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1.
A mathematical model describing the dissolution of nuclear glass directly disposed in clay combines a first-order dissolution rate law with the diffusion of dissolved silica in clay. According to this model, the main parameters describing the long-term dissolution of the glass are etaR, the product of the diffusion accessible porosity eta and the retardation factor R, and the apparent diffusion coefficient D(app) of dissolved silica in clay. For determining the migration parameters needed for long-term predictions, four Through-Diffusion (T-D) experiments and one percolation test have been performed on undisturbed clay cores. In the Through-Diffusion experiments, the concentration decrease after injection of 32Si (radioactive labelled silica) was measured in the inlet compartment. At the end of the T-D experiments, the clay cores were cut in thin slices and the activity of labelled silica in each slice was determined. The measured activity profiles for these four clay cores are well reproducible. Since no labelled silica could be detected in the outlet compartments, the Through-Diffusion experiments are fitted by two In-Diffusion models: one model assuming linear and reversible sorption equilibrium and a second model taking into account sorption kinetics. Although the kinetic model provides better fits, due to the sufficiently long duration of the experiments, both models give approximately similar values for the fit parameters. The single percolation test leads to an apparent diffusion coefficient value about two to three times lower than those of the Through-Diffusion tests. Therefore, dissolved silica appears to be strongly retarded in Boom Clay. A retardation factor R between 100 and 300 was determined. The corresponding in situ distribution coefficient K(d) is in the range 25-75 cm(3) g(-1). The apparent diffusion coefficient of dissolved silica in Boom Clay is estimated between 2 x 10(-13) and 7 x 10(-13) m(2) s(-1). The pore diffusion coefficient is in the range from 6 x 10(-11) to 1 x 10(-10) m(2) s(-1). 相似文献
2.
For the performance assessment study of a geological disposal of High Level Waste (HLW) in clayey formations, migration studies are essential. For low permeability soils (clays), classical diffusion studies take a very long time. In order to reduce the experimental time, we propose an electrical field as driving force to accelerate the migration of ionic species. This paper reports the assessment of the electromigration technique as a powerful new and fast technique for migration studies. The apparent molecular diffusion coefficient can be derived by two independent methods using the migration parameters obtained from an electromigration experiment, namely the apparent dispersion coefficient and the apparent convection velocity. First, it can be calculated from the velocity of the migrating species by the Einstein relation. But, corrections are necessary for electroosmotic flow. The apparent electroosmotic mobility is experimentally determined as 2.2·10−9 m2/Vs. Second, it can be calculated from the relation between the apparent dispersion coefficient and the total apparent convection velocity. But it is necessary to know the dispersion length of the medium. The dispersion length for Boom Clay is experimentally determined as 8·10−5 m. Because of the serious reduction in time, it becomes possible to run series of experiments at different electrical fields to obtain averaged values for the apparent molecular diffusion coefficient according to the two methods. Experiments at different electrical fields have another advantage: the intercept of the linear relationship between the total apparent convection velocity and the apparent dispersion coefficient gives the apparent molecular diffusion coefficient. The apparent molecular diffusion coefficients obtained for 85Sr, 131I and HTO are respectively 0.8·10−11, 15·10−11, and 24·10−11 m2/s. These values are confirmed by pure diffusion experiments. The excellent agreement with the apparent molecular diffusion coefficients obtained by classical diffusion tests clearly demonstrates the feasibility of the electromigration technique for the determination of diffusion coefficients. 相似文献
3.
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
4.
The quantum yield of the phototransformation of 4-nitrophenol has been evaluated as 4.5×10−5±0.6×10−5 at pH=2; at 3.0×10−5±0.6×10−5 at pH=5.5; 1.8×10−5±0.5×10−5 at pH=8.3. However the half-life is relatively low and no accumulation of aromatic or quinonic products was observed. Hydroquinone (QH2) is the main organic primary product formed when an air-saturated or degassed solution was irradiated in 365 nm monochromatic light (about 80% of the 4-nitrophenol initially converted at pH=5.5 in the absence of oxygen). In air-saturated neutral or acidic solution, the formation of NO−3 ions accounted for about 80% of the 4-nitrophenol converted, but in degassed medium a mixture NO : NO−2 : NO−3 is formed. An heterolytical mechanism of photohydrolysis with primary formation of QH2 and HNO2 is suggested. Several by-products as benzoquinone, 4-nitrosophenol, 4-nitrocatechol and nitrohydroquinone are formed according to the conditions. Many secondary reactions are involved as the disproportionation or the oxidation of HNO2, the oxidation of QH2 by HNO2 and oxidations induced by excitation of NO−2 and NO−3. 相似文献
5.
