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1.
Fe2O3 and CeO2 modified activated coke (AC) synthesized by the equivalent-volume impregnation were employed to remove elemental mercury (Hg0) from simulated flue gas at a low temperature. Effects of the mass ratio of Fe2O3 and CeO2, reaction temperature, and individual flue gas components including O2, NO, SO2, and H2O (g) on Hg0 removal efficiency of impregnated AC were investigated. The samples were characterized by Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). Results showed that with optimal mass percentage of 3 % Fe2O3 and 3 % CeO2 on Fe3Ce3/AC, the Hg0 removal efficiency could reach an average of 88.29 % at 110 °C. Besides, it was observed that O2 and NO exhibited a promotional effect on Hg0 removal, H2O (g) exerted a suppressive effect, and SO2 showed an insignificant inhibition without O2 to some extent. The analysis of XPS indicated that the main species of mercury on used Fe3Ce3/AC was HgO, which implied that adsorption and catalytic oxidation were both included in Hg0 removal. Furthermore, the lattice oxygen, chemisorbed oxygen, and/or weakly bonded oxygen species made a contribution to Hg0 oxidation.  相似文献   

2.
Rare earth (Dy3+ and Sm3+)-doped sodium magnesium borate (NaMgBO3) is synthesized by solution combustion synthesis method keeping their thermoluminescence properties in mind. The reaction produced very stable crystalline NaMgBO3:RE (RE?=?Dy3+, Sm3+) phosphors. The phosphors are exposed to 60Co gamma-ray radiations dose of varying rate from 5 to 25 Gy, and their TL characteristics with kinetic parameters are studied. NaMgBO3:Dy3+ phosphor shows two peaks for lower doping concentration of Dy3+ while it reduced to single peak for the higher concentrations of activator Dy3+. NaMgBO3:Dy3+ shows the major glow peak around 200 °C while NaMgBO3:Sm3+ phosphors show two well-separated glow peaks at 200 and 332 °C respectively. The thermoluminescence intensity of these phosphors was compare with the commercially available TLD-100 (Harshaw) phosphor. The TL responses for gamma-ray radiations dose were found to be linear from 5 to 25 Gy for both phosphors while the fading in each case is calculated for the tenure of 45 days.  相似文献   

3.
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   

4.
More attention has been paid to the deterioration of water bodies polluted by drinking water treatment sludge (DWTS) in recent years. It is important to develop methods to effectively treat DWTS by avoiding secondary pollution. We report herein a novel investigation for recovery of Si and Fe from DWTS, which are used for the synthesis of two iron oxide@SiO2 composites for adsorption of reactive red X-3B (RRX-3B) and NaNO2. The results show that Fe3+ (acid-leaching) and Si4+ (basic-leaching) can be successfully recovered from roasted DWTS. Whether to dissolve Fe(OH)3 precipitation is the key point for obtaining Fe3O4 or γ-Fe2O3 particles using the solvothermal method. The magnetic characteristics of Fe3O4@SiO2 (390.0 m2 g?1) or Fe2O3@SiO2 (220.9 m2 g?1) are slightly influenced by the coated porous SiO2 layer. Peaks of Fe–O stretching vibration (580 cm?1) and asymmetric Si–O–Si stretching vibrations (1080 cm?1) of Fe3O4@SiO2 indicate the successful coating of a thin silica layer (20–150 nm). The adsorption capacity of RRX-3B and NaNO2 by Fe3O4@SiO2 is better than that of Fe2O3@SiO2, and both composites can be recycled through an external magnetic field. This method is an efficient and environmentally friendly method for recycling DWTS.  相似文献   

5.
Gaseous nitrogen dioxide (NO2) represents an oxidant that is present in relatively high concentrations in various indoor settings. Remarkably increased NO2 levels up to 1.5 ppm are associated with homes using gas stoves. The heterogeneous reactions of NO2 with adsorbed water on surfaces lead to the generation of nitrous acid (HONO). Here, we present a HONO source induced by heterogeneous reactions of NO2 with selected indoor paint surfaces in the presence of light (300 nm?<?λ?<?400 nm). We demonstrate that the formation of HONO is much more pronounced at elevated relative humidity. In the presence of light (5.5 W m?2), an increase of HONO production rate of up to 8.6?·?109 molecules cm?2 s?1 was observed at [NO2]?=?60 ppb and 50 % relative humidity (RH). At higher light intensity of 10.6 (W m?2), the HONO production rate increased to 2.1?·?1010 molecules cm?2 s?1. A high NO2 to HONO conversion yield of up to 84 % was observed. This result strongly suggests that a light-driven process of indoor HONO production is operational. This work highlights the potential of paint surfaces to generate HONO within indoor environments by light-induced NO2 heterogeneous reactions.  相似文献   

6.
It has been shown that manganese dioxide (MnO2) can mediate transformation of phenolic contaminants to form phenoxyl radical intermediates, and subsequently, these intermediates intercouple to form oligomers via covalent binding. However, the reaction kinetics and transformation mechanisms of phenolic contaminants with humic molecules present in nano-MnO2-mediated systems were still unclear. In this study, it was proven that nano-MnO2 were effective in transforming triclosan under acidic conditions (pH 3.5–5.0) during manganese reduction, and the apparent pseudo first-order kinetics rate constants (k?=?0.0599–1.5314 h?1) increased as the pH decreased. In particular, the transformation of triclosan by nano-MnO2 was enhanced in the presence of low-concentration humic acid (1–10 mg L?1). The variation in the absorption of humic molecules at 275 nm supported possible covalent binding between humic molecules and triclosan in the nano-MnO2-mediated systems. A total of four main intermediate products were identified by high-resolution mass spectrometry (HRMS), regardless of humic molecules present in the systems or not. These products correspond to a suite of radical intercoupling reactions (dimers and trimers), ether cleavage (2,4-dichlorophenol), and oxidation to quinone-like products, triggered by electron transfer from triclosan molecules to nano-MnO2. A possible reaction pathway in humic acid solutions, including homo-coupling, decomposition, oxidation, and cross-coupling, was proposed. Our findings provide valuable information regarding the environmental fate and transformation mechanism of triclosan by nano-MnO2 in complex water matrices.  相似文献   

7.
The influences of HCO3 ?, Cl?, and other components on the UV/TiO2 degradation of the antineoplastic agents ifosfamide (IFO) and cyclophosphamide (CP) were studied in this work. The results indicated that the presence of HCO3 ?, Cl?, NO3 ?, and SO4 2? in water bodies resulted in lower degradation efficiencies. The half-lives of IFO and CP were 1.2 and 1.1 min and increased 2.3–7.3 and 3.2–6.3 times, respectively, in the presence of the four anions (initial compound concentration = 100 μg/L, TiO2 loading =100 mg/L, anion concentration = 1000 mg/L, and pH = 8). Although the presence of HCO3 ? in the UV/TiO2/HCO3 ? system resulted in a lower degradation rate and less byproduct formation for IFO and CP, two newly identified byproducts, P11 (M.W. = 197) and P12 (M.W. = 101), were formed and detected, suggesting that additional pathways occurred during the reaction of ?CO3 ? in the system. The results also showed that ?CO3 ? likely induces a preferred ketonization pathway. Besides the inorganic anions HCO3 ?, Cl?, NO3 ?, and SO4 2?, the existence of dissolved organic matter in the water has a significant effect and inhibits CP degradation. Toxicity tests showed that higher toxicity occurred in the presence of HCO3 ? or Cl? during UV/TiO2 treatment and within 6 h of reaction time, implying that the effects of these two anions should not be ignored when photocatalytic treatment is applied to treat real wastewater.  相似文献   

8.
The impact of nanoparticles on fish health is still a matter of debate, since nanotechnology is quite recent. In this study, freshwater benthonic juvenile fish Prochilodus lineatus were exposed through water to three concentrations of TiO2 (0.1, 1, and 10 μg l?1) and ZnO (7, 70, and 700 μg l?1) nanoparticles, as well as to a mixture of both (TiO2 1 μg l?1?+?ZnO 70 μg l?1) for 5 and 30 days. Nanoparticle characterization revealed an increase of aggregate size in the function of concentration, but suspensions were generally stable. Fish mortality was high at subchronic exposure to 70 and 700 μg l?1 of ZnO. Nanoparticle exposure led to decreased acetylcholinesterase activity either in the muscle or in the brain, depending on particle composition (muscle—TiO2 10 μg l?1; brain—ZnO 7 and 700 μg l?1), and protein oxidative damage increased in the brain (ZnO 70 μg l?1) and gills (ZnO 70 μg l?1 and mixture) but not in the liver. Exposed fish had more frequent alterations in the liver (necrosis, vascular congestion, leukocyte infiltration, and basophilic foci) and gills (hyperplasia and epithelial damages, e.g., epithelial disorganization and epithelial loss) than the control fish. Thus, predicted concentrations of TiO2 and ZnO nanoparticles caused detectable effects on P. lineatus that may have important consequences to fish health. But, these effects are much more subtle than those usually reported in the scientific literature for high concentrations or doses of metal nanoparticles.  相似文献   

9.
Land use conversion and fertilization have been widely reported to be important managements affecting the exchanges of greenhouse gases between soil and atmosphere. For comprehensive assessment of methane (CH4) and nitrous oxide (N2O) fluxes from hilly red soil induced by land use conversion and fertilization, a 14-month continuous field measurement was conducted on the newly converted citrus orchard plots with fertilization (OF) and without fertilization (ONF) and the conventional paddy plots with fertilization (PF) and without fertilization (PNF). Our results showed that land use conversion from paddy to orchard reduced the CH4 fluxes at the expense of increasing the N2O fluxes. Furthermore, fertilization significantly decreased the CH4 fluxes from paddy soils in the second stage after conversion, but it failed to affect the CH4 fluxes from orchard soils, whereas fertilizer applied to orchard and paddy increased soil N2O emissions by 68 and 113.9 %, respectively. Thus, cumulative CH4 emissions from the OF were 100 % lower, and N2O emissions were 421 % higher than those from the PF. Although cumulative N2O emissions were stimulated in the newly converted orchard, the strong reduction of CH4 led to lower global warming potentials (GWPs) as compared to the paddy. Besides, fertilization in orchard increased GWPs but decreased GWPs of paddy soils. In addition, measurement of soil moisture, temperature, dissolved carbon contents (DOCs), and ammonia (NH4 +-N) and nitrate (NO3 ?-N) contents indicated a significant variation in soil properties and contributed to variations in soil CH4 and N2O fluxes. Results of this study suggest that land use conversion from paddy to orchard would benefit for reconciling greenhouse gas mitigation and citrus orchard cultivation would be a better agricultural system in the hilly red soils in terms of greenhouse gas emission. Moreover, selected fertilizer rate applied to paddy would lead to lower GWPs of CH4 and N2O. Nevertheless, more field measurements from newly converted orchard are highly needed to gain an insight into national and global accounting of CH4 and N2O emissions.  相似文献   

10.
This article reports a dataset on 8 years of monitoring carbon fluxes in a subarctic palsa mire based on micrometeorological eddy covariance measurements. The mire is a complex with wet minerotrophic areas and elevated dry palsa as well as intermediate sub-ecosystems. The measurements document primarily the emission originating from the wet parts of the mire dominated by a rather homogenous cover of Eriophorum angustifolium. The CO2/CH4 flux measurements performed during the years 2001–2008 showed that the areas represented in the measurements were a relatively stable sink of carbon with an average annual rate of uptake amounting to on average ?46 g C m?2 y?1 including an equally stable loss through CH4 emissions (18–22 g CH4–C m?2 y?1). This consistent carbon sink combined with substantial CH4 emissions is most likely what is to be expected as the permafrost under palsa mires degrades in response to climate warming.  相似文献   

11.
Sulfur dioxide (SO2) is considered as a main air pollutant in industrialized areas that can damage vegetation. In the present study, we investigated how exposure to SO2 and foliar application of iron (Fe) would affect certain physiological characteristics of Plantago major. The plant seedlings exposed or unexposed to SO2 (3900 μg m?3) were non-supplemented or supplemented with Fe (3 g L?1) as foliar spray. Plants were exposed to SO2 for 6 weeks in 100 × 70 × 70 cm chambers. Fumigation of plants with SO2 was performed for 3 h daily for 3 days per week (alternate day). Lower leaf Fe concentration in the plants exposed to SO2 at no added Fe treatment was accompanied with incidence of chlorosis symptoms and reduced chlorophyll concentration. No visible chlorotic symptoms were observed on the SO2-exposed plants supplied with Fe that accumulated higher Fe in their leaves. Both at with and without added Fe treatments, catalase (CAT) and peroxidase (POD) activity was higher in the plants fumigated with SO2 in comparison with those non-fumigated with SO2. Foliar application of Fe was also effective in increasing activity of antioxidant enzymes CAT and POD. Exposure to SO2 led to reduced cellulose but enhanced lignin content of plant leaf cell wall. The results obtained showed that foliar application of Fe was effective in reducing the effects of exposure to SO2 on cell wall composition. In contrast to SO2, application of Fe increased cellulose while decreased lignin content of the leaf cell wall. This might be due to reduced oxidative stress induced by SO2 in plants supplied with Fe compared with those unsupplied with Fe.  相似文献   

12.
We investigated air temperature and pressure gradients and their trends for the period 1996–2014 in Greenland and compared these to other periods since 1958. Both latitudinal temperature and pressure gradients were strongest during winter. An overall temperature increase up to 0.15 °C year?1 was observed for 1996–2014. The strongest warming happened during February at the West coast (up to 0.6 °C year?1), weaker but consistent and significant warming occurred during summer months (up to 0.3 °C year?1) both in West and East Greenland. Pressure trends on a monthly basis were mainly negative, but largely statistically non-significant. Compared with other time windows in the past six decades, the period 1996–2014 yielded an above-average warming trend. Northeast Greenland and the area around Zackenberg follow the general pattern but are on the lower boundary of observed significant trends in Greenland. We conclude that temperature-driven ecosystem changes as observed in Zackenberg may well be exceeded in other areas of Greenland.  相似文献   

13.
A microscale zero-valent iron (mZVI)-based in situ reactive zone is a promising technology for contaminated groundwater remediation. Estimation of mZVI aging behavior after its injection into the subsurface is essential for efficiency and longevity assessments. In this study, batch tests were conducted to investigate the effect of initial pH on mZVI aging dynamics, as well as the formation and evolution of aging products over 112 days. Results indicated that mZVI aging accelerated with decreasing initial pH. Corrosion rates of mZVI particles under pH 6.0 and 7.5 were approximately two orders of magnitude higher than those observed at pH 9.0. The morphological, structural, and compositional evolution of mZVI particles in three systems (pH = 6.0, 7.5, and 9.0) were investigated using scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. In acidic and neutral solutions, a thick passivation layer with loosely and unevenly distributed aging precipitates was observed, and Fe3O4 was the final aging precipitate. Nevertheless, in alkaline solutions, minute aging precipitates were detected on the mZVI surface at 112 day. Characterization results suggested that mZVI was oxidized via the Fe0–Fe(OH)2–Fe3O4 route. These findings shed new light on mZVI aging mechanisms, particularly its physicochemical characteristics and the structural evolution of mZVI in field-scale groundwater remediation applications.  相似文献   

14.
In coastal Antarctica, freezing and thawing influence many physical, chemical and biological processes for ice-free tundra ecosystems, including the production of greenhouse gases (GHGs). In this study, penguin guanos and ornithogenic soil cores were collected from four penguin colonies and one seal colony in coastal Antarctica, and experimentally subjected to three freezing–thawing cycles (FTCs) under ambient air and under N2. We investigated the effects of FTCs on the emissions of three GHGs including nitrous oxide (N2O), carbon dioxide (CO2) and methane (CH4). The GHG emission rates were extremely low in frozen penguin guanos or ornithogenic soils. However, there was a fast increase in the emission rates of three GHGs following thawing. During FTCs, cumulative N2O emissions from ornithogenic soils were greatly higher than those from penguin guanos under ambient air or under N2. The highest N2O cumulative emission of 138.24 μg N2O–N kg?1 was observed from seal colony soils. Cumulative CO2 and CH4 emissions from penguin guanos were one to three orders of magnitude higher than those from ornithogenic soils. The highest cumulative CO2 (433.0 mgCO2–C kg?1) and CH4 (2.9 mgCH4–C kg?1) emissions occurred in emperor penguin guanos. Penguin guano was a stronger emitter for CH4 and CO2 while ornithogenic soil was a stronger emitter for N2O during FTCs. CO2 and CH4 fluxes had a correlation with total organic carbon (TOC) and soil/guano moisture (Mc) in penguin guanos and ornithogenic soils. The specific CO2–C production rate (CO2–C/TOC) indicated that the bioavailability of TOC was markedly larger in penguin guanos than in ornithogenic soils during FTCs. This study showed that FTC-released organic C and N from sea animal excreta may play a significant role in FTC-related GHG emissions, which may account for a large proportion of annual fluxes from tundra ecosystems in coastal Antarctica.  相似文献   

15.
Potassium-fly ash (K-FA) sorbents were investigated for high-temperature CO2 sorption. K-FAs were synthesised using coal fly ash as source of silica and aluminium. The synthesised materials were also mixed with Li2CO3 and Ca(OH)2 to evaluate their effect on CO2 capture. Temperature strongly affected the performance of the K-FA sorbents, resulting in a CO2 uptake of 1.45 mmol CO2/g sorbent for K-FA 1:1 at 700 °C. The CO2 sorption was enhanced by the presence of Li2CO3 (10 wt%), with the K-FA 1:1 capturing 2.38 mmol CO2/g sorbent at 700 °C in 5 min. This sorption was found to be similar to previously developed Li-Na-FA (2.54 mmol/g) and Li-FA (2.4 mmol/g) sorbents. The presence of 10 % Li2CO3 also accelerated sorption and desorption. The results suggest that the increased uptake of CO2 and faster reaction rates in presence of K-FA can be ascribed to the formation of K-Li eutectic phase, which favours the diffusion of potassium and CO2 in the material matrix. The cyclic experiments showed that the K-FA materials maintained stable CO2 uptake and reaction rates over 10 cycles.  相似文献   

16.
The Arctic land area has warmed by >1 °C in the last 30 years and there is evidence that this has led to increased productivity and stature of tundra vegetation and reduced albedo, effecting a positive (amplifying) feedback to climate warming. We applied an individual-based dynamic vegetation model over the Arctic forced by observed climate and atmospheric CO2 for 1980–2006. Averaged over the study area, the model simulated increases in primary production and leaf area index, and an increasing representation of shrubs and trees in vegetation. The main underlying mechanism was a warming-driven increase in growing season length, enhancing the production of shrubs and trees to the detriment of shaded ground-level vegetation. The simulated vegetation changes were estimated to correspond to a 1.75 % decline in snow-season albedo. Implications for modelling future climate impacts on Arctic ecosystems and for the incorporation of biogeophysical feedback mechanisms in Arctic system models are discussed.  相似文献   

17.
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   

18.
19.
The surface energy balance (SEB) is essential for understanding the coupled cryosphere–atmosphere system in the Arctic. In this study, we investigate the spatiotemporal variability in SEB across tundra, snow and ice. During the snow-free period, the main energy sink for ice sites is surface melt. For tundra, energy is used for sensible and latent heat flux and soil heat flux leading to permafrost thaw. Longer snow-free period increases melting of the Greenland Ice Sheet and glaciers and may promote tundra permafrost thaw. During winter, clouds have a warming effect across surface types whereas during summer clouds have a cooling effect over tundra and a warming effect over ice, reflecting the spatial variation in albedo. The complex interactions between factors affecting SEB across surface types remain a challenge for understanding current and future conditions. Extended monitoring activities coupled with modelling efforts are essential for assessing the impact of warming in the Arctic.  相似文献   

20.
The catalysts such as Fe, Bi2O3, and Fe-doped Bi2O3 were synthesized for the sonophotocatalytic treatment of synthetic dye and real textile wastewater. The resultant catalysts were characterized for its size and uniform shape using x-ray diffractogram (XRD) and scanning electron microscopy (SEM) which signified the nanorod shape formed Bi2O3. The higher ultraviolet light absorbance capacity of the catalysts was also evident using diffuse reflectance spectroscopy (DRS). Initially, the effect of conventional parameters such as initial pH, gas bubbling (argon, oxygen, air and nitrogen) and oxidant addition (H2O2 and peroxymonosulfate) in the presence of sonolysis (22 and 37 kHz frequency) and photolysis (UV-C light) on 10 ppm Basic Brown 1 dye was studied. The results showed that highest decolorization of 62 % was attained for 3 g/L peroxymonosulfate under 37 kHz frequency sonolysis treatment. Secondly, with the catalyst study, highest of 46 % dye color removal was obtained with 4 g/L Fe under 37 kHz frequency sonolysis treatment. The sonophotocatalytic treatment of dye with Fe-doped Bi2O3 catalyst in combination with peroxymonosulfate showed highest color removal of 99 %. Finally, the sonophotocatalytic treatment of real textile wastewater in the presence of 3 g/L Fe-doped Bi2O3 and 6 g/L peroxymonosulfate reduced the total organic carbon (TOC) and chemical oxygen demand (COD) level to 77 and 91 %, respectively, in 180 min. The reported treatment process was found to treat the synthetic dye and real textile wastewater effectively.  相似文献   

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