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1.

Background, aim, and scope  

Sorption of hydrophobic organic compounds (HOCs) to natural organic matter (NOM) is an important process that affects the transport, transformation, bioavailability, and fate of HOCs in the environment. Manufactured nanoparticles (NPs) such as nano-oxides will inevitably enter the environment in the processes of their production, transfer, and use and could be coated by the ubiquitous NOM. Thus, sorption of HOCs to NOM in the environment could be affected by the NP interactions with NOM. Furthermore, the toxicity of nano-oxides could be increased due to the adsorbed HOCs. Therefore, sorption of phenanthrene by nano-Al2O3 coated with humic acid (HA) was examined in this study to explore the possible effect of nanoparticles (NPs) on the environmental behavior of HOCs and the potential environmental and health risks of NPs.  相似文献   

2.
Sorption of phenanthrene by soils contaminated with heavy metals   总被引:4,自引:0,他引:4  
Gao Y  Xiong W  Ling W  Xu J 《Chemosphere》2006,65(8):1355-1361
The fate of polycyclic aromatic hydrocarbons (PAHs) in soils with co-contaminants of heavy metals has yet to be elucidated. This study examined sorption of phenanthrene as a representative of PAHs by three soils contaminated with Pb, Zn or Cu. Phenanthrene sorption was clearly higher after the addition of heavy metals. The distribution coefficient (K(d)) and the organic carbon-normalized distribution coefficient (K(oc)) for phenanthrene sorption by soils spiked with Pb, Zn or Cu (0-1000 mg kg(-1)) were approximately 24% larger than those by unspiked ones, and the higher contents of heavy metals added into soils resulted in the larger K(d) and K(oc) values. The enhanced sorption of phenanthrene in the case of heavy metal-contaminated soils could be ascribed to the decreased dissolved organic matter (DOM) in solution and increased soil organic matter (SOM) as a consequence of DOM sorption onto soil solids. Concentrations of DOM in equilibrium solution for phenanthrene sorption were lower in the case of the heavy metal-spiked than unspiked soils. However, the decreased DOM in solution contributed little to the enhanced sorption of phenanthrene in the presence of metals. On the other hand, the sorbed DOM on soil solids after the addition of heavy metals in soils was found to be much more reactive and have far stronger capacity of phenanthrene uptake than the inherent SOM. The distribution coefficients of phenanthrene between water and the sorbed DOM on soil solids (K(ph/soc)) were about 2-3 magnitude larger than K(d) between water and inherent SOM, which may be the dominant mechanism of the enhanced sorption of phenanthrene by soils with the addition of heavy metals.  相似文献   

3.
The objective of this study was to investigate the influence of salinity on the effectiveness of surfactants in the remediation of sediments contaminated with phenanthrene (PHE). This is an example of a more general application of surfactants in removing hydrophobic organic compounds (HOCs) from contaminated soil/sediment in saline environments via in-situ enhanced sorption or ex-situ soil washing. Salinity effects on surfactant micelle formation and PHE partitioning into solution surfactant micelles and sorbed surfactant were investigated. The critical micelle concentration of surfactants decreased, and PHE partition between surfactant micelles and water increased with increasing salinity. Carbon-normalized partition coefficients (Kss) of PHE onto the sorbed cationic surfactant increased significantly with increasing salinity, which illustrates a more pronounced immobilization of PHE by cationic surfactant in a saline system. Reduction of PHE sorption by anionic surfactant was more pronounced in the saline system, indicating that the anionic surfactant has a higher soil washing effectiveness in saline systems.  相似文献   

4.
Phenanthrene is a 3-ring polycyclic aromatic hydrocarbon which exists mainly in the gas-phase in the atmosphere. Recent concern over the presence of 9,10-phenanthrenequinone in ambient particles led us to study the products of the gas-phase reactions of phenanthrene with hydroxyl radicals, nitrate radicals and ozone. The formation yields of 9,10-phenanthrenequinone were measured to be ∼3%, 33±9%, and ∼2% from the OH radical, NO3 radical and O3 reactions, respectively. Calculations suggest that daytime OH radical-initiated and nighttime NO3 radical-initiated reactions of gas-phase phenanthrene may be significant sources of 9,10-phenanthrenequinone in ambient atmospheres. In contrast, the ozone reaction with phenanthrene is unlikely to contribute significantly to ambient 9,10-phenanthrenequinone.  相似文献   

5.
Phenanthrene uptake by Medicago sativa L. was investigated under the influence of an arbuscular mycorrhizal fungus. Inoculation of lucerne with the arbuscular mycorrhizal fungus Glomus etunicatum L. resulted in higher phenanthrene accumulation in the roots and lower accumulation in the shoots compared to non-mycorrhizal controls. Studies on sorption and desorption of phenanthrene by roots and characterization of heterogeneity of mycorrhizal and non-mycorrhizal roots using solid-state 13C nuclear magnetic resonance spectroscopy (13C NMR) demonstrated that increased aromatic components due to mycorrhizal inoculation resulted in enhanced phenanthrene uptake by the roots but lower translocation to the shoots. Direct visualization using two-photon excitation microscopy (TPEM) revealed higher phenanthrene accumulation in epidermal cells of roots and lower transport into the root interior and stem in mycorrhizal plants than in non-mycorrhizal controls. These results provide some insight into the mechanisms by which arbuscular mycorrhizal inoculation may influence the uptake of organic contaminants by plants.  相似文献   

6.
《Chemosphere》2009,74(11):1832-1837
Sorption of nonpolar (phenanthrene and butylate) and polar (atrazine and diuron) organic chemicals to oil-contaminated soil was examined to investigate oil effects on sorption of organic chemicals and to derive oil–water distribution coefficients (Koil). The resulting oil-contaminated soil–water distribution coefficients (Kd) for phenanthrene demonstrated sorption-enhancing effects at both lower and higher oil concentrations (Coil) but sorption-reducing (competitive) effects at intermediate Coil (approximately 1 g kg−1). Rationalization of the different dominant effects was attempted in terms of the relative aliphatic carbon content which determines the accessibility of the aromatic cores to phenanthrene. Little or no competitive effect occurred for butylate because its sorption was dominated by partitioning. For atrazine and diuron, the changes in Kd at Coil above approximately 1 g kg−1 were negligible, indicating that the presently investigated oil has little or no effect on the two tested compounds even though the polarity of the oil is much less than soil organic matter (SOM). Therefore, specific interactions with the active groups (aromatic and polar domains) are dominantly responsible for the sorption of polar sorbates, and thus their sorption is controlled by available sorption sites. This study showed that the oil has the potential to be a dominant sorptive phase for nonpolar pollutants when compared to SOM, but hardly so for polar compounds. The results may aid in a better understanding of the role of the aliphatic and aromatic domains in sorption of nonpolar and polar organic pollutants.  相似文献   

7.
A method for measurement of atmospheric carbonaceous particulate matter is proposed and evaluated. A diffusion denuder, placed ahead of a filter, is used to exclude vapor-phase organic compounds which might be retained by adsorption on the filter. The carbonaceous material lost by volatilization from the filter after collection is retained with a fluidized bed of powdered Al2O3. The efficiencies of the denuder and Al2O3 were evaluated with vapor phase phenanthrene and octadecane. Atmospheric sampling was done at two urban and one background site in California using the proposed technique in parallel with conventional hi-vol and dichotomous samplers. Hi-vol samples appear to have lost up to half of the particle phase carbon during sampling. About half this error could be eliminated by sampling at low face velocity. The effects of face velocity appear to distort the proportions of fine and coarse particulate carbon obtained with a dichotomous sampler.  相似文献   

8.
Yu Z  Huang W  Song J  Qian Y  Peng P 《Chemosphere》2006,65(11):2493-2501
The objective of this study was to quantify sorption properties for kerogen/black carbon (BC)-bearing sediments. Single-solute sorption isotherms were measured for five pristine marine sediments using phenanthrene, naphthalene, 1,3,5-trichlorobenzene, and 1,4-dichlorobenzene as the sorbates. The results showed that the sorption isotherms were nonlinear and that the organic carbon normalized single point KOC values were comparable to those reported in the literature for the purified keorgen and BC, but are much higher than the data reported for HA and kerogen/BC-containing terrestrial soils and sediments. It is likely that koergen and BC associated with these pristine marine sediments may not be encapsulated with humic acids or Fe and Mn oxides and hydroxides as often do in terrestrial soils and sediments. As a result, they may be fully accessible to sorbing molecules, exhibiting higher sorption capacities. The study suggests that competition from background HOCs and reduced accessibility when kerogen and BC are associated with terrestrial sediments may dramatically increase variability of sorption reactivities of geosorbents. Such variability may lead to large uncertainties in the prediction of sorption from the contents of kerogen and/or BC along with TOC.  相似文献   

