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1.
Although polycyclic aromatic hydrocarbons (PAHs) are common pollutants in snow, there is little quantitative data about their rates of photodegradation in this environment. To begin to address this gap, we have measured the degradation kinetics of phenanthrene, pyrene, and fluoranthene on ice, as these are the most abundant PAHs in arctic snow. Frozen aqueous solutions of individual PAHs, with and without added hydrogen peroxide (HOOH) as a source of hydroxyl radical (OH), were illuminated with simulated sunlight. For all three PAHs, direct photodecay is the main mechanism of degradation, while OH-initiated indirect photodegradation is a minor sink. Rate constants (±1 SE) for direct photodegradation extrapolated to midday, surface snow conditions at Summit, Greenland on the summer solstice are 3.8 (±0.8) × 10?5, 28 (±3) × 10?5, and 1.4 (±0.7) × 10?5 s?1 for phenanthrene, pyrene, and fluoranthene, respectively. Apparent quantum efficiencies for photodegradation with simulated sunlight were 3.8 (±0.8) × 10?3, 4.3 (±0.5) × 10?4, and 2 (±1) × 10?5, respectively. Calculated PAH lifetimes in surface snow under Summit conditions are 1–19 h during mid-summer, but increase to >100 days in the dark winter. While the short photodegradation lifetimes in the summer suggest that there should be no appreciable PAH levels in this season, past measurements at Summit sometimes show significant levels of these PAHs in summer surface snow. This discrepancy is likely due to differences in PAH location between lab samples (where the PAHs are probably in quasi-liquid layers) and real snow (where PAHs are likely primarily associated with particulate matter).  相似文献   

2.
El Nemr A  Abd-Allah AM 《Chemosphere》2003,52(10):1711-1716
The residues of seven polycyclic aromatic hydrocarbons (PAHs) pollutants in microlayer and subsurface seawater samples collected from Alexandria coast, Egypt, were analyzed by gas chromatography–electron-impact mass spectrometry-selected ion monitoring mode (GC–MS-SIM). The pollutants studied were, fluorene, phenanthrene, anthracene, fluoranthene, pyrene, chrysene and benzo[a]pyrene. Total PAH levels in microlayer ranged from 103 to 523 ng/l, while it ranged in subsurface samples from 13 to 120 ng/l. The Western Harbor location recorded the highest level of PAHs pollutant over all the other location for both subsurface and microlayer waters. The two major PAHs in microlayer water at the Western Harbor were fluorene and phenanthrene, making up 27% and 20% of the total PAHs, while the two major PAHs in subsurface water at the Eastern Harbor were phenanthrene and fluoranthene recording up 21% each of the total PAHs. The total PAH levels were generally in the nano-gram per liter for microlayer and subsurface seawater samples. The dominant PAHs in both subsurface and microlayer samples were fluoranthene, pyrene and benzo[a]pyrene. The microlayer enrichment factor at Alexandria’s Mediterranean coast was ranged from 29 for fluorene to 3 for phenanthrene and benzo[a]pyrene which showed PAHs concentration in the microlayer with an average of five times more than the total PAH in the subsurface samples.  相似文献   

3.
This study investigated the levels, sources and ecological risks of 16 polycyclic aromatic hydrocarbons (PAHs) in two sediment cores that were collected along the Huaxi Reservoir. The spatial distributions and residue levels of the 16 priority PAHs in the sediments from the Huaxi Reservoir were analyzed for their potential ecological risk, source apportionment and contribution to the total PAH residue. The concentration level of the total PAHs (TPAHs) was in the range 1805 ng·g?1 to 20023 ng·g?1 based on dry weight, and the content of PAHs in the Huaxi Reservoir exhibited a gradual upward trend. The PAH congener ratios fluoranthene/(fluoranthene + pyrene) and indeno[1, 2, 3-cd]pyrene/(indeno[1, 2, 3-cd]pyrene + benzo[g, h, i]perylene) were used to identify the source. The main source of the low molecular weight PAHs was wood and coal combustion, whereas the high molecular weight PAHs were primarily from petroleum combustion sources. The results of an ecological risk assessment demonstrated that ACE poses a potential ecological risk, while FLU, NAP, ANT, BaP, DBA, PHEN and PYR can have serious ecological risks.  相似文献   