Dennis J. Paustenbach Tibor T. Sarlos Brent L. Finley David A. Jeffrey Michael J. Ungs 《Chemosphere》1991,23(11-12)
Conservative models were used to estimate the airborne concentrations of 2,3,7,8 tetrachlorodibenzo-p-dioxin (TCDD) vapor and particulates originating from soil containing 100 ppb TCDD. The upper-bound estimates were 3.25 pg/m3 of airborne TCDD vapor on-site and 0.51 pg/m3 for TCDD vapor 100 meters downwind. The TCDD air concentration on-site due to suspended particulate is estimated to be 1.4 pg/m3, based on a TSP level of 0.07 mg/m3. Assuming 70 years of continuous exposure to these concentrations, the upper-bound cancer risks determined from the Jury model were estimated to be 9.4 × 10−6 to 1.1 × 10−4 and 1.5 × 10−6 to 1.7 × 10−5 for inhalation of on- and off-site vapor, respectively, and 4.1 × 10−6 to 4.6 × 10−5 for dust inhalation. Since few sites have average soil concentrations as high as 100 ppb TCDD, this worst-case analysis indicates that inhalation will rarely, if ever, be a significant route of exposure to TCDD-contaminated soil. Experimental results support this claim and point to much lower risk estimates (8.4 × 10−9 to 9.9 × 10−8), suggesting that the parameters used in the Jury model are likely to overestimate the actual airborne levels of TCDD at contaminated sites. 相似文献
6.
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
7.
To determine the mobility of colloids (0.001–0.45 μm) and suspended particles (> 0.45 μm) in granite fractures, laboratory particle-migration and conservative tracer studies have been carried out in a natural fracture within a large granite block, with overall dimensions of 83×90×60 cm. Flow fields within this horizontal fracture were controlled through a set of 9 boreholes drilled orthogonally to the fracture. Laboratory experiments were performed using a range of average water velocities which contained values low enough to closely approximate the natural flow velocities of < 2 m yr−1 in plutonic rocks of the Canadian Shield. The particles used had diameters between 0.02 and 22 μm, and included latex spheres, glass spheres and colloidal silica. Migration experiments were carried out with a filtered groundwater, ionic strength of 0.01 mol kg−1, obtained from a granite fracture within the Whiteshell Research Area of Manitoba. Flushing experiments showed that suspended particles as large as 40 μm could be mobilized from the fracture surface. The mobility of suspended particles was significantly less than that of colloids. However, within the size range of colloids used in these studies (0.022–0.090 μm), colloid size did not affect colloid migration. Although, in general, colloids eluted ahead of the conservative tracer, colloid mobility was significantly reduced when the average groundwater velocity dropped below between 32 and 240 m yr−1. Colloid transport was found to be very sensitive to flow path and flow direction. 相似文献
8.
Ai-Jun Miao Kathy A. Schwehr Chen Xu Sai-Jin Zhang Zhiping Luo Antonietta Quigg Peter H. Santschi 《Environmental pollution (Barking, Essex : 1987)》2009,157(11):3034-3041
In this study, we report that silver ions (Ag+) from the oxidative dissolution of silver engineered nanoparticles (Ag-ENs) determined the EN toxicity to the marine diatom Thalassiosira weissflogii. Most of the Ag-ENs formed non-toxic aggregates (>0.22 μm) in seawater. When the free Ag+ concentration ([Ag+]F) was greatly reduced by diafiltration or thiol complexation, no toxicity was observed, even though the Ag-ENs were better dispersed in the presence of thiols with up to 1.08 × 10−5 M Ag-ENs found in the <0.22 μm fraction, which are orders of magnitude higher than predicted for the natural aquatic environment. The secretion of polysaccharide-rich algal exopolymeric substances (EPS) significantly increased at increasing [Ag+]F. Both dissolved and particulate polysaccharide concentrations were higher for nutrient-limited cells, coinciding with their higher Ag+ tolerance, suggesting that EPS may be involved in Ag+ detoxification. 相似文献
9.
