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1.
The photodegradation of two common and very stable azo-dyes, i.e. methyl-orange (C 14H 14N 3SO 3Na) and orange II (C 16H 11N 2SO 4Na), is reported. The photocatalytic oxidation was carried out in aqueous suspensions of polycrystalline TiO 2 irradiated by sunlight. Compound parabolic collectors, installed at the “Plataforma Solar de Almería” (PSA, Spain) were used as the photoreactors and two identical reacting systems allowed to perform photoreactivity runs for the two dyes at the same time and under the same irradiation conditions. The disappearance of colour and substrates together with the abatement of total organic carbon content was monitored. The main sulfonate-containing intermediates were found to be in lower number in respect to those obtained under artificial irradiation. In particular there were no more evidence of the presence of hydroxylated transients. The dependence of dye photooxidation rate on: (i) substrate concentration; (ii) catalyst amount; and (iii) initial pH was investigated. The influence of the presence of strong oxidant species (H 2O 2, S 2O 82−) and some ions (Cl −, SO 42−) on the process was also studied. 相似文献
2.
UV/TiO 2/H 2O 2, UV/TiO 2 and UV/H 2O 2 were compared as pre-treatment processes for the detoxification of mixtures of 4-chlorophenol (4CP), 2,4-dichlorophenol (DCP), 2,4,6-trichlorophenol (TCP) and pentachlorophenol (PCP) prior to their biological treatment. When each chlorophenol was initially supplied at 50 mg l −1, UV/TiO 2/H 2O 2 treatment supported the highest pollutant removal, COD removal, and dechlorination efficiencies followed by UV/TiO 2 and UV/H 2O 2. The remaining toxicity to Lipedium sativum was similar after all pre-treatments. Chlorophenol photodegradation was always well described by a first order model kinetic ( r2 > 0.94) and the shortest 4CP, DCP, TCP and PCP half-lives of 8.7, 7.1, 4.5 and 3.3 h, respectively, were achieved during UV/TiO 2/H 2O 2 treatment. No pollutant removal was observed in the controls conducted with H 2O 2 or TiO 2 only. Inoculation of all the photochemically pre-treated mixtures with activated sludge microflora was followed by complete removal of the remaining pollutants. Combined UV/TiO 2/H 2O 2-biological supported the highest detoxification, dechlorination (99%) and COD removal (88%) efficiencies. Similar results were achieved when each chlorophenol was supplied at 100 mg l −1. COD and Cl mass balances indicated UV, UV/H 2O 2, and UV/TiO 2 treatments lead to the formation of recalcitrant photoproducts, some of which were chlorinated. 相似文献
3.
The combined electrochemical oxidation-solar-light/immobilized TiO 2 film process was conducted to degrade an azo dye, Reactive Black 5 (RB5). The toxicity was also monitored by the Vibrio fischeri light inhibition test. The electrochemical oxidation rapidly decolorized RB5 (55, 110 μM) with a supporting electrolyte of 2 g l −1 NaCl at current density 277 A m −2 and pH 4. However, TOC mineralization and A 310 removal were low. Additionally, the treated solution showed high biotoxicity. RB5 at 110 μM significantly retarded the de-colorization efficiency by using the solar-light/immobilized TiO 2 film process. The combined electrochemical oxidation-solar-light/immobilized TiO 2 process effectively increased the removal of color, A 310, and TOC. The toxicity was also significantly reduced after 3 h of solar irradiation. The results indicated that the low-cost combined process is a potential technique for rapid treatment of RB5. 相似文献
4.
Aqueous 4-nitrophenol solutions containing TiO 2 or Al 2O 3 nanoparticles were irradiated with electron beam. 4-nitrophenol was decomposed by the ionizing radiation process in the absence of the nanoparticles. The addition of TiO 2 or Al 2O 3 (2 g l −1) before irradiation improved the removal of 4-nitrophenol, total organic carbon (TOC) but also nitrogen (TN). To identify the origin of the loss (catalysis or simply adsorption), TiO 2 or Al 2O 3 nanoparticles were added after irradiation. Experiments show that the effect of the presence of TiO 2 or Al 2O 3 during irradiation is just due to adsorption. 相似文献
5.