4.
The bioaccumulation of two isomeric non-alternant non-priority polycyclic aromatic hydrocarbons (PAHs), namely cyclopenta[cd]pyrene and benzo[ghi]fluoranthene, was investigated in caged mussels (Mytilus galloprovincialis) exposed for 30 days in three sites of a coastal lagoon (Pialassa Baiona, Ravenna, Italy) contaminated by pyrogenic PAHs. The concentration of cyclopenta[cd]pyrene and benzo[ghi]fluoranthene increased from undetectable levels in reference mussels withdrawn from the Adriatic sea to 10-30 ng g(-1) dry weight in transplanted mussels. Other contaminants bioaccumulated by caged mussels included pyrene, fluoranthene and mercury. Whilst the isomer concentration ratio pyrene/fluoranthene in biota was comparable to that observed in sediments, the cyclopenta[cd]pyrene/benzo[ghi]fluoranthene ratio was much lower in mussels than in sediments. The lower sediment biota accumulation factor of cyclopenta[cd]pyrene with respect to that of benzo[ghi]fluoranthene was tentatively attributed to the greater biological activity of the former compound, which contains a reactive olefinic bond in the cyclopenta fused ring moiety. Given the higher mutagenic activity of cyclopenta[cd]pyrene with respect to other priority PAHs, its bioaccumulation from contaminated sediments may rise considerably the overall toxicity of PAH residues in exposed biota.  相似文献   

5.
Surface soil (0-20 cm) samples from nine representative vegetable fields located in Guangzhou, Shenzhen, Zengcheng and Huadu within the Pearl River Delta, South China were collected and analyzed for 16 USEPA priority polycyclic aromatic hydrocarbons (PAHs) using gas chromatography coupled to mass spectrometry (GC-MS). Total concentrations of 16 PAHs (Sigma(PAHs)) ranged from 160 to 3700 microg kg(-1). Large variations were observed also between concentrations of individual PAHs from different vegetable fields and within the site as well. Acenapthylene, benzo[b]fluoranthene, fluoranthene, benzo[a]pyrene and benzo[k]fluoranthene were consistently the most prevalent individual PAHs. The values of PAH isomer ratios [anthracene/(anthracene+phenanthrene) and fluoranthene/(fluoranthene+pyrene)] indicate that combustion processes are the major sources of PAHs. Concentrations of PAHs were poorly correlated with organic carbon concentrations of soils, suggesting different sources and also indicating that the PAH pollution of this area is recent. The same outcome is confirmed by the predominance of PAHs with fewer rings (相似文献   

6.
Diesel exhaust consists of a complex mixture of chemicals which contain known genotoxicants, one of which is polycyclic aromatic hydrocarbons (PAHs) which may be associated with adverse respiratory health outcomes. This study aimed to evaluate the distribution patterns of PAHs (anthracene, naphthalene, fluorene, phenanthrene, cyclopentaphenanthrene, pyrene, fluoranthene, benzanthracene, chrysene, benzo(e)pyrene, benzoacephenanthrylene, and benzo(a)pyrene) in serum collected from asthmatic and healthy control children. PAH serum levels were measured in samples collected from children who lived in 11 different locations in/round Riyadh, Saudi Arabia (Al-yarmouk, Usaibi, Sultana Al-kadema, Omrrojam, Kof, Janoob Dawdmi, Guberah, Arabbuah, Al-mozahemyah, Iskan Al-mazzer, and Al-gharabi) during the period 2010–2011. Our results showed that the highest total mean concentrations of PAH were found in serum samples collected from people who lived in Sultana Aljadhida, Almozahemyah, Guberah, and Omrrojam and were 663.9, 486.17, 412.18, and 258.6 ng ml?1, respectively. The most prevalent PAHs in serum samples were naphthalene, bezanthracene, benzoacephenanthrylene, phenanthrene, chrysene, and benzo(a)pyrene with a frequency that ranged from 54.5 to 90.9 % positive samples. A close monitoring of PAH pollution is strongly recommended, especially in food and plant samples, because of their high bioaccumulation capacity.  相似文献   

