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1.
Relationships between sedimentary organic matter (SOM) composition and PAH desorption behavior were determined for vegetated and non-vegetated refinery distillate waste sediments. Sediments were fractionated into size, density, and humin fractions and analyzed for their organic matter content. Bulk sediment and humin fractions differed more in organic matter composition than size/density fractions. Vegetated humin and bulk sediments contained more polar organic carbon, black carbon, and modern (plant) carbon than non-vegetated sediment fractions. Desorption kinetics of phenanthrene, pyrene, chrysene, and C3-phenanthrene/anthracenes from humin and bulk sediments were investigated using Tenax® beads and a two-compartment, first-order kinetic model. PAH desorption from distillate waste sediments appeared to be controlled by the slow desorbing fractions of sediment; rate constants were similar to literature values for kslow and kvery slow. After several decades of plant colonization and growth (Phragmites australis), vegetated sediment fractions more extensively desorbed PAHs and had faster desorption kinetics than non-vegetated sediment fractions.  相似文献   

2.
《Chemosphere》1987,16(10-12)
The presence of polychlorinated biphenyls (PCBs) was investigated in samples of water, suspended particles, sediments and fish from the Kupa river, Croatia, Yugoslavia, along a river stretch extending up to 10 km upstream and 200 km downstream of the primary contaminated karst region. Contamination was due to improper disposal of industrial waste discharge. The PCB levels detected in the samples collected downstream ranged from 1 to 52 ng 1−1 for water, from 50 to 190 μg kg−1 for suspended particles and from 8 to 39 μg kg−1 for the sediment. A wide range of PCB concentrations, from 0.1 to 42.3 μg g−1, which were measured in edible portions of different fish confirmed a long-term contamination of the river with PCBs. As the Kupa may be classified among low to moderately contaminated waters, it is essential that the investigations of the presence and behaviour of PCBs in the river and its environment be continued.  相似文献   

3.
As one of China’s great metropolises, Taiyuan is affected by heavy chemical industry and manufacture of chemical products, and faces pollution from polychlorinated biphenyls (PCBs). Therefore, this study was conducted to determine the PCB concentrations in various environmental media in Taiyuan. We collected 15 soil samples, 34 respirable particulate matter (PM) samples (17 of PM2.5 and 17 of PM10) from urban areas of Taiyuan, and measured a total of 144 PCB congeners (including some coeluting PCB congeners). The total PCB concentrations were 51–4.7 × 103 pg g−1 in soil, 27–1.4 × 102 pg m−3 in PM2.5 and 16–1.9 × 102 pg m−3 in PM10. Of the PCB homologues, the dominant PCBs detected in the various media were all tri-CBs. Soil was relatively the most polluted media. Furthermore, principal-component analysis revealed that the major PCB source in Taiyuan may be associated with the main commercial PCB through long-range transmission. Toxic equivalency (TEQ) concentrations (based on ten dioxin-like PCBs) ranged from N.D. to 5.9 × 10−3 pg-WHO TEQ g−1 in soil, 2.0 × 10−4–3.4 × 10−3 pg-WHO TEQ m−3 and 1.0 × 10−4–1.2 × 10−3 pg-WHO TEQ m−3 in PM2.5 and PM10, respectively. In previous studies, PCBs were not a severe component of contaminant in Taiyuan; however, this study suggested there is a potential threat of human exposure to PCBs for residents of Taiyuan.  相似文献   

4.
Lake sediments contaminated with polychlorinated biphenyls (PCBs) were purged using a gas stripping technique to estimate desorption rate constants. Desorption profiles and modeling of the data clearly show a two-step release of PCBs from sediment suspensions that can be described as a labile (fast) release followed by a non-labile (slow) release. Data are summarized by labile and non-labile rate constants and by mass in each phase as a function of suspended solids concentration for twelve pure congeners and nine co-eluting data sets (twenty-one chromatograph peaks total). Labile desorption rate constants range from 113 days(-1) to 1.43 days(-1) for the 100 mg/l sediment suspension, from 67.7 days(-1) to 2.45 days(-1) for the 1000 mg/l sediment suspension, and from 8.41 days(-1) to 0.946 days(-1) for the 5000 mg/l sediment suspension. Labile rate constants consistently decreased with increasing suspended solids, and, in general, decreased with increasing degree of chlorination (reflected in increasing retention time in the chromatogram). No consistent trend was observed for the non-labile rate constants with suspended solids concentration or degree of chlorination. The average non-labile rate constant for the PCB congeners studied here was 0.154 days(-1) (s.d.=0.158; n=63). The distribution between the labile and non-labile phases also failed to indicate dependence on suspended solids concentration, chlorine substitution pattern, or molecular weight of the congener, although the data from the 5000 mg/l suspension consistently contained less labile components. The average distributions (n=63) were 60.1% in the labile phase and 39.9% in the non-labile phase.  相似文献   

