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1.
The effects of monoterpenes on the degradation of 14C-2,4-dichlorophenol (DCP) were investigated in soils collected from areas surrounding monoterpene and non-monoterpene-emitting vegetation. Indigenous microorganisms degraded 14C-2,4-DCP to 14CO2, after 1 d contact time. Degradation was enhanced by prior exposure of the soils to 2,4-DCP for 32 d, increasing extents of mineralisation up to 60%. Monoterpene amendments further enhanced 2,4-DCP degradation, but only following pre-exposure to both 2,4-DCP and monoterpene, with total 2,4-DCP mineralisation extents of up to 71%. Degradation was greatest at the higher monoterpene concentrations (≥1 μg kg−1). Total mineralisation extents were similar between concentrations, but higher than the control and the 0.1 μg kg−1 amendment, indicating that increases in monoterpene concentration has a diminishing enhancing effect. We suggest that monoterpenes can stimulate the biodegradation of 2,4-DCP by indigenous soil microorganisms and that monoterpene amendment in soils is an effective strategy for removing organic contaminants.  相似文献   

2.
We evaluated the catalytic activity of a water-soluble iron-porphyrin in an oxidative coupling reaction to form covalent bonds between 2,4-dichlorophenol (2,4-DCP) and humic molecules. The biomimetic catalysis in the presence of H2O2 was tested in the dark and in daylight, and changes in reaction products were revealed by high-performance liquid chromatography (HPLC) and nuclear magnetic resonance (NMR) spectroscopy. In all conditions, iron-porphyrin was effective in promoting complete disappearance of 2,4-DCP, although catalyst activity was enhanced in daylight (with a maximum turnover number of 85.13). Further evidence of the occurred covalent coupling between 2,4-DCP and humic molecules was revealed by diffusion-ordered nuclear magnetic resonance (DOSY-NMR) spectroscopy that showed a reduced diffusivity of 2,4-DCP after the catalytic reaction. These findings indicate that iron-porphyrin is an efficient catalyst for the covalent binding of polyhalogenated phenols to humic molecules, thereby suggesting that the copolymerization reactions may become a useful technology to remediate soils and waters contaminated by halogenated phenols and their analogues.  相似文献   

3.
2,4-Dichlorophenol (2,4-DCP) is widely distributed in wastewaters discharged from several industries, and it is considered as a priority pollutant due to its high toxicity. In this study, the use of different peroxidase extracts for 2,4-DCP removal from aqueous solutions was investigated. Tobacco hairy roots (HRs), wild-type (WT), and double-transgenic (DT) for tomato basic peroxidases (TPX1 and TPX2) were used to obtain different peroxidase extracts: total peroxidases (TPx), soluble peroxidases (SPx), and peroxidases ionically bound to the cell wall (IBPx). All extracts derived from DT HRs exhibited higher peroxidase activity than those obtained from WT HRs. TPx and IBPx DT extracts showed the highest catalytic efficiency values. The optimal conditions for 2,4-DCP oxidation were pH 6.5, H2O2 0.5 mM, and 200 U mL?1 of enzyme, for all extracts analyzed. Although both TPx extracts were able to oxidize different 2,4-DCP concentrations, the removal efficiency was higher for TPx DT. Polyethylene glycol addition slightly improved 2,4-DCP removal efficiency, and it showed some protective effect on TPx WT after 2,4-DCP oxidation. In addition, using Lactuca sativa test, a reduction of the toxicity of post removal solutions was observed, for both TPx extracts. The results demonstrate that TPx extracts from both tobacco HRs appear to be promising candidate for future applications in removing 2,4-DCP from wastewaters. This is particularly true considering that these peroxidase sources are associated with low costs and are readily available. However, TPx DT has increased peroxidase activity, catalytic efficiency, and higher removal efficiency than TPx WT, probably due to the expression of TPX1 and TPX2 isoenzymes.  相似文献   