7.
Polycyclic aromatic hydrocarbons (PAHs) were determined by the GC-MS chromatography in the leaves of Quercus ilex L., an evergreen Mediterranean oak, to monitor the degree of pollution in the urban area of Naples compared to remote areas. Leaf samples were collected in July 1998 from four urban parks, six roadsides and two sites in remote areas. The total PAH contents in Q. ilex leaves ranged from 106.6 in a control site to 4607.5 ng/g d.w. along a road with a high traffic flow. The mean concentration factors (urban/control) were 3.8 for the parks and 15 for the roads. The contribution of carcinogenic PAHs (benz[a]anthracene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene, dibenz[a,h]anthracene, indeno[1,2,3-c,d]pyrene) was higher in urban area and differed according to the site, ranging from 6.7% to 21.3%. The total PAH burden in control sites was dominated by the low molecular weight PAHs, whilst along the urban roads fluoranthene, pyrene and benz[a]anthracene among the measured PAHs showed the highest values. PAHs were positively correlated (P<0.01) to trace metals measured in a previous study.  相似文献   

8.

The simultaneous fate of organic matter and 4 endocrine disruptors (3 polycyclic aromatic hydrocarbons (PAHs) (fluoranthene, benzo(b)fluoranthene, and benzo(a)pyrene) and nonylphenols (NP)) was studied during the anaerobic digestion followed by composting of sludge at lab-scale. Sludge organic matter was characterized, thanks to chemical fractionation and 3D fluorescence deciphering its accessibility and biodegradability. Total chemical oxygen demand (COD) removal was 41% and 56% during anaerobic digestion and composting, respectively. 3D fluorescence highlighted the quality changes of organic matter. During continuous anaerobic digestion, organic micropollutants’ removal was 22?±?14%, 6?±?5%, 18?±?9%, and 0% for fluoranthene, benzo(b)fluoranthene, benzo(a)pyrene, and nonylphenols, respectively. Discontinuous composting allowed to go further on the organic micropollutants’ removal as 34?±?8%, 31?±?20%, 38?±?10%, and 52?±?6% of fluoranthene, benzo(b)fluoranthene, benzo(a)pyrene, and nonylphenols were dissipated, respectively. Moreover, the accessibility of PAH and NP expressed by their presence in the various sludge organic matter fractions and its evolution during both treatments was linked to both the quality evolution of the organic matter and the physicochemical properties of the PAH and NP; the presence in most accessible fractions explained the amount of PAH and NP dissipated.

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9.
Two birch clones originating from metal-contaminated sites were exposed for 3 months to soils (sand-peat ratio 1:1 or 4:1) spiked with a mixture of polyaromatic hydrocarbons (PAHs; anthracene, fluoranthene, phenanthrene, pyrene). PAH degradation differed between the two birch clones and also by the soil type. The statistically most significant elimination (p ≤ 0.01), i.e. 88% of total PAHs, was observed in the more sandy soil planted with birch, the clearest positive effect being found with Betula pubescens clone on phenanthrene. PAHs and soil composition had rather small effects on birch protein complement. Three proteins with clonal differences were identified: ferritin-like protein, auxin-induced protein and peroxidase. Differences in planted and non-planted soils were detected in bacterial communities by 16S rRNA T-RFLP, and the overall bacterial community structures were diverse. Even though both represent complex systems, trees and rhizoidal microbes in combination can provide interesting possibilities for bioremediation of PAH-polluted soils.  相似文献   

10.
The concentrations of 15 priority PAHs were determined in the atmospheric gaseous and particulate phases from nine sites across Assiut City, Egypt. While naphthalene, acenaphthene, and fluorene were the most abundant in the gaseous phase with average concentrations of 377, 184, and 181 ng/m3, benzo[b]fluoranthene, chrysene, and benzo[g,h,i]perylene showed the highest levels in the particulate phase with average concentrations of 76, 6, and 52 ng/m3. The average total atmospheric concentration of target PAHs (1,590 ng/m3) indicates that Assiut is one of the highest PAH-contaminated areas in the world. Statistical analysis revealed a significant difference between the levels of PAHs in the atmosphere of urban and suburban sites (P?=?0.029 and 0.043 for gaseous and particulate phases, respectively). Investigation of diagnostic PAH concentration ratios revealed vehicular combustion and traffic exhaust emissions as the major sources of PAHs with a higher contribution of gasoline rather than diesel vehicles in the sampled areas. Benzo[a]pyrene has the highest contribution (average?=?32, 4 % for gaseous and particulate phases) to the total carcinogenic activity (TCA) of atmospheric PAHs. While particulate phase PAHs have higher contribution to the TCA, gaseous phase PAHs present at higher concentrations in the atmosphere are more capable of undergoing atmospheric reactions to form more toxic derivatives.  相似文献   

11.
The feasibility of a two-step treatment process has been assessed at laboratory scale for the remediation of soil contaminated with a model mixture of polycyclic aromatic hydrocarbons (PAHs) (phenanthrene, pyrene, and fluoranthene). The initial step of the process involved contacting contaminated soil with thermoplastic, polymeric pellets (polyurethane). The ability of three different mobilizing agents (water, surfactant (Biosolve) and isopropyl alcohol) to enhance recovery of PAHs from soil was investigated and the results were compared to the recovery of PAHs from dry soil. The presence of isopropyl alcohol had the greatest impact on PAH recovery with approximately 80% of the original mass of PAHs in the soil being absorbed by the polymer pellets in 48 h. The second stage of the suggested treatment involved regeneration of the PAH loaded polymers via PAH biodegradation, which was carried out in a solid-liquid two-phase partitioning bioreactor. In addition to the PAH containing polymer pellets, the bioreactor contained a microbial consortium that was pre-selected for its ability to degrade the model PAHs and after a 14 d period approximately 78%, 62% and 36% of phenanthrene, pyrene, and fluoranthene, respectively, had been desorbed from the polymer and degraded. The rate of phenanthrene degradation was shown to be limited by mass transfer of phenanthrene from the polymer pellets. In case of pyrene and fluoranthene a combination of mass transfer and biodegradation rate might have been limiting.  相似文献   

12.
Polycyclic aromatic hydrocarbons (PAHs) were quantified in 30 soil profiles from the Yangtze River Delta Region, in east China. Relative concentrations of PAH compounds with different benzene rings and ratios of fluoranthene to fluoranthene plus pyrene and benz(a)anthracene to benz(a)anthracene plus chrysene were used to identify the possible sources of soil PAHs. Total concentrations of 15 PAHs in topsoils ranged from 8.6 to 3881 microg kg(-1) with an average of 397 microg kg(-1). Half of the soil samples were considered to be contaminated with PAHs (>200 microg kg(-1)) and two sampling sites were heavily polluted by PAHs with concentrations >1000 microg kg(-1). Phenanthrene was found in soils below a depth of 100 cm in half of the sampling sites, but the detectable ratio of benzo(a)pyrene decreased sharply from 100% in topsoil to 0 in the 4th horizon.  相似文献   

13.
Triolein embedded cellulose acetate membrane (TECAM) was used for passive sampling of the fraction of naphthalene, phenanthrene, pyrene and benzo[a]pyrene in 18 field-contaminated soils. The sampling process of PAHs by TECAM fitted well with a first-order kinetics model and PAHs reached 95% of equilibrium in TECAM within 20 h. Concentrations of PAHs in TECAM (CTECAM) correlated well with the concentrations in soils (r2 = 0.693-0.962, p < 0.001). Furthermore, concentrations of PAHs determined in the soil solution were very close to the values estimated by CTECAM and the partition coefficient between TECAM and water (KTECAM-w). After lipid normalization nearly 1:1 relationships were observed between PAH concentrations in TECAMs and earthworms exposed to the soils (r2 = 0.591-0.824, n = 18, p < 0.01). These results suggest that TECAM can be a useful tool to predict bioavailability of PAHs in field-contaminated soils.  相似文献   

14.
Liu Y  Yu N  Li Z  Wei Y  Ma L  Zhao J 《Chemosphere》2012,89(7):893-899
Concentrations of polycyclic aromatic hydrocarbons (PAHs) were detected in sediment cores and surface sediment samples from the Liangtan River of Chongqing, Southwest China. The total concentration of 16 PAHs ranged from 69 to 6251 ng g−1. The spatial distribution of the PAHs reflects the intensity and scope of human activity in the catchment. A historical record of PAH contamination was reconstructed using a sediment core from a background segment of the river. The characteristic changes of concentrations, fluxes and patterns of 16 PAHs over the past ∼90 years were captured in detail. An obvious peak of PAH concentration and flux was found in the 1940s, i.e., during war time, and then a sharp increase was observed from the early 1980s to the present. The maximum concentration and flux reached 1260 ng g−1 and 470 ng cm−2 year−1, respectively. The sharp increase was attributed to the contribution of pyrogenic sources of PAHs. The population, length of highways and energy consumption of Chongqing, as indexes of socioeconomic development, were positively correlated with PAH input in the sediment core from the 1950s to the present. The results clearly show that the local socioeconomic development in the last decades remarkably aggravated the environmental load of sedimentary PAHs.  相似文献   

15.
Hydrocarbon deposition and soil microflora as affected by highway traffic.   总被引:3,自引:0,他引:3  
The proximity of a busy highway (90,000 vehicles/day) increased the amount of polycyclic aromatic hydrocarbons (PAHs) in soil at the depth of 5-15 cm from 106 ng/g as a grassland background to 3095 ng/g dry soil at the highway verge (a sum of 10 PAH species). The PAH concentration was related to the distance from the source and exhibited a biphasic character, which is interpreted in terms of bimodal distribution of the exhaust microparticles with different rates of deposition. Similarly, the tendency of benz(a)anthracene, chrysene, benzo(b)fluoranthene, benzo(k)fluoranthene, and indeno(1,2,3-cd)pyrene to decrease their proportion with distance from the highway, in contrast to phenanthrene, fluoranthene, pyrene, benzo(a)pyrene, and benzo(g,h,i)perylene, was attributed to their prevalent localisation on the heavier particle fraction. The abundance of bacteria (8.33 x background) and fungi (3.17 x background) close to the highway is thought to be a consequence of hydrocarbon deposition from the traffic that serves as a significant energetic input into the soil. The elevated concentrations of hydrocarbon substrates, as indicated by PAHs, increased both the absolute and relative numbers of the microbial degraders of diesel fuel, biphenyl, naphthalene, and pyrene. Their maximum numbers at 0.5-1.5 m from the pavement reached 1.3 x 10(4), 1.2 x 10(5), 1.1 x 10(4), and 6.6 x 10(3) colony-forming units (CFU) or infection units per gramme dry soil, respectively. On the other hand, the number of anthracene degraders (1.1 x 10(3) CFU per g dry soil) remained close to the detection limit of the enumeration technique used (0.1-0.2 x 10(3) per g dry soil), consistently with the absence of anthracene and higher linear PAHs in the investigated soil samples. The amounts of persisting PAHs justify artificial inoculation with effective degrader strains in the vicinity of motorways.  相似文献   

16.
Polycyclic aromatic hydrocarbons (PAHs) in a sediment core taken from intertidal flat in the Yangtze Estuary were determined by gas chromatography-mass spectrometry. The results indicate that the total concentration of PAHs ranged from 0.08 to 11.74 microg/g. The concentration levels of total and individual PAHs changed dramatically with depth. The concentrations of PAHs were relatively high above 35 cm depth and remained constantly low below this depth. The historical record of PAHs in the core shows subsurface maximum (one or more peak values), followed by decreased levels to the surface and with depth. And, PAH sediment record in the core profile is in agreement with historically sewage discharge events during the 1980s to 1990s. The distribution of target molecule acenephthene, the fluoranthene/pyrene ratio, the proportion of 2-3-ring and 4-5-ring PAHs, and alkylated naphthalene to parent naphthalene in the core profile show that the sources in this area are characterized by petroleum-derived PAH contamination (mainly sewage discharge and the river runoff) and the incorporation of atmospheric inputs. Studies indicate the PAH profile pattern in this site in comparison with other regions appear to reflect its particular local position (near the sewage outlet). Moreover, physico-chemical conditions and sedimentation rate as well as biodegradation also affect the PAH concentration levels in the core sediments.  相似文献   