5.
Twenty-seven surface sediment samples were collected from the mainstream and eight tributaries of the Wuhan reach of the Yangtze River, China, in 2005, in order to assess the distribution, possible sources, and potential risk of polychlorinated biphenyls (PCBs) in the environment. The total concentrations of PCBs (the sum of 39 congeners) ranged from 1.2 to 45.1 ng g−1 dry weight, with a mean value of 9.2 ng g−1. Sediment samples with the highest PCB concentrations came from the tributary sites, which are closer to PCB sources. Conversely, PCB concentrations in the sediment from the mainstream sites of Yangtze River were relatively low. The observed PCB levels were higher than those found in the sediments of other rivers in China, but lower than those in river sediments from other urban areas and harbors around the world. Low-chlorinated PCBs, dominated by tetra-PCBs and penta-PCBs, were identified as being prevalent in the surface sediments. Correlation analyses between the PCBs and the geochemistry and heavy metal content of the sediments suggest that the washing of these compounds from the land into the river by floods and heavy rains, or industrial wastewater and domestic sewage, may be the major sources of the PCBs. According to established sediment quality guidelines, the risk of adverse biological effects from the levels of PCBs recorded at most of the studied sites should be insignificant, although the higher concentrations at other sites could cause acute biological damage.  相似文献   

6.
At a former wood preservation plant severely contaminated with coal tar oil, in situ bulk attenuation and biodegradation rate constants for several monoaromatic (BTEX) and polyaromatic hydrocarbons (PAH) were determined using (1) classical first order decay models, (2) Michaelis–Menten degradation kinetics (MM), and (3) stable carbon isotopes, for o-xylene and naphthalene. The first order bulk attenuation rate constant for o-xylene was calculated to be 0.0025 d− 1 and a novel stable isotope-based first order model, which also accounted for the respective redox conditions, resulted in a slightly smaller biodegradation rate constant of 0.0019 d− 1. Based on MM-kinetics, the o-xylene concentration decreased with a maximum rate of kmax = 0.1 µg/L/d. The bulk attenuation rate constant of naphthalene retrieved from the classical first order decay model was 0.0038 d− 1. The stable isotope-based biodegradation rate constant of 0.0027 d− 1 was smaller in the reduced zone, while residual naphthalene in the oxic part of the plume further downgradient was degraded at a higher rate of 0.0038 d− 1. With MM-kinetics a maximum degradation rate of kmax = 12 µg/L/d was determined. Although best fits were obtained by MM-kinetics, we consider the carbon stable isotope-based approach more appropriate as it is specific for biodegradation (not overall attenuation) and at the same time accounts for the dominant electron-accepting process. For o-xylene a field based isotope enrichment factor εfield of − 1.4 could be determined using the Rayleigh model, which closely matched values from laboratory studies of o-xylene degradation under sulfate-reducing conditions.  相似文献   

7.
Organochlorine pesticide residues and PCBs were measured in bulked samples of whole eels collected in 1991 from 11 reedbed sites of wildlife conservation importance in Britain. Eels from some sites had only trace amounts of dieldrin, p,p-DDE and PCBs. Maximum concentrations were 0.21 mg kg−1 for dieldrin, 0.27 mg kg−1 for p,p-DDE and 0.91mg kg−1 for PCBs (fresh weight). Concentrations of contaminants in eels from reedbeds were considered in general to be lower than in eels from rivers, but nevertheless concentrations were considered to be sufficiently high at some sites to adversely affect top carnivores such as the otter.  相似文献   

8.
9.
Sequential supercritical fluid extraction (SFE) was performed in order to estimate desorption of PAHs from river floodplain soils which contain coal and coal-derived particles. Original soils, soils' light fractions (ρ < 2 g cm−3), and <63 μm fractions were studied for PAHs' desorption kinetics. Desorption data were successfully described using a two-site model. Desorption rate constants were one order of magnitude lower than those of “slow” and “very slow” desorption rates from other studies. This suggests very slow and extremely slow desorption. Estimated time scales releasing 99% of total extractable contaminants ranged from decades for 2-4-ring PAHs and hundreds of years for 5-6-ring PAHs. We demonstrate that, despite high soil PAH concentrations which are due to coal and coal-derived particles, the general environmental risk is reduced by the very slow and extremely slow desorption rates.  相似文献   

10.
Amorphous ferric oxyhydroxide is being used to treat groundwater contaminated with uranium(VI); the compound also has potential for use as a component in in situ chemical barriers. To quantitatively evaluate its effectiveness in such applications, adsorption of uranium(VI) onto amorphous ferric oxyhydroxide was experimentally investigated under a wide range of uranium(VI) (8.40·10−7−2.10·10−3 mol L−1; 0.2–500 mg L−1), sulfur(VI) (0–0.07 mol L−1; 0–2240 mg L−1) and carbon(IV) (0–0.0195 mol L−1; 0–234 mg L−1) concentrations, and pH-values (4–9.6). The adsorption behavior of uranium(VI) (uranyl ion and its complexes) is similar to that of other cations; it exhibits a sharp rise in the extent of adsorption with increasing pH. Interactions among uranyl complexes and surface sites are interpreted using a site complexation model. Although the model does not incorporate electrostatics and includes only a single type of adsorption site, it provides a reasonable match to measured adsorption and proton exchange data. The simplicity of the model and the resulting reduction in computational demand allow its efficient incorporation into coupled reaction-transport models.  相似文献   

11.
PAHs and PCBs were collected simultaneously indoors and outdoors at eight non-smoking homes located in four buildings in high-traffic areas of Rome. The purpose was to evaluate the relevance of indoor air in contributing to the overall exposure of the urban population. The vertical distribution was also investigated by collecting outdoor samples at both road and roof level, and indoor samples in both a high and a low floor flat of each building. At one coal-heated building, samples were collected during both the heating and the non-heating season. No evident PAH source was present indoors. Indoor and outdoor daily concentrations of benzo[a]pyrene (BaP) ranged, respectively, 0.1–4.6 ng m−3 and 0.7–2.3 ng m−3. With the heating on, indoor PAH concentrations equalled or exceeded those outdoors, with BaP indoor/outdoor ratios up to 4; during the warm season, ratios decreased to 0.2–0.6. Indoor PAHs at the low floors exceeded the high-floor ones when the heating was off (vehicle exhausts being the dominant source), while being equal or lower with the heating on; the vertical gradient of indoor PAHs between different floors was within a factor of 2. Outdoor PAHs at roof level were 20–70% of those at road level, which in turn exceeded those at the medium-traffic station up to a factor of 4. The outdoor concentrations of Σ6 indicator PCBs ranged 0.1–1.6 ng m−3. Indoor PCB concentrations exceeded those outdoors by an approximate factor of 2–50. No vertical gradient was observed. The results indicated that indoor air may contribute to the overall exposure to PAHs and PCBs more than the urban air. They were also consistent with recent findings suggesting that indoor air can be a relevant source of PCBs for outdoor air.  相似文献   

12.
Simazine is a s-triazine herbicide that has been applied worldwide for agriculture. This herbicide is the second most commonly detected pesticide in surface and groundwater in the United States, Europe and Australia. In this study, simazine adsorption behaviour was studied in two agricultural soils of the Aconcagua valley, central Chile. The two studied soils were soil A (loam, 8.5% organic matter content) and soil B (clay-loam, 3.5% organic matter content). Three times higher simazine adsorption capacity was observed in soil A (68.03 mg kg−1) compared to soil B (22.03 mg kg−1). The simazine adsorption distribution coefficients (Kd) were 9.32 L kg−1 for soil A and 7.74 L kg−1 for soil B. The simazine adsorption enthalpy in soil A was −21.0 kJ mol−1 while in soil B the adsorption enthalpy value was −11.5 kJ mol−1. These results indicate that simazine adsorption process in these soils is exothermic, governing H bonds the adsorption process of simazine in both the loam and clay-loam soils. These results and the potentiometric profiles of both soils, suggest that simazine adsorption in soil A is mainly governed by simazine–organic matter interactions and in soil B by simazine–clay interactions. The understanding of simazine sorption–desorption processes is essential to determine the pesticide fate and availability in soil for pest control, biodegradation, runoff and leaching.  相似文献   

13.
This study investigated the influence of solution salinity, pH and the sediment characteristics on the sorption and desorption of perfluorooctane sulfonate (PFOS). The results showed that the sorption of PFOS onto sediment increased by a factor of 3 as the CaCl2 concentration increased from 0.005 to 0.5 mol L−1 at pH 7.0, and nearly 6 at pH 8.0. Desorption hysteresis occurred over all salinity. The thermodynamic index of irreversibility (TII) values increased with increasing concentration of CaCl2. Maximum irreversibility was found in the sorption systems with CaCl2 in the concentration of 0.5 mol L−1. The results suggested that PFOS can be largely removed from the water with increasing salinity, and get trapped onto sediments irreversibly. These phenomena could be explained by salting-out effect and Ca-bridging effect. Studies also suggested that the content of total organic carbon is the dominant psychochemical properties of sediment controlling the sorption of PFOS.  相似文献   

14.
Larch forests are distributed extensively in the east Eurasian continent and are expected to play a significant role in the terrestrial ecosystem carbon cycling process. In view of the fact that studies on carbon exchange for this important biome have been very limited, we have initiated a long-term flux observation in a larch forest ecosystem in Hokkaido in northern Japan since 2000. The net ecosystem CO2 exchange (NEE) showed large seasonal and diurnal variation. Generally, the larch forest ecosystem released CO2 in nighttime and assimilated CO2 in daytime during the growing season from May to October. The ecosystem started to become a net carbon sink in May, reaching a maximum carbon uptake as high as 186 g C m−2 month−1 in June. With the yellowing, senescing and leaf fall, the ecosystem turned into a carbon source in November. During the non-growing season, the larch forest ecosystem became a net source of CO2, releasing an average of 16.7 g C m−2 month−1. Overall, the ecosystem sequestered 141–240 g C m−2 yr−1 in 2001. The NEE was significantly influenced by environmental factors. Respiration of the ecosystem, for example, was exponentially dependent on air temperature, while photosynthesis was related to the incident PAR in a manner consistent with the Michaelis–Menten model. Although the vapor pressure deficit (VPD) was scarcely higher than 15 hPa, the CO2 uptake rate was also depressed when VPD surpassed 10 hPa.  相似文献   

15.
Particulate matter having an aerodynamic diameter less than 2.5 μm (PM2.5) is thought to be implicated in a number of medical conditions, including cancer, rheumatoid arthritis, heart attack, and aging. However, very little chemical speciation data is available for the organic fraction of ambient aerosols. A new direct thermal desorption-gas chromatography/mass spectrometry (TD-GC/MS) method was developed for the analysis of the organic fraction of PM2.5. Samples were collected in Golden, British Columbia, over a 15-month period. n-Alkanes constituted 33–98% by mass of the organic compounds identified. PAHs accounted for 1–65% and biomarkers (hopanes and steranes) 1–8% of the organic mass. Annual mean concentrations were: n-alkanes (0.07–1.55 ng m−3), 16 PAHs (0.02–1.83 ng m−3), and biomarkers (0.02–0.18 ng m−3). Daily levels of these organics were 4.89–74.38 ng m−3, 0.27–100.24 ng m−3, 0.14–4.39 ng m−3, respectively. Ratios of organic carbon to elemental carbon (OC/EC) and trends over time were similar to those observed for PM2.5. There was no clear seasonal variation in the distribution of petroleum biomarkers, but elevated levels of other organic species were observed during the winter. Strong correlations between PAHs and EC, and between petroleum biomarkers and EC, suggest a common emission source – most likely motor vehicles and space heating.  相似文献   

16.
The associations of personal carbon monoxide (CO) exposures with ambient air CO concentrations measured at fixed monitoring sites, were studied among 194 children aged 3–6 yr in four downtown and four suburban day-care centers in Helsinki, Finland. Each child carried a personal CO exposure monitor between 1 and 4 times for a time period of between 20 and 24 h. CO concentrations at two fixed monitoring sites were measured simultaneously. The CO concentrations measured at the fixed monitoring sites were usually lower (mean maximum 8-h concentration: 0.9 and 2.6 mg m−3) than the personal CO exposure concentrations (mean maximum 8-h concentration: 3.3 mg m−3). The fixed site CO concentrations were poor predictors of the personal CO exposure concentrations. However, the correlations between the personal CO exposure and the fixed monitoring site CO concentrations increased (−0.03–−0.12 to 0.13–0.16) with increasing averaging times from 1 to 8 h. Also, the fixed monitoring site CO concentrations explained the mean daily or weekly personal CO exposures of a group of simultaneously measured children better than individual exposure CO concentrations. This study suggests that the short-term CO personal exposure of children cannot be meaningfully assessed using fixed monitoring sites.  相似文献   

17.
Diffusion coefficients (T=23±2 °C) and accessible porosities for HTO, 36Cl and 125I were measured on Opalinus Clay (OPA) samples from the Mont Terri Underground Rock Laboratory (URL) using the through-diffusion technique. The direction of transport (diffusion) was perpendicular to bedding. Special cells that allowed the application of confining pressure were designed and constructed. The pressures ranged from 1 to 5 MPa, the latter value simulating the overburden at the Mont Terri URL (about 200 m). The test solution used in the experiments was a synthetic version of the Opalinus Clay pore water, which has Na+ and Cl as the main components (I=0.42 M).The measured values of the effective diffusion coefficients (De) and rock capacity factors (α) are: De=1.2–1.5×10−11 m2 s−1 and α=0.09–0.11 for HTO, De=4.0–5.5×10−12 m2 s−1 and α=0.05 for 36Cl and De=3.2–4.6×10−12 m2 s−1 and α=0.07–0.10 for 125I. For non-sorbing tracers (HTO, 36Cl) the rock capacity factor α is equal to the diffusion-accessible porosity . The experimental results showed that pressure only had a small effect on the value of the diffusion coefficients. Increasing the pressure from 1 to 5 MPa resulted in a decrease of the diffusion coefficient of 17% for HTO, 28% for 36Cl and 30% for 125I. Moreover, the diffusion coefficients for 36Cl and 125I are smaller than for HTO, which is consistent with an effect arising from anion exclusion.The diffusion coefficients of HTO and 125I measured in this study are in good agreement with recent measurements at three other laboratories performed within the framework of a laboratory comparison exercise. The values of the diffusion-accessible porosities show a larger degree of scatter.  相似文献   

18.
The results of tests for the purification of fish oils with activated carbon for industrial use are presented. The optimum parameters for the process of purification (granulation of the activated carbon, its dosage, the oil temperature, and the duration of mixing the oil with activated carbon) were previously established for the laboratory scale. The optimization of the process consisted of selecting purification parameters that would allow for maximum reduction of the toxic polychlorinated dibenzo-para-dioxins and polychlorinated dibenzofurans (PCDD/Fs) content, while retaining the favorable high fatty acid content [C20:5 n−3, eicosapentaenoic acid (EPA) and C22:6 n−3, docosahexaenoic acid (DHA)]. The use of that optimum parameters in industrial conditions confirmed the satisfactory results obtained in laboratory tests. Five types of oil derived from various Baltic fish were purified. Reduction in the PCDD/Fs content was 77.0–93.6% on average, whereas in the dioxin-like polychlorinated biphenyls (dl-PCBs)—it was 42.7–50.5% on average, with insignificant changes in the total amount of EPA and DHA content. Furthermore, a significant reduction in the content of arsenic was noted (by about 62% on average), with insignificant changes in the content of organochlorine pesticides (OCPs), and marker polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), cadmium, lead, and mercury.Purification provided fish oil having standardized parameters that allow for its use as feed additives, whilst retaining its favorable fatty acid content.  相似文献   

19.
Atmospheric transport and deposition of polychlorinated biphenyls (PCBs) is an important problem for ecosystems around the world. Data from several monitoring networks demonstrate that atmospheric PCB concentrations are dramatically elevated in urban areas compared to rural or background regions, such that these urban emissions of PCBs support the regional and global transport and deposition of PCBs to more remote areas. Identifying and controlling the sources of urban atmospheric PCBs is thus essential in minimizing the regional and global transport and deposition of these compounds. From December 1999 to November 2000, gas-phase PCB concentrations were measured at two monitoring locations, 8 km apart, within the New York City metropolitan area, at Jersey City and Bayonne, NJ. Concentrations, congener patterns, and temporal patterns of PCBs differ dramatically at the two sites, suggesting that a significant source of atmospheric PCBs exists within 8 km of the Bayonne site, resulting in spikes in gas-phase PCB concentration at Bayonne that are not observed at Jersey City. The Regional Atmospheric Model System (RAMS) coupled with the Hybrid Particle and Concentration Transport model (HYPACT) was used to estimate that the PCB source near Bayonne emits a flux of ΣPCBs on the order of 100 g d−1. Extrapolation of this source magnitude to the area of New York City suggests that this urban area emits at least 300 kg yr−1 ΣPCBs to the regional atmosphere, similar in magnitude to the flow of ΣPCB out of the Upper Hudson River into the New York/New Jersey Harbor.  相似文献   

20.
Background, aim, and scope  Herbicide fate and its transport in soils and sediments greatly depend upon sorption–desorption processes. Quantitative determination of herbicide sorption–desorption is therefore essential for both the understanding of transport and the sorption equilibrium in the soil/sediment–water system; and it is also an important parameter for predicting herbicide fate using mathematical simulation models. The total soil/sediment organic carbon content and its qualitative characteristics are the most important factors affecting sorption–desorption of herbicides in soil or sediment. Since the acetochlor is one of the most frequently used herbicides in Slovakia to control annual grasses and certain annual broad-leaved weeds in maize and potatoes, and posses various negative health effects on human beings, our aim in this study was to investigate acetochlor sorption and desorption in various soil/sediment samples from Slovakia. The main soil/sediment characteristics governing acetochlor sorption–desorption were also identified. Materials and methods  The sorption–desorption of acetochlor, using the batch equilibration method, was studied on eight surface soils, one subsurface soil and five sediments collected from the Laborec River and three water reservoirs. Soils and sediments were characterized by commonly used methods for their total organic carbon content, distribution of humus components, pH, grain-size distribution, and smectite content, and for calcium carbonate content. The effect of soil/sediment characteristics on acetochlor sorption–desorption was examined by simple correlation analysis. Results  Sorption of acetochlor was expressed as the distribution coefficient (K d). K d values slightly decreased as the initial acetochlor concentration increased. These values indicated that acetochlor was moderately sorbed by soils and sediments. Highly significant correlations between the K d values and the organic carbon content were observed at both initial concentrations. However, sorption of acetochlor was most closely correlated to the humic acid carbon, and less to the fulvic acid carbon. The total organic carbon content was found to also significantly influence acetochlor desorption. Discussion  Since the strong linear relationship between the K d values of acetochlor and the organic carbon content was already released, the corresponding K oc values were calculated. Considerable variation in the K oc values suggested that other soil/sediment parameters besides the total soil organic carbon content could be involved in acetochlor sorption. This was revealed by a significant correlation between the K oc values and the ratio of humic acid carbon to fulvic acid carbon (CHA/CFA). Conclusions  When comparing acetochlor sorption in a range of soils and sediments, different K d values which are strongly correlated to the total organic carbon content were found. Concerning the humus fractions, the humic acid carbon content was strongly correlated to the K d values, and it is therefore a better predictor of the acetochlor sorption than the total organic carbon content. Variation in the K oc values was attributed to the differences in distribution of humus components between soils and sediments. Desorption of acetochlor was significantly influenced by total organic carbon content, with a greater organic carbon content reducing desorption. Recommendations and perspectives  This study examined the sorption–desorption processes of acetochlor in soils and sediments. The obtained sorption data are important for qualitative assessment of acetochlor mobility in natural solids, but further studies must be carried out to understand its environmental fate and transport more thoroughly. Although, the total organic carbon content, the humus fractions of the organic matter and the CHA/CFA ratio were sufficient predictors of the acetochlor sorption–desorption. Further investigations of the structural and chemical characteristics of humic substances derived from different origins are necessary to more preciously explain differences in acetochlor sorption in the soils and sediments observed in this study.  相似文献   

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