4.
Jin X  Zha J  Xu Y  Wang Z  Kumaran SS 《Chemosphere》2011,84(10):1506-1511
2,4-Dichlorophenol (2,4-DCP) is known as an important chemical intermediate and an environmental endocrine disruptor. There is no paper dealing with the predicted no-effect concentration (PNEC) of 2,4-DCP, mainly due to shortage of chronic and site-specific toxicity data. In the present study, toxicity data was obtained from the tests using six Chinese native aquatic species. The HC5 (hazardous concentration for 5% of species) was derived based on the constructed species sensitivity distribution (SSD), which was compared with that derived from literature toxicity data of non-native species. For invertebrates, the survival no-observed effect concentrations (NOECs) were 0.05 and 1.00 mg L−1 for Macrobrachium superbum and Corbicula fluminea, respectively. NOECs based on fishes’ growth were 0.10, 0.20 and 0.40 mg L−1 for Mylopharyngodon piceus, Plagiognathops microlepis and Erythroculter ilishaeformis, respectively. For aquatic plant Soirodela polyrhiza, NOEC based on concentration of chlorophyll was 1.00 mg L−1. A final PNEC calculated using the SSD approach with a 50% certainty based on different taxa ranged between 0.008 and 0.045 mg L−1. There is no significant difference between HC5 derived from native and that from non-native taxa.  相似文献   

5.
Photoelectrocatalysis driven by visible light offers a new and potentially powerful technology for the remediation of water contaminated by organo-xenobiotics. In this study, the performance of a visible light-driven photoelectrocatalytic (PEC) batch reactor, applying a tungsten trioxide (WO3) photoelectrode, to degrade the model pollutant 2,4-dichlorophenol (2,4-DCP) was monitored both by toxicological assessment (biosensing) and chemical analysis. The bacterial biosensor used to assess the presence of toxicity of the parent molecule and its breakdown products was a multicopy plasmid lux-marked E. coli HB101 pUCD607. The bacterial biosensor traced the removal of 2,4-DCP, and in some case, its toxicity response suggests the identification of transient toxic intermediates. The loss of the parent molecule, 2,4-DCP determined by HPLC, corresponded to the recorded photocurrents. Photoelectrocatalysis offers considerable potential for the remediation of chlorinated hydrocarbons, and that the biosensor based toxicity results identified likely compatibility of this technology with conventional, biological wastewater treatment.  相似文献   

6.
Wu BZ  Chen HY  Wang SJ  Wai CM  Liao W  Chiu K 《Chemosphere》2012,88(7):757-768
Technologies such as thermal, oxidative, reductive, and microbial methods for the remediation of polychlorinated biphenyls (PCBs) have previously been reviewed. Based on energy consumption, formation of PCDD/F, and remediation efficiency, reductive methods have emerged as being advantageous for remediation of PCBs. However, many new developments in this field have not been systematically reviewed. Therefore, reductive technologies published in the last decade related to remediation of PCBs will be reviewed here. Three categories, including catalytic hydrodechlorination with H2, Fe-based reductive dechlorination, and other reductive dechlorination methods (e.g., hydrogen-transfer dechlorination, base-catalyzed dechlorination, and sodium dispersion) are specifically reviewed. In addition, the advantages of each remediation technology are discussed. In this review, 108 articles are referenced.  相似文献   

7.
Wang SG  Liu XW  Zhang HY  Gong WX  Sun XF  Gao BY 《Chemosphere》2007,69(5):769-775
Development of aerobic granules for the biological degradation of 2,4-dichlorophenol (2,4-DCP) in a sequencing batch reactor was reported. A key strategy was involving the addition of glucose as a co-substrate and step increase in influent 2,4-DCP concentration. After operation of 39d, stable granules with a diameter range of 1-2mm and a clearly defined shape and appearance were obtained. After granulation, the effluent 2,4-DCP and chemical oxygen demand concentrations were 4.8mgl(-1) and 41mgl(-1), with high removal efficiencies of 94% and 95%, respectively. Specific 2,4-DCP biodegradation rates in the granules followed the Haldane model for substrate inhibition, and peaked at 39.6mg2,4-DCPg(-1)VSS(-1)h(-1) at a 2,4-DCP concentration of 105mgl(-1). Efficient degradation of 2,4-DCP by the aerobic granules suggests their potential application in the treatment of industrial wastewater containing chlorophenols and other inhibitory chemicals.  相似文献   

8.
Jeong JY  Kim HK  Kim JH  Park JY 《Chemosphere》2012,89(2):172-178
The present study investigates the performance of the zero valent iron (ZVI, Fe0) packed bed bipolar electrolytic cell for nitrate removal. The packing mixture consists of ZVI as electronically conducting material and silica sand as non-conducting material between main cathode and anode electrodes. In the continuous column experiments for the simulated groundwater (initial nitrate and electrical conductivity of about 30 mg L−1 as N and 300 μS cm−1, respectively), above 99% of nitrate was removed at the applied potential of 600 V with the main anode placed on the bottom of reactor. The influx nitrate was converted to ammonia (20% to maximum 60%) and nitrite (always less than 0.5 mg L−1 as N in the effluent). The optimum packing ratio (v/v) of silica sand to ZVI was found to be 1:1-2:1. Magnetite was observed on the surface of the used ZVI as corrosion product. The reduction at the lower part of the reactor in acidic condition and adsorption at the upper part of the reactor in alkaline condition are the major mechanism of nitrate removal.  相似文献   

9.
Chemical oxidation of cable insulating oil contaminated soil   总被引:2,自引:0,他引:2  
Xu J  Pancras T  Grotenhuis T 《Chemosphere》2011,84(2):272-277
Leaking cable insulating oil is a common source of soil contamination of high-voltage underground electricity cables in many European countries. In situ remediation of these contaminations is very difficult, due to the nature of the contamination and the high concentrations present. Chemical oxidation leads to partial removal of highly contaminated soil, therefore chemical oxidation was investigated and optimized aiming at a subsequent bioremediation treatment. Chemical oxidation of cable oil was studied with liquid H2O2 and solid CaO2 as well as permanganate at pH 1.8, 3.0 and 7.5. Liquid H2O2 most effectively removed cable oil at pH 7.5 (24%). At pH 7.5 poor oil removal of below 5% was observed with solid CaO2 and permanganate within 2 d contact time, whereas 18% and 29% was removed at pH 1.8, respectively. A prolonged contact time of 7 d showed an increased oil removal for permanganate to 19%, such improvement was not observed for CaO2.Liquid H2O2 treatment at pH 7.5 was most effective with a low acid use and was best fit to a subsequent bioremediation treatment. To further optimize in situ chemical oxidation with subsequent bioremediation the effect of the addition of the iron catalyst and a stepwise liquid H2O2 addition was performed. Optimization led to a maximum of 46% cable oil removal with 1469 mM of H2O2, and 6.98 mM Fe(II) chelated with citric acid (H2O2:FeSO4 = 210:1 (mol mol−1). The optimum delivery method was a one step addition of the iron catalyst followed by step wise addition of H2O2.  相似文献   

10.
Quan X  Shi H  Wang J  Qian Y 《Chemosphere》2003,50(8):1069-1074
2,4-Dichlorophenol (2,4-DCP) degrading mixed culture was immobilized in polyvinyl alcohol jel beads and supplemented to sequencing batch reactors (SBR) to treat 2,4-DCP containing wastewater. Impacts of bioaugmentation level on the performance of bioaugmented systems were studied. Results show that inoculum size affected the start-up time of the SBR systems. For the non-augmented SBR system, nine days was needed for the system to start-up, whereas it only took six, four, three and two days for the SBRs with 1.9%, 3.7%, 5.6% and 9.3% immobilized culture, respectively. In addition, bioaugmented SBR systems demonstrated stronger capacity to cope with high 2,4-DCP shock loading than the control system. The control SBR failed to treat 2,4-DCP at 166 mg/l in influent, while the SBR with 1.9% inoculation could successfully cope with 2,4-DCP at 166 mg/l, but failed at 250 mg/l, and the SBR with 3.7%, 5.6% and 9.3% immobilized culture could successfully degrade 250 mg/l 2,4-DCP in feed. Furthermore, the contributions to the removal of 2,4-DCP by the introduced and indigenous culture in an augmented SBR system at various operation stages were investigated. It was found that augmented culture played the primary role in degrading 2,4-DCP at the beginning of system start-up, but after one-month operation, both the indigenous and the introduced culture posed strong ability to degrade 2,4-DCP.  相似文献   

11.
Lim LL  Lynch R 《Chemosphere》2011,82(4):613-620
Methyl tert-butyl ether (MTBE) groundwater remediation projects often require a combination of technologies resulting in increasing the project costs. A cost-effective in situ photocatalytic reactor design, Honeycomb II, is proposed and tested for its efficiency in MTBE degradation at various flows. This study is an intermediate phase of the research in developing an in situ photocatalytic reactor for groundwater remediation. It examines the effect of the operating variables: air and water flow and double passages through Honeycomb II, on the MTBE removal. MTBE vaporisation is affected by not only temperature, Henry’s law constant and air flow to volume ratio but also reactor geometry. The column reactor achieved more than 84% MTBE removal after 8 h at flows equivalent to horizontal groundwater velocities slower than 21.2 cm d−1. Despite the contrasting properties between a photocatalytic indicator methylene blue and MTBE, the reactor efficiency in degrading both compounds showed similar responses towards flow (equivalent groundwater velocity and hydraulic residence time (HRT)). The critical HRT for both compounds was approximately 1 d, which corresponded to a velocity of 21.2 cm d−1. A double pass through both new and used catalysts achieved more than 95% MTBE removal after two passes in 48 h. It also verified that the removal efficiency can be estimated via the sequential order of the removal efficiency of one pass obtained in the laboratory. This study reinforces the potential of this reactor design for in situ groundwater remediation.  相似文献   

12.
Soil washing is a treatment process that can be used to remediate both organic and inorganic pollutants from contaminated soils, sludges, and sediments. A soil washing procedure was evaluated utilizing about 100 g samples of soil that had been field-contaminated with arsenic, chromium, copper, pentachlorophenol (PCP), polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs). The highest level of mobilization/detoxification was achieved in three soil washes with a mixture of 0.1M [S,S]-ethyelnediaminedisuccinate ([S,S]-EDDS) and 2% Brij 98 at pH 9 with 20 min of ultrasonication treatment at room temperature. This combination mobilized 70% of arsenic, 75% of chromium, 80% of copper, 90% of PCP, and 79% of PCDDs and PCDFs, so that the decontaminated soil met the maximum acceptable concentrations of the generic C-level criteria regulated by the Ministère du Développement Durable, de l’Environnement et des Parcs for the Province of Québec, Canada.The organic pollutants were back-extracted from the aqueous suspension with hexane. Heavy metals were virtually completely precipitated from the aqueous washing suspension with Mg0 particles at room temperature. The PCP was detoxified by catalytic hydrodechlorination with a stream of 5% (v/v) H2-supercritical CO2 that transported the organosoluble fraction through a reaction chamber containing 2% Pd/γ-Al2O3.In toto, this soil washing procedure demonstrates that persistent organic pollutants and selected heavy metals can be co-extracted efficiently from a field-contaminated soil with three successive washes with the same soil washing solution containing [S,S]-EDDS and a non-ionic surfactant (Brij 98) in admixture. An industrial-scale ex situ soil washing procedure with a combination of a non-ionic surfactant and a complexing reagent seems to be a plausible remediation technique for this former wooden utility pole storage facility.  相似文献   

13.
Luo Q  Zhang X  Wang H  Qian Y 《Chemosphere》2005,59(9):1289-1298
The poor mobility of organic pollutants in contaminated sites frequently results in slow remediation processes. Organics, especially hydrophobic compounds, are generally retained strongly in soil matrix as a result of sorption, sequestration, or even formation into non-aqueous-phase liquids and their mobility is thus greatly reduced. The objective of this study was to evaluate the feasibility of using non-uniform electrokinetic transport processes to enhance the mobility of organic pollutants in unsaturated soils with no injection reagents. Phenol and 2,4-dichlorophenol (2,4-DCP), and kaolin and a natural sandy loam soil were selected as model organics and soils, respectively. The results showed that non-uniform electrokinetics can accelerate the desorption and movement of phenol and 2,4-DCP in unsaturated soils. Electromigration and electroosmotic flow were the main driving forces, and their role in the mobilization of phenol and 2,4-DCP varied with soil pH. The movement of 2,4-DCP in the sandy loam towards the anode (about 1.0 cmd(-1)V(-1)) was 1.0-1.5 cmd(-1)V(-1) slower than that in the kaolin soil, but about 0.5 cmd(-1)V(-1) greater than that of phenol in the sandy loam. When the sandy loam was adjusted to pH 9.3, the movement of phenol and 2,4-DCP towards the anode was about twice and five times faster than that at pH 7.7, respectively. The results also demonstrated that the movement of phenol and 2,4-DCP in soils can be easily controlled by regulating the operational mode of electric field. It is believed that non-uniform electrokinetics has the potential for practical application to in situ remediation of organics-contaminated sites.  相似文献   

14.
The organic matter present in the concentrate streams generated from reverse osmosis (RO) based municipal wastewater reclamation processes poses environmental and health risks on its disposal to the receiving environment (e.g., estuaries, bays). The potential of a biological activated carbon (BAC) process combined with pre-oxidation using a UVC/H2O2 advanced oxidation process for treating a high salinity (TDS ∼ 10 000 mg L−1) municipal wastewater RO concentrate (ROC) was evaluated at lab scale during 90 d of operation. The combined treatment reduced the UVA254 and colour of the ROC to below those for the influent of the RO process (i.e., biologically treated secondary effluent), and the reductions in DOC and COD were approximately 60% and 50%, respectively. UVC/H2O2 was demonstrated to be an effective means of converting the recalcitrant organic compounds in the ROC into biodegradable substances which were readily removed by the BAC process, leading to a synergistic effect of the combined treatment in degrading the organic matter. The tests using various BAC feed concentrations suggested that the biological treatment was robust and consistent for treating the high salinity ROC. Using Microtox analysis no toxicity was detected for the ROC after the combined treatment, and the trihalomethane formation potential was reduced from 3.5 to 2.8 mg L−1.  相似文献   

15.
The development of slow-release chemical oxidants for sub-surface remediation is a relatively new technology. Our objective was to develop slow-release persulfate-paraffin candles to treat BTEX-contaminated groundwater. Laboratory-scale candles were prepared by heating and mixing Na2S2O8 with paraffin in a 2.25 to 1 ratio (w/w), and then pouring the heated mixture into circular molds that were 2.38 cm long and either 0.71 or 1.27 cm in diameter. Activator candles were prepared with FeSO4 or zerovalent iron (ZVI) and wax. By treating benzoic acid and BTEX compounds with slow-release persulfate and ZVI candles, we observed rapid transformation of all contaminants. By using 14C-labeled benzoic acid and benzene, we also confirmed mineralization (conversion to CO2) upon exposure to the candles. As the candles aged and were repeatedly exposed to fresh solutions, contaminant transformation rates slowed and removal rates became more linear (zero-order); this change in transformation kinetics mimicked the observed dissolution rates of the candles. By stacking persulfate and ZVI candles on top of each other in a saturated sand tank (14 × 14 × 2.5 cm) and spatially sampling around the candles with time, the dissolution patterns of the candles and zone of influence were determined. Results showed that as the candles dissolved and persulfate and iron diffused out into the sand matrix, benzoic acid or benzene concentrations (Co = 1 mM) decreased by >90% within 7 d. These results support the use of slow-release persulfate and ZVI candles as a means of treating BTEX compounds in contaminated groundwater.  相似文献   

16.
Oxidation of bisphenol F (BPF) by manganese dioxide   总被引:1,自引:0,他引:1  
Bisphenol F (BPF), an environmental estrogen, is used as a monomer in plastic industry and its environmental fate and decontamination are emerging concern. This study focused on the kinetics, influencing factors and pathways of its oxidation by MnO2. At pH 5.5, about 90% of BPF was oxidized in 20 min in a solution containing 100 μM MnO2 and 4.4 μM BPF. The reaction was pH-dependent, following an order of pH 4.5 > pH 5.5 > pH 8.6 > pH 7.5 > pH 6.5 > pH 9.6. Humic acids inhibited the reaction at low (≤pH 5.5) and high pH (≥pH 8.6) at high concentrations. In addition, metal ions and anions also suppressed the reaction, following the order Mn2+ > Ca2+ > Mg2+ > Na+ and HPO42− > Cl > NO3 ≈ SO42−, respectively. A total of 5 products were identified, from which a tentative pathway was proposed.  相似文献   

17.
Dieldrin, one of persistent pesticides, is highly resistant to biotic and abiotic degradation. It is accumulated in organisms. Recent studies suggest that dieldrin exerts a potent cytotoxic action on cells exposed to oxidative stress. In this study, the effect of dieldrin on rat thymocytes exposed to hydrogen peroxide (H2O2)-induced oxidative stress was examined. Dieldrin at 5 μM and H2O2 at 300 μM slightly increased cell lethality from a control value of 5.4 ± 0.5% (mean ± standard deviation of four experiments) to 7.8 ± 1.3% and 9.0 ± 0.3%, respectively. Simultaneous application of dieldrin and H2O2 significantly increased cell lethality to 46.2 ± 1.8%. The synergistic increase in cell lethality was dependent on dieldrin concentration (0.3–5 μM) but not on H2O2 concentration (30–300 μM). Dieldrin accelerated H2O2-induced cell death, which was estimated with the help of annexin V-FITC and propidium iodide. Presence of either dieldrin or H2O2 decreased the cellular content of nonprotein thiol and increased intracellular Zn2+ concentration. The combination of dieldrin and H2O2 further pronounced these effects. TPEN, a chelator of intracellular Zn2+, significantly attenuated the synergistic increase in cell lethality induced by dieldrin and H2O2. It is, therefore, suggested that dieldrin augments the cytotoxicity of H2O2 in a Zn2+-dependent manner.  相似文献   

18.
The effect of the addition of materials on the leaching pattern of As and metals (Cu, Zn, Ni, Pb, and Cd) in two contaminated soils was investigated. The examined materials included bentonites, silicates and industrial wastes, such as sugar foam, fly ashes and a material originated from the zeolitization of fly ash. Soil + material mixtures were prepared at 10% doses. Changes in the acid neutralization capacity, crystalline phases and contaminant leaching over a wide range of pHs were examined by using pHstat leaching tests. Sugar foam, the zeolitic material and MX-80 bentonite produced the greatest decrease in the leaching of pollutants due to an increase in the pH and/or the sorption capacity in the resulting mixture. This finding suggests that soil remediation may be a feasible option for the reuse of non-hazardous wastes.  相似文献   

19.
The kinetics of the catalytic hydrodechlorination (HDC) process of selected dichlorobenzenes (DCBs), dichlorotoluenes (DCTs) and dichlorodiphenyls (DCDs) was studied in the presence of a sulphided carbon-supported Ni-Mo catalyst. The HDC runs were performed in a magnetic stirred batch reactor in the range of 210-230 °C under the hydrogen pressure of 3 MPa. The kinetic constants were evaluated and the reaction network was proposed assuming the pseudo-first order kinetics of dechlorination process. The HDC of aromatic dichloroderivatives proceeded via a network of sequential-parallel reactions. At 210 °C DCBs, DCTs and DCDs followed mainly the pathway of direct transformation to respective aromatic hydrocarbon. At 230 °C, the contribution of sequential dechlorination to monochloroderivative became more predominant.  相似文献   

20.
Liu X  Zhao W  Sun K  Zhang G  Zhao Y 《Chemosphere》2011,82(5):773-777
The conventional hydrothermal reaction with iron powder, NaOH and H2O as reactants was reported to occur at temperature above 423 K, and iron oxides (Fe3O4 and NaFeO2) and hydrogen were produced. In this study, microwave heating was adopted to take the place of conventional heating to induce the hydrothermal reaction. Under microwave irradiation, NaOH and H2O absorbed microwave energy by space charge polarization and dipolar polarization and instantly converted it into thermal energy, which initiated the hydrothermal reaction that involved with zero-valent iron. X-ray diffraction (XRD) analysis found Fe3O4/NaFeO2 and confirmed the occurrence of microwave-induced hydrothermal reaction. The developed microwave-hydrothermal reaction was employed for the dechlorination of PCBs. Hexadecane containing 100 mg L−1 of Aroclor1254 was used as simulative transformer oil, and the dechlorination of PCBs was evaluated by GC/ECD, GC/MS and ion chromatography. For PCBs in 10 mL simulative transformer oil, almost complete dechlorination was achieved by 750 W microwave irradiation for 10 min, with 0.3 g iron powder, 0.3 g NaOH and 0.6 mL H2O added. The effects of important factors including microwave power and the amounts of reactants added, on the dechlorination degree were investigated, moreover, the dechlorination mechanism was suggested. Microwave irradiation combined with the common and cheap materials, iron powder, NaOH and H2O, might provide a fast and cost-effective method for the treatment of PCBs-containing wastes.  相似文献   

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