9.
Evaluation of impacts of soil fractions on phenanthrene sorption   总被引:3,自引:0,他引:3  
Luo L  Zhang S  Ma Y 《Chemosphere》2008,72(6):891-896
Phenanthrene sorption to soils and soil fractions was investigated using two contrasting soils with different clay mineral and organic carbon (OC) contents in an attempt to evaluate the contribution of each soil fraction to phenanthrene sorption and the applicability of the carbon-normalized distribution constant (K(OC)) in soils. Sorbents were characterized using surface analysis, solid-state (13)C NMR analysis, and glass transition temperature (T(g)) analysis to gain a insight into the chemical nature of OC in soils. Dissolved organic carbon (DOC) in the soil solution impeded the phenanthrene sorption, while humins accounted for the predominant phenanthrene sorption in soils. The contribution of OC to phenanthrene sorption in soil would be overestimated if only a K(OC)-approach was adopted, since clay minerals could account for much of the sorption, especially when OC was low in soils. Nitrogen gas was shown to be inappropriate for probing non-polar sorption capacity. The results obtained highlight the importance of clay minerals in governing the sorption of phenanthrene in soil, and emphasize the inapplicability of the carbon-normalized distribution coefficient K(OC) in soils.  相似文献   

10.
Soil organic matter (SOM) releasing with dissolved organic matter (DOM) formed in solution was confirmed in a sediment/water system, and the effects of SOM releasing on the sorption of phenanthrene on sediments were investigated. Inorganic salt (0–0.1 mol L?1 NaCl) was used to adjust SOM releasing, and two sediments were prepared, the raw sediment (S1) from Weihe River, Shann’xi, China, and the eluted sediments with and without DOM supernatant remained, termed as S2a and S2b, respectively. The FTIR and 1H NMR analysis indicate that the low molecular weight hydrophilic SOM fraction released prior to the high molecular weight hydrophobic fraction. As a response, phenanthrene sorption kinetics on S1 showed atypical and expressed as three stages: rapid sorption, pseudo sorption with partial desorption, and slow sorption, thus a defined “sorption valley” occurred in kinetic curve. In all cases, partition dominates the sorption, and sorption capacity (Kd) ranked as S2b > S1 > S2a. Compared with the alterations of sediment characters, DOM solubilization produced by SOM releasing exhibited a greater inhibitory effect on sorption with a relative contribution of 0.67. Distribution coefficients (Kdoc) of PHE into DOM clusters were 2.10?×?104–4.18?×?104 L kg?1, however a threshold concentration of 6.83 mg L?1 existed in DOM solubilization. The study results will help to clarify PAHs transport and their biological fate in a sediment/water system.  相似文献   

11.
Toxicity of nano-scaled aluminum, silicon, titanium and zinc oxides to bacteria (Bacillus subtilis, Escherichia coli and Pseudomonas fluorescens) was examined and compared to that of their respective bulk (micro-scaled) counterparts. All nanoparticles but titanium oxide showed higher toxicity (at 20 mg/L) than their bulk counterparts. Toxicity of released metal ions was differentiated from that of the oxide particles. ZnO was the most toxic among the three nanoparticles, causing 100% mortality to the three tested bacteria. Al2O3 nanoparticles had a mortality rate of 57% to B. subtilis, 36% to E. coli, and 70% to P. fuorescens. SiO2 nanoparticles killed 40% of B. subtilis, 58% of E. coli, and 70% of P. fluorescens. TEM images showed attachment of nanoparticles to the bacteria, suggesting that the toxicity was affected by bacterial attachment. Bacterial responses to nanoparticles were different from their bulk counterparts; hence nanoparticle toxicity mechanisms need to be studied thoroughly.  相似文献   

12.
Wang X  Cook R  Tao S  Xing B 《Chemosphere》2007,66(8):1476-1484
Sorption behavior of hydrophobic organic contaminants (HOCs) (i.e., pyrene, phenanthrene and naphthalene) by native and chemically modified biopolymers (lignin, chitin and cellulose) was examined. Lignins (native and treated) showed nonlinear sorption for all compounds studied, emphasizing their glassy character. Chitins and celluloses had linear isotherms for phenanthrene and naphthalene, illustrating the dominance of partitioning, while pyrene yielded nonlinear isotherms. Sorption capacity (K(oc)) of HOCs was negatively correlated with the polarity [(O+N)/C] of the biopolymers. Aromatic and alkyl+aromatic C percentages, rather than alkyl C content, demonstrated a better correlation with K(oc) values, indicating the importance of aromatic structures for HOC affinity. Hydrophobicity (K(ow))-normalized K(oc) values decreased sharply with increasing percentage of O-alkyl C versus total aliphatic C (O-alkyl C/total aliphatic C) or with polar C/(alkyl+aromatic C) ratio of the biopolymers until their values reached 80% and 4, respectively, illustrating the effect of surrounding polar groups on reducing affinity for HOCs. Overall, the results of this study highlight the role of spatial arrangement of domains within biopolymers in sorption of HOCs, and point to sorbent properties, such as functionality, polarity and structure, jointly regulating the sorption of HOCs in biopolymers.  相似文献   

13.
The main objective of this work concerns the coupling of biomass gasification reaction and CO2 sorption. The study shows the feasibility to promote biomass steam gasification in a dense fluidized bed reactor with CO2 sorption to enhance tar removal and hydrogen production. It also proves the efficiency of CaO-Ca12Al14O33/olivine bi-functional materials to reduce heavy tar production. Experiments have been carried out in a fluidized bed gasifier using steam as the fluidizing medium to improve hydrogen production. Bed materials consisting of CaO-based oxide for CO2 sorption (CaO-Ca12Al14O33) deposited on olivine for tar reduction were synthesized, their structural and textural properties were characterized by Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), and temperature-programmed reduction (TPR) methods, and the determination of their sorption capacity and stability analyzed by thermogravimetric analysis (TGA). It appears that this CaO-Ca12Al14O33/olivine sorbent/catalyst presents a good CO2 sorption stability (for seven cycles of carbonation/decarbonation). Compared to olivine and Fe/olivine in a fixed bed reactor for steam reforming of toluene chosen as tar model compound, it shows a better hydrogen production rate and a lower CO2 selectivity due to its sorption on the CaO phase. In the biomass steam gasification, the use of CaO-Ca12Al14O33/olivine as bed material at 700 °C leads to a higher H2 production than olivine at 800 °C thanks to CO2 sorption. Similar tar concentration and lighter tar production (analyzed by HPLC/UV) are observed. At 700 °C, sorbent addition allows to halve tar content and to eliminate the heaviest tars.  相似文献   

14.
Chen H  Chen S  Quan X  Zhao H  Zhang Y 《Chemosphere》2008,73(11):1832-1837
Sorption of nonpolar (phenanthrene and butylate) and polar (atrazine and diuron) organic chemicals to oil-contaminated soil was examined to investigate oil effects on sorption of organic chemicals and to derive oil–water distribution coefficients (Koil). The resulting oil-contaminated soil–water distribution coefficients (Kd) for phenanthrene demonstrated sorption-enhancing effects at both lower and higher oil concentrations (Coil) but sorption-reducing (competitive) effects at intermediate Coil (approximately 1 g kg−1). Rationalization of the different dominant effects was attempted in terms of the relative aliphatic carbon content which determines the accessibility of the aromatic cores to phenanthrene. Little or no competitive effect occurred for butylate because its sorption was dominated by partitioning. For atrazine and diuron, the changes in Kd at Coil above approximately 1 g kg−1 were negligible, indicating that the presently investigated oil has little or no effect on the two tested compounds even though the polarity of the oil is much less than soil organic matter (SOM). Therefore, specific interactions with the active groups (aromatic and polar domains) are dominantly responsible for the sorption of polar sorbates, and thus their sorption is controlled by available sorption sites. This study showed that the oil has the potential to be a dominant sorptive phase for nonpolar pollutants when compared to SOM, but hardly so for polar compounds. The results may aid in a better understanding of the role of the aliphatic and aromatic domains in sorption of nonpolar and polar organic pollutants.  相似文献   

15.
以市售活性炭、硅藻土和氧化铝小球为载体,考察了负载铁基活性组分对催化臭氧化过程中溴酸盐的控制情况,其中,铁基复合氧化铝小球体现出更好的溴酸盐还原特性和催化剂稳定性,证实催化剂中铁氧化物是溴酸盐得到有效控制的主要活性组分。进一步考察了铁基复合氧化铝小球催化臭氧化处理实际原水过程中对溴酸盐的生成控制,以及反应过程中溶解性有机碳(DOC)的去除情况。结果表明,与单独臭氧化相比,该催化剂既能有效去除水中的溶解性有机物,又能明显抑制溴酸盐的生成,反应50 h,其活性并没有明显下降。催化剂失活主要归因于吸附位点数量的下降,可以通过负载铁氧化物来实现催化剂的再生。  相似文献   

16.
Two sediments were demineralized and sequentially fractionated into extracted fractions [free lipid (FL), bound lipid (BL) and lignin (LG)] and residual fractions [free lipid free (FLF), bound lipid free (BLF) and lignin free (LGF)]. The sorption isotherms of phenanthrene (Phen) were examined to evaluate the importance of various fractions on sorption. A lignin extraction procedure was for the first time applied to separate the lignin or degraded lignin fraction from sediment organic matter (SOM). The extracted LG was similar to model lignin in terms of elemental ratios and sorption behavior. FL and LG fractions were quite important, as their contents were much higher than reported values. Phen sorption for the extracted fractions was almost linear, whereas that for the residual fractions was nonlinear, especially for LGF with n 0.56–0.63. As the different organic fractions were removed sequentially, sorption energy distribution on the residual sediment organic matter (SOM) became more heterogeneous. In addition, increasing sorption capacity for the residual fractions, except for BLF with its high polarity, suggested that more sorption sites on the SOM matrix became accessible to Phen. The sorption capacity for LGF was comparable to that of condensed SOM. The residual fraction LGF generally controlled the overall sorption at low Phen concentration, but the extractable fraction FL surpassed the former fraction at high Phen concentration, demonstrating the importance of condensed SOM in the sorption of hydrophobic organic compounds (HOCs) in sediments.  相似文献   

17.
Experiments were conducted to compare the sorption and desorption of phenanthrene and its primary degradation product, 1-hydroxy-2-naphthoic acid (HNA), in estuarine sediment, humic acid (HA) and humin. Ionic composition, ionic strength (0.4 M) and pH (7.6) were employed to mimic native estuarine pore water at the sediment-water interface. Sorption to whole sediment and organic matter (OM) fractions was significantly lower for HNA than for phenanthrene. Whereas HNA did not sorb to HA, uptake to sediment and humin was observed, suggesting that HNA does not bind directly to OM. Phenanthrene uptake was characterized by hysteretic behavior and exhibited slow desorption. In contrast, HNA initially was more readily desorbed from sediment and humic fractions, but a significant fraction was not recovered in repeated desorption runs. The lower sorption of HNA reflects its greater polarity and water solubility, but the consistent retention of a non-desorbing fraction suggests strong binding and/or chemical transformation reactions may be important. It was postulated that abiotic transformation of HNA may occur in estuarine sediments, in part due to the presence of redox active minerals (Fe(III) and Mn(IV) oxides). The presence of Fe and Mn solids in the estuarine sediment was verified by sequential extraction and studies were then conducted to investigate the transformation of HNA in the presence of synthetic goethite (alpha-FeOOH) and birnessite (delta-MnO2) as model solids. Reaction with birnessite led to transformation of all HNA in solution within 24 h and resulted in the formation of partial oxidation products (POPs). Following reaction with goethite, HNA was present in solution and POPs were observed in the weakly bound fraction. This study indicates that degradation products of polycyclic aromatic hydrocarbons (PAHs) may have distinctly different sorption affinities and reactivities toward environmental surfaces than their parent compounds.  相似文献   

18.
As in vivo system, we propose Drosophila melanogaster as a useful model for study the genotoxic risks associated with nanoparticle exposure. In this study we have carried out a genotoxic evaluation of titanium dioxide (TiO2), zirconium oxide (ZrO2) and aluminium oxide (Al2O3) nanoparticles and their microparticulated forms in D. melanogaster by using the wing somatic mutation and recombination assay. This assay is based on the principle that loss of heterozygosis and the corresponding expression of the suitable recessive markers, multiple wing hairs and flare-3, can lead to the formation of mutant clones in treated larvae, which are expressed as mutant spots on the wings of adult flies. Third instar larvae were feed with TiO2, ZrO2 and Al2O3 nanoparticles, and their microparticulated forms, at concentrations ranging from 0.1 to 10 mM. Although a certain level of aggregation/agglomeration was observed in solution, it must be noted than the constant digging activity of larvae ensures that treated medium pass constantly through the digestive tract ensuring exposure. The results showed that no significant increases in the frequency of all spots (e.g. small single, large single, twin, total mwh and total spots) were observed, indicating that these nanoparticles were not able to induce genotoxic activity in the wing spot assay of D. melanogaster. Negative data were also obtained with the microparticulated forms. This indicates that the nanoparticulated form of the selected nanomaterials does not modify the potential genotoxicity of their microparticulated versions. These in vivo results contribute to increase the genotoxicity database on the TiO2, ZrO2 and Al2O3 nanoparticles.  相似文献   

19.
The increasing use of nanoparticles (NPs) worldwide has raised some concerns about their impact on the environment. The aim of the study was to assess the toxicity of metal oxide nanoparticles, singly or combined, in a freshwater fish (Carassius auratus). The fish were exposed for 7, 14, and 21 days to different concentrations of NPs (10 μg Al2O3.L?1, 10 μg ZnO.L?1, 10 μg Al2O3.L?1 plus 10 μg ZnO.L?1, 100 μg Al2O3.L?1, 100 μg ZnO.L?1, and 100 μg Al2O3.L?1 plus 100 μg ZnO.L?1). At the end of each exposure period, antioxidant enzyme activity (catalase, glutathione-S-transferase, and superoxide dismutase), lipid peroxidation, and histopathology were assessed in the gills and livers of C. auratus. The results show an increase in catalase (CAT) and superoxide dismutase (SOD) activity in the gills and livers of fish, especially after 14 days of exposure to single and combined NPs, followed by a reduction at 21 days. An increase in glutathione S-transferase (GST) was observed in gills after 7 days for all tested NP concentrations (single and combined); while in livers, a significant increase was determined after 14 days of exposure to 100 μg.L?1 of both single ZnO and Al2O3 NPs. Lipid peroxidation (LPO) significantly increased in gills after 7 days of exposure to 100 μg.L?1 Al2O3 NPs (single or combined). In livers, LPO increased significantly after 7 days of exposure to all tested concentrations of both single ZnO and Al2O3 (except for 10 μg Al2O3.L?1), and after 14 days of exposure to ZnO (10 and 100 μg.L?1) and Al2O3 (100 μg.L?1). The results from histological observations suggest that exposure to metal oxide NPs affected both livers and gills, presenting alterations such as gill hyperplasia and liver degeneration. However, the most pronounced effects were found in gills. In general, this study shows that the tested NPs, single or combined, are capable of causing sub-lethal effects on C. auratus, but when combined, NPs seem to be slightly more toxic than when added alone.  相似文献   

20.
选择YT-1000型活性炭纤维(ACF)作为催化剂,考察ACF与O3协同作用催化降解水溶液中4-氯酚的最佳反应条件,并将该条件应用于焦化废水生物处理尾水中难降解有机污染物的催化氧化。ACF表面具有丰富的微孔结构,对4-氯酚有良好的吸附作用,在动力学上提高了其与O3反应的起始浓度,并且在ACF表面含氧、含氮等基团的催化作用下发生氧化反应,1 L浓度为100 mg/L的4-氯酚水样中投加2 g ACF反应6 min时,吸附作用对TOC的去除率为43.4%,而ACF协同O3作用时的TOC去除率提高到72.5%,协同增效作用为67.1%;在选定的反应条件下,ACF协同O3降解焦化废水生物处理尾水,60 min时的TOC与色度的去除率分别达到56.8%和96.3%。上述研究过程证明了吸附作用与催化作用的协同能有效降解生物过程不能降解的焦化废水中惰性有机污染物。  相似文献   

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