An experiment was carried out to decompose chlorinated dioxins (PCDDs, PCDFs) Chlorobenzenes, NOx and odourous compounds (H 2S, CH 4S, C 2H 6S 2, C 8H 8, C 2H 6S, C 2H 4O, NH 3) simultaneously using a catalyst in the MSW incineration plant. The experiments were conducted at temperatures from 200°C to 400°C and from 3000h −1 to 6000h −1 at space velocity. A catalyst containing V 2O 5 and WO 3 on the basis of TiO 2 is used, an oxidizing catalyst of the honeycomb type. The average decomposition efficiencis were 95%, 98%, 92% for PCDDs(48CDDs), PCDFs(48CDFs) and Chlorobenzenes(36CLBs) at a reaction temperature of 350°C and a space velocity of 3000h −1, more than 90% for NOx at a reactiont temperature of 300°C and more than 80% for odourous compounds at the reaction temperature of 300°C and a space velocity of 6000h −1. All those compounds were decomposed successfully with increasing contact time and surface. The rate-determing step was the chemical reaction of catalyst surface. 相似文献
6.
Arsenic oxidation (As(III) to As(V)) and As(V) removal from water were assessed by using TiO 2 immobilized in PET (polyethylene terephthalate) bottles in the presence of natural sunlight and iron salts. The effect of many parameters was sequentially studied: TiO 2 concentration of the coating solution, Fe(II) concentration, pH, solar irradiation time; dissolved organic carbon concentration. The final conditions (TiO 2 concentration of the coating solution: 10%; Fe(II): 7.0 mg l −1; solar exposure time: 120 min) were applied to natural water samples spiked with 500 μg l −1 As(III) in order to verify the influence of natural water matrix. After treatment, As(III) and total As concentrations were lower than the limit of quantitation (2 μg l −1) of the voltammetric method used, showing a removal over 99%, and giving evidence that As(III) was effectively oxidized to As(V). The results obtained demonstrated that TiO 2 can be easily immobilized on a PET surface in order to perform As(III) oxidation in water and that this TiO 2 immobilization, combined with coprecipitation of arsenic on Fe(III) hydroxides(oxides) could be an efficient way for inorganic arsenic removal from groundwaters. 相似文献
7.
In this paper, we present two years of seasonal nitric oxide (NO), ammonia (NH 3), and nitrous oxide (N 2O) trace gas fluxes measured in a recovering riparian zone with cattle excluded and adjacent riparian zone grazed by cattle. In the recovering riparian zone, average NO, NH 3, and N 2O fluxes were 5.8, 2.0, and 76.7 ng N m −2 s −1 (1.83, 0.63, and 24.19 kg N ha −1 y −1), respectively. Fluxes in the grazed riparian zone were larger, especially for NO and NH 3, measuring 9.1, 4.3, and 77.6 ng N m −2 s −1 (2.87, 1.35, and 24.50 kg N ha −1 y −1) for NO, NH 3, and N 2O, respectively. On average, N 2O accounted for greater than 85% of total trace gas flux in both the recovering and grazed riparian zones, though N 2O fluxes were highly variable temporally. In the recovering riparian zone, variability in seasonal average fluxes was explained by variability in soil nitrogen (N) concentrations. Nitric oxide flux was positively correlated with soil ammonium (NH 4+) concentration, while N 2O flux was positively correlated with soil nitrate (NO 3−) concentration. Ammonia flux was positively correlated with the ratio of NH 4+ to NO 3−. In the grazed riparian zone, average NH 3 and N 2O fluxes were not correlated with soil temperature, N concentrations, or moisture. This was likely due to high variability in soil microsite conditions related to cattle effects such as compaction and N input. Nitric oxide flux in the grazed riparian zone was positively correlated with soil temperature and NO 3− concentration. Restoration appeared to significantly affect NO flux, which increased ≈600% during the first year following restoration and decreased during the second year to levels encountered at the onset of restoration. By comparing the ratio of total trace gas flux to soil N concentration, we show that the restored riparian zone is likely more efficient than the grazed riparian zone at diverting upper-soil N from the receiving stream to the atmosphere. This is likely due to the recovery of microbiological communities following changes in soil physical characteristics. 相似文献
8.
The present work focuses on the fate of two cancerostatic platinum compounds (CPC), cisplatin and carboplatin, as well as of two inorganic platinum compounds, [PtCl 4] 2− and [PtCl 6] 2− in biological wastewater treatment. Laboratory experiments modelling adsorption of these compounds onto activated sludge showed promising specific adsorption coefficients KD and KOC and Freundlich adsorption isotherms. However, the adsorption properties of the investigated substances were differing significantly. Adsorption decreased following the order cisplatin > [PtCl 6] 2− > [PtCl 4] 2− > carboplatin. Log KD-values were ranging from 2.5 to 4.3 , log KOC from 3.0 to 4.7. A pilot membrane bioreactor system (MBR) was installed in a hospital in Vienna and fed with wastewater from the oncologic in-patient treatment ward to investigate CPC-adsorption in a sewage treatment plant. During three monitoring periods Pt-concentrations were measured in the influent (3–250 μg l−1 Pt) and the effluent (2–150 μg l−1 Pt) of the treatment plant using ICP-MS. The monitoring periods (duration 30 d) revealed elimination efficiencies between 51% and 63% based on averaged weekly input–output budgets. The derived log KD-values and log KOC-values ranged from 2.4 to 4.8 and from 2.8 to 5.3, respectively. Species analysis using HPLC-ICP-MS proofed that mainly carboplatin was present as intact drug in the influent and – due to low log KD – in the effluent of the MBR. 相似文献
9.