M. Srensen M. D. Hurley T. J. Wallington T. S. Dibble O. J. Nielsen 《Atmospheric environment (Oxford, England : 1994)》2002,36(39-40)
Smog chamber/FTIR techniques were used to study the relative reactivity of OH radicals with methanol, ethanol, phenol, C2H4, C2H2, and p-xylene in 750 Torr of air diluent at 296±2 K. Experiments were performed with, and without, 500–8000 μg m−3 (4000–50 000 μm2 cm−3 surface area per volume) of NaCl, (NH4)2SO4 or NH4NO3 aerosol. In contrast to the recent findings of Oh and Andino (Atmospheric Environment 34 (2000) 2901, 36 (2002) 149; International Journal of Chemical Kinetics 33 (2001) 422) there was no discernable effect of aerosol on the rate of loss of the organic compounds via reaction with OH radicals. Gas kinetic theory arguments cast doubt upon the findings of Oh and Andino. The available data suggest that the answer to the title question is “No”. As part of this work the rate constants for reactions of OH radicals with methanol, ethanol, and phenol in 750 Torr of air at 296 K were determined to be: kOH+CH3OH=(8.12±0.54)×10−13, kOH+C2H5OH=(3.47±0.32)×10−12 and kOH+phenol=(3.27±0.31)×10−11 cm3 molecule−1 s−1. 相似文献
10.
Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/DFs) were detected in waterfowl such as common cormorants, tufted ducks, and their prey, namely fish and bivalves from Lake Shinji, Japan. The concentration of total PCDDs/DFs-TEQ was found to be higher in the muscle tissues of common cormorants than in those of tufted ducks. The results of hierarchical cluster analysis implied that the residue distribution pattern of PCDD/DF homologues was considerably different between these two species. Furthermore, biomagnification factors (BMFs) were estimated from bivalves as prey to tufted duck muscles as target organs. Despite the highest concentrations of 1,3,6,8- and 1,3,7,9-TeCDD in tufted ducks and their prey, however, the BMFs of these isomers were calculated to be lower than those of the toxic 2,3,7,8-substituted PCDDs/DFs. On the other hand, log BMF of toxic 2,3,7,8-substituted PCDDs/DFs were significantly higher for lower chlorinated isomers than those of the higher chlorinated isomers. The biota-sediment accumulation factors (BSAFs) of PCDDs/DFs were also estimated using shijimi clam and fish samples against sediment from Lake Shinji. The average BSAFs were estimated and ranged from 4.0×10−3 to 2.2×10−1 and 2.0×10−4 to 2.0×10−1 for bivalve and fish samples, respectively. Based on calculated BMFs and BSAFs, the total PCDD/DF-TEQ levels in the tufted duck were estimated to have been lowest (2.0 pg TEQ/g dry weight basis) in 1947 and highest (9.8 pg TEQ/g) in 1971. 相似文献
11.
Permeable reactive barriers (PRBs) are an alternative technology to treat mine drainage containing sulfate and heavy metals. Two column experiments were conducted to assess the suitability of an organic carbon (OC) based reactive mixture and an Fe0-bearing organic carbon (FeOC) based reactive mixture, under controlled groundwater flow conditions. The organic carbon mixture contains about 30% (volume) organic carbon (composted leaf mulch) and 70% (volume) sand and gravel. The Fe0-bearing organic carbon mixture contains 10% (volume) zero-valent iron, 20% (volume) organic carbon, 10% (volume) limestone, and 60% (volume) sand and gravel. Simulated groundwater containing 380 ppm sulfate, 5 ppm As, and 0.5 ppm Sb was passed through the columns at flow rates of 64 (the OC column) and 62 (the FeOC column) ml d− 1, which are equivalent to 0.79 (the OC column) and 0.78 (the FeOC column) pore volumes (PVs) per week or 0.046 m d− 1 for both columns. The OC column showed an initial sulfate reduction rate of 0.4 µmol g (OC)− 1 d− 1 and exhausted its capacity to promote sulfate reduction after 30 PVs, or 9 months of flow. The FeOC column sustained a relatively constant sulfate reduction rate of 0.9 µmol g (OC)− 1 d− 1 for at least 65 PVs (17 months). In the FeOC column, the δ34S values increase with the decreasing sulfate concentration. The δ34S fractionation follows a Rayleigh fractionation model with an enrichment factor of 21.6‰. The performance decline of the OC column was caused by the depletion of substrate or electron donor. The cathodic production of H2 by anaerobic corrosion of Fe probably sustained a higher level of SRB activity in the FeOC column. These results suggest that zero-valent iron can be used to provide an electron donor in sulfate reducing PRBs. A sharp increase in the δ13C value of the dissolved inorganic carbon and a decrease in the concentration of HCO3− indicate that hydrogenotrophic methanogenesis is occurring in the first 15 cm of the FeOC column. 相似文献
12.