17.
A new gravel-contact assay using rainbow trout, Oncorhynchus mykiss, embryos was developed to assess the toxicity of polycyclic aromatic hydrocarbons (PAHs) and other hydrophobic compounds. Environmentally realistic exposure conditions were mimicked with a direct exposure of eyed rainbow trout embryos incubated onto chemical-spiked gravels until hatching at 10 °C. Several endpoints were recorded including survival, hatching delay, hatching success, biometry, developmental abnormalities, and DNA damage (comet and micronucleus assays). This bioassay was firstly tested with two model PAHs, fluoranthene and benzo[a]pyrene. Then, the method was applied to compare the toxicity of three PAH complex mixtures characterized by different PAH compositions: a pyrolytic extract from a PAH-contaminated sediment (Seine estuary, France) and two petrogenic extracts from Arabian Light and Erika oils, at two environmental concentrations, 3 and 10 μg g?1 sum of PAHs. The degree and spectrum of toxicity were different according to the extract considered. Acute effects including embryo mortality and decreased hatching success were observed only for Erika oil extract. Arabian Light and pyrolytic extracts induced mainly sublethal effects including reduced larvae size and hemorrhages. Arabian Light and Erika extracts both induced repairable DNA damage as revealed by the comet assay versus the micronucleus assay. The concentration and proportion of methylphenanthrenes and methylanthracenes appeared to drive the toxicity of the three PAH fractions tested, featuring a toxic gradient as follows: pyrolytic?Arabian Light?Erika. The minimal concentration causing developmental defects was as low as 0.7 μg g?1 sum of PAHs, indicating the high sensitivity of the assay and validating its use for toxicity assessment of particle-bound pollutants.  相似文献   

18.
Polycyclic aromatic hydrocarbons in the sediments of the South China Sea   总被引:22,自引:0,他引:22  
Sixteen sediment samples, collected from the South China Sea, were analyzed for 11 parent polycyclic aromatic hydrocarbons (PAHs) using gas chromatography and gas chromatography-mass spectrometry. Total concentrations of the 11 PAHs studied in the sediments ranged from 24.7 to 275.4 ng/g with a mean of 145.9 ng/g dry sediment. PAH concentrations displayed a consistent distribution trend with the sediment organic carbon content. The linear regression analysis showed that the total concentration of PAHs in the sediment was significantly correlated to the sediment organic carbon content with a correlation coefficient of 0.735 (n=16). Special PAH compound ratios, such as phenanthrene/anthracene and fluoranthene/pyrene, were calculated to evaluate the relative importance of different origins. The collected data showed that pyrolytic input from anthropogenic combustion processes was predominant at almost all the stations investigated. Only one station, located in the proximity of oil wells, appeared to be contaminated predominantly by petrogenic input. Three anthropogenic PAHs, i.e. pyrene, benzo[a]pyrene and benzo[e]pyrene, exhibited similar distribution patterns in the studied area, implying that these compounds possess identical sources. However, perylene did not entirely follow the distribution trend of the three PAHs, suggesting that the sediment perylene probably derived from other sources such as in situ biogenic origins. Dibenzothiophene, a sulfur heterocyclic aromatic compound, was also measured in this study.  相似文献   

19.
Polyaromatic hydrocarbons (PAHs) are emitted from a variety of sources and can accumulate on and within surface soil layers. To investigate the level of potential risk posed by surface contaminated soils, vertical soil column experiments were conducted to assess the mobility, when leached with simulated rainwater, of six selected PAHs (naphthalene, phenanthrene, fluoranthene, pyrene, benzo(e)pyrene and benzo(ghi)perylene) with contrasting hydrophobic characteristics and molecular weights/sizes. The only PAH found in the leachate within the experimental period of 26 days was naphthalene. The lack of migration of the other applied PAHs was consistent with their low mobilities within the soil columns which generally paralleled their log K oc values. Thus, only 2.3 % of fluoranthene, 1.8 % of pyrene, 0.2 % of benzo(e)pyrene and 0.4 % of benzo(ghi)perylene were translocated below the surface layer. The PAH distributions in the soil columns followed decreasing power relationships with 90 % reductions in the starting levels being shown to occur within a maximum average depth of 0.94 cm compared to an average starting depth of 0.5 cm. A simple predictive model identifies the extensive time periods, in excess of 10 years, required to mobilise 50 % of the benzo(e)pyrene and benzo(ghi)perylene from the surface soil layer. Although this reduces to between 2 and 7 years for fluoranthene and pyrene, it is concluded that the possibility of surface-applied PAHs reaching and contaminating a groundwater aquifer is unlikely.  相似文献   

20.
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