The photocatalytic removal of humic acid (HA) using TiO 2 under UVA irradiation was examined by monitoring changes in the UV 254 absorbance, dissolved organic carbon (DOC) concentration, apparent molecular weight distribution, and trihalomethane formation potentials (THMFPs) over treatment time. A resin fractionation technique in which the samples were fractionated into four components: very hydrophobic acids (VHA), slightly hydrophobic acids, hydrophilic charged (CHA) and hydrophilic neutral (NEU) was also employed to elucidate the changes in the chemical nature of the HA components during treatment. The UVA/TiO 2 process was found to be effective in removing more than 80% DOC and 90% UV 254 absorbance. The THMFPs of samples were decreased to below 20 μg l −1 after treatments, which demonstrate the potential to meet increasingly stringent regulatory level of trihalomethanes in water. Resin fractionation analysis showed that the VHA fraction was decreased considerably as a result of photocatalytic treatments, forming CHA intermediates which were further degraded with increased irradiation time. The NEU fraction, which comprised of non-UV-absorbing low molecular weight compounds, was found to be the most persistent component. 相似文献
10.
The photocatalytic inactivation (PCI) of Escherichia coli (Gram-negative) and Bacillus subtilis (Gram-positive) was performed using polyoxometalate (POM) as a homogeneous photocatalyst and compared with that of heterogeneous TiO 2 photocatalyst. Aqueous suspensions of the microorganisms (10 7–10 8 cfu ml −1) and POM (or TiO 2) were irradiated with black light lamps. The POM-PCI was faster than (or comparable to) TiO 2-PCI under the experimental conditions employed in this study. The relative efficiency of POM-PCI was species-dependent. Among three POMs (H 3PW 12O 40, H 3PMo 12O 40, and H 4SiW 12O 40) tested in this study, the inactivation of E. coli was fastest with H 4SiW 12O 40 while that of B. subtilis was the most efficient with H 3PW 12O 40. Although the biocidal action of TiO 2 photocatalyst has been commonly ascribed to the role of photogenerated reactive oxygen species such as hydroxyl radicals and superoxides, the cell death mechanism with POM seems to be different from TiO 2-PCI. While TiO 2 caused the cell membrane disruption, POM did not induce the cell lysis. When methanol was added to the POM solution, not only the PCI of E. coli was enhanced (contrary to the case of TiO 2-PCI) but also the dark inactivation was observed. This was ascribed to the in situ production of formaldehyde from the oxidation of methanol. The interesting biocidal property of POM photocatalyst might be utilized as a potential disinfectant technology. 相似文献
11.
Methane fluxes were measured from three exposed tundra sites and four snowpack sites on the Fildes Peninsula in the maritime Antarctic in the summertime of 2002. The average fluxes at two normal tundra sites were −15.3 μg m −2 h −1 and −14.3 μg m −2 h −1, respectively. The fluxes from tundra site with fresh penguin dropping addition showed positive values with the average of 36.1 μg m −2 h −1, suggesting that the deposition of fresh droppings greatly enhanced CH 4 emissions from the poor Antarctic tundra during penguin breeding periods. The summertime variation in CH 4 flux was correlated with surface ground temperature and the precipitation. The correlation between the flux and PT 0, which is the product of the precipitation and surface ground temperature, was quite strong. The diurnal cycle of CH 4 flux from the tundra soils was not obtained due to local fluky weather conditions. The fluxes through four snowpack sites were also obtained by the vertical CH 4 concentration gradient and their average fluxes were −46.5 μg m −2 h −1, −28.2 μg m −2 h −1, −46.4 μg m −2 h −1 and −17.9 μg m −2 h −1, respectively, indicating that tundra soils under snowpack also consume atmospheric CH 4 in the maritime Antarctic; therefore these fluxes could constitute an important part of the annual CH 4 budget for Antarctic tundra ecosystem. 相似文献
12.
The photocatalytic degradation of dimethyl phthalate (DMP) in aqueous TiO 2 suspension under UV illumination has been investigated using oxygen (O 2) and ferrate (Fe(VI)) as electron acceptors. The experiments demonstrated that Fe(VI) was a more effective electron acceptor than O 2 for scavenging the conduction band electrons from the surface of the catalyst. Some major intermediate products from DMP degradation were identified by HPLC and GC/MS analyses. The analytical results identified dimethyl 3-hydroxyphthalate and dimethyl 2-hydroxyphthalate as the two main intermediate products from the DMP degradation in the TiO 2–UV–O 2 system, while in contrast phthalic acid was found to be the main intermediate product in the TiO 2–UV–Fe(VI) system. These findings indicate that DMP degradation in the TiO 2–UV–O 2 and TiO 2–UV–Fe(VI) systems followed different reaction pathways. An electron spin resonance analysis confirmed that hydroxyl radicals existed in the TiO 2–UV–O 2 reaction system and an unknown radical species (most likely an iron–oxo species) is suspected to exist in the TiO 2–UV–Fe(VI) reaction system. Two pathway schemes of DMP degradation in the TiO 2–UV–O 2 and TiO 2–UV–Fe(VI) reaction systems are proposed. It is believed that the radicals formed in the TiO 2–UV–O 2 reaction system preferably attack the aromatic ring of the DMP, while in contrast the radicals formed in the TiO 2–UV–Fe(VI) reaction systems attack the alkyl chain of DMP. 相似文献
13.
Micellar electrokinetic chromatography (MEKC) using sodium dodecyl sulfate was tested for its ability to analyze mixtures containing three dioxin derivatives. Dioxin-containing samples, subjected to photocatalytic oxidation using TiO 2 and/or SnO 2 as the semiconductor catalyst were analyzed by MEKC to obtain the rate constant for each dioxin when it was degraded individually or in the presence of the other two dioxins. A significant degree of analyze competition was observed and the mixed catalyst offered important synergism. 相似文献
14.
This study examines the oxidation of reduced sulfur compounds (RSCs) in urban ambient air. The photochemical conversions of RSC (such as DMS, CS 2, H 2S, DMDS, and CH 3SH) to a further oxidized form (e.g., SO 2, MSA, and H 2SO 4) were assessed using a photochemical box model. For our model simulation of RSC oxidation, measurements were taken at an urban monitoring station in Seoul, Korea (37.6° N, 127° E) during three separate time periods (e.g., Sept. 17–18, Oct. 23, and Oct. 27–28, 2003). The results indicate that DMS and H 2S were the dominant RSCs with concentrations of 370 ± 140 and 110 ± 60 pptv, respectively. The photochemical conversion of DMDS to SO 2 was found to occur more efficiently than other RSCs. The overall results of our study suggest that photochemical conversion of RSCs accounted for less than 15% of the observed SO 2 during the measurement period. The SO 2 production from DMS oxidation (mainly by the reaction with OH) was found to be affected primarily by the abstraction channel due to high NO x levels during the experimental conditions. 相似文献
15.
TiO 2 powder-containing paper composites, called TiO 2 paper, were prepared by a papermaking technique, and their photocatalytic efficiency was investigated. The TiO 2 paper has a porous structure originating from the layered pulp fiber network, with TiO 2 powders scattered on the fiber matrix. Under UV irradiation, the TiO 2 paper decomposed gaseous acetaldehyde more effectively than powdery TiO 2 and a pulp/TiO 2 mixture not in paper form. Scanning electron microscopy and mercury intrusion analysis revealed that the TiO 2 paper had characteristic unique voids ca. 10 μm in diameter, which might have contributed to the improved photocatalytic performance. TiO 2 paper composites having different void structures were prepared by using beaten pulp fibers with different degrees of freeness and/or ceramic fibers. The photodecomposition efficiency was affected by the void structure of the photocatalyst paper, and the initial degradation rate of acetaldehyde increased with an increase in the total pore volume of TiO 2 paper. The paper voids presumably provided suitable conditions for TiO 2 catalysis, resulting in higher photocatalytic performance by TiO 2 paper than by TiO 2 powder and a pulp/TiO 2 mixture not in paper form. 相似文献
16.
Cold season (winter and thaw) CH 4, CO 2 and N 2O fluxes from freshwater marshes (47°35′N, 133°31′E, Northeast China) were measured, using the static chamber method. The mean CH 4 and CO 2 fluxes from Carex lasiocarpa (Cl) were 0.5 ± 0.19 and 6.23 ± 1.36 mg C m −2 h −1, respectively, and those from Deyeuxia angustifoli (Da) were 0.18 ± 0.15 and 5.22 ± 2.48 mg C m −2 h −1, respectively in winter. There was no significant difference between Cl and Da ( p > 0.05). The contributions of winter CH 4 fluxes were about 5.5% and 3% in the Cl and Da, respectively. Marshes are an important potential N 2O sink in winter season in northeast China. During thaw, the CH 4 and CO 2 emissions rapidly increased, 4.5–6 times of winter emissions. Wetland became a source of N 2O. Cold season gases flux from northern wetlands play an important role in the seasonal gas exchange. 相似文献
17.
Adsorption at the air–water interface and soil sorption from aqueous solution have been investigated for a group of ethylene oxide (EO)–propylene oxide (PO) block copolymeric surfactants. The group which have a common structural formula of EO m PO n EO m is distinguished by the fact that they have large critical micelle concentration (CMC) values and therefore do not readily form micelles at common environmental concentrations and temperatures. Adsorption at the air–water interface is readily shown to be driven by the size of the hydrophobic PO block. The size of the reduction in surface tension produced by a common concentration of 10 −5 mol dm −3 linearly increases with the size of the PO block as does the efficiency of adsorption at the air–water interface as measured by pC 20 – the negative logarithm of the surfactant concentration that produces a reduction in surface tension of 20 mN m −1. Soil sorption data have also been captured for these compounds and the data are readily fitted to the Freundlich adsorption isotherm. However soil sorption is shown to be inversely related to the molecular mass of the molecules and appears to be related to the size of the hydrophilic EO blocks in the molecule. 相似文献
18.
An increasing percentage of agricultural land in Germany is used for oil seed plants. Hence, rape has become an important agricultural plant (in Saxony 1998: 12% of the farmland) in the recent years. During flowering of rape along with intensive radiation and high temperatures, a higher production and emission of biogenic VOC was observed. The emissions of terpenes were determined and more importantly, high concentrations of organic carbonyl compounds were observed during this field experiment. All measurements of interest have been carried out during two selected days with optimal weather conditions. It is found that the origin or the mechanism of formation of different group of compounds had strong influence on the day to day variation of their concentrations. The emission flux of terpenes from flowering rape plants was determined to be 16–32 μg h −1 m −2 (30–60 ng h −1 per g dry plant––540–1080 ng h −1 per plant), in total. Limonene, -thujene and sabinene were the most important compounds (about 60% of total terpenes). For limonene and sabinene reference emission rates ( MS) and temperature coefficients were determined: β limonene=0.108 K −1 and MS=14.57 μg h −1 m −2; β sabinene=0.095 K −1 and MS=5.39 μg h −1 m −2. The detected carbonyl compound concentrations were unexpectedly high (maximum formaldehyde concentration was 18.1 ppbv and 3.4 ppbv for butyraldehyde) for an open field. Possible reasons for these concentrations are the combination of primary emission from the plants induced by high temperature and high ozone stress, the secondary formation from biogenically and advected anthropogenically emitted VOC at high radiation intensities and furthered by the low wind speeds at this time. 相似文献
19.
Reductive dechlorination rate constants for five chlorobenzenes in the presence of Pd/Fe as catalyst were determined experimentally. Linear free energy relationships (LFER) for the dechlorination rate constants of five chlorobenzenes and three chlorophenols were developed by partial least squares (PLS) regression based on quantum chemical parameters computed by PM3 Hamiltonian. The optimal LFER model obtained is logk=−1.63+1.46×10−3ΔHf−7.69×10−1ELUMO where k stands for the dechlorination rate constants, Δ Hf is the standard heat of formation, and ELUMO is the energy of the lowest unoccupied molecular orbital. The Q2cum value of the model is 0.879, indicating good robustness and predictive power of the model. 相似文献
20.
We investigated the effects of various factors on the aerobic degradation of nonylphenol (NP) in sewage sludge. NP (5 mg/kg) degradation rate constants ( k1) calculated were 0.148 and 0.224 day −1 for the batch experiment and the bioreactor experiment, respectively, and half-lives ( t1/2) were 4.7 and 3.1 days, respectively. The optimal pH value for NP degradation in sludge was 7.0 and the degradation rate was enhanced when the temperature was increased and when yeast extract (5 mg/l) and surfactants such as brij 30 or brij 35 (55 or 91 μM) were added. The addition of aluminum sulfate (200 mg/l) and hydrogen peroxide (1 mg/l) inhibited NP degradation within 28 days of incubation. Of the microorganism strains isolated from the sludge samples, we found that strain CT7 (identified as Bacillus sphaericus) manifested the best degrading ability. 相似文献
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