To investigate whether wind is a significant driving force in the diffusion of CO and CH4 from the atmosphere into soil, we measured the concentrations of these two gases at two heights above a temperate grass field in Japan and estimated their deposition velocities using micrometeorological techniques. The concentrations were inversely correlated with wind speed, indicating that the local concentrations were influenced by ground sources. The CO and CH4 concentrations at 0.33 m were usually lower than those at 1.3 m. Although nocturnal data are suspected to be non-stationary, by selecting several periods when the changes of the concentrations were small but larger than analytical precision, we obtained a CO velocity of 2.9 and 3.9×10−2 cms−1, agreeing with a CO deposition velocity, 3.4×10−2 cms−1, obtained by applying a method using CO2 as a tracer. The CH4 influx obtained by the method using CO2 as a tracer was 13 ngm−2 s−1. The ranges of the CO deposition velocity and CH4 influx were similar to those obtained in previous studies in grassfields and in a nearby arable field using a closed-chamber technique. This shows that light winds do not greatly accelerate CO and CH4 uptake by soil. 相似文献
13.
E. Gerasopoulos P. Zanis A. Stohl C. S. Zerefos C. Papastefanou W. Ringer L. Tobler S. Hübener H. W. Gggeler H. J. Kanter L. Tositti S. Sandrini 《Atmospheric environment (Oxford, England : 1994)》2001,35(36):294
The 7Be activity concentrations measured from 1996 to 1998 at four high-altitude stations, Jungfraujoch—Switzerland, Zugspitze—Germany, Sonnblick—Austria and Mt. Cimone—Italy, were analyzed in combination with a set of, meteorological and atmospheric parameters such as the tropopause height, relative and specific humidity and also in conjunction with 3D back-trajectories in order to investigate the climatological features of 7Be. A frequency distribution analysis on 7Be activity concentrations revealed the existence of two concentration classes around 1.5 and 6 mBq m−3 and a transition class between the two modes of the distribution at 3–4 mBq m−3. Cross-correlation analysis performed between 7Be and a number of meteorological and atmospheric parameters at the first three stations showed a strong negative correlation with relative humidity (−0.56, −0.51, −0.41) indicating the importance of wet scavenging as a controlling mechanism. Also, the positive correlation with the height of 3-days back-trajectories and tropopause height (+0.49/+0.43, +0.59/+0.36, +0.44/+0.38) shows that downward transport from the upper or middle to lower troposphere within anticyclonic conditions plays also an important role. Trajectory statistics showed that low 7Be concentrations typically originate from lower-altitude subtropical ocean areas, while high concentrations arrive from the north and high altitudes, as is characteristic for stratospheric intrusions. Although the 7Be activity concentrations are highly episodic, the monthly means indicate an annual cycle with a late-summer maximum at all stations. The correlation coefficients calculated for monthly means of the 7Be and atmospheric data suggest that the main predictor controlling the seasonality of the 7Be concentrations is tropopause height (+0.76, +0.56, +0.60), reflecting more vertical transport from upper tropospheric levels into the lower troposphere during the warm season than during the cold season. 相似文献
14.
Flux density values, computed from observed infiltration and outflow measurements at 184 locations in a 0.3-m-thick, 9m × