bragin, Gail | Febbo, Eric | Palandro, David | Nedwed, Tim
Methods that quantify dissolved hydrocarbons are needed to link oil exposures to toxicity. Solid phase microextraction (SPME) fibers can serve this purpose. If fibers are equilibrated with oiled water, dissolved hydrocarbons partition to and are concentrated on the fiber. The absorbed concentration (Cpolymer) can be quantified by thermal desorption using GC/FID. Further, given that the site of toxic action is hypothesized as biota lipid and partitioning of hydrocarbons to lipid and fibers is well correlated, Cpolymer is hypothesized to be a surrogate for toxicity prediction. To test this method, toxicity data for physically and chemically dispersed oils were generated for shrimp, Americamysis bahia, and compared to test exposures characterized by Cpolymer. Results indicated that Cpolymer reliably predicted toxicity across oils and dispersions. To illustrate field application, SPME results are reported for oil spills at the Ohmsett facility. SPME fibers provide a practical tool to improve characterization of oil exposures and predict effects in future lab and field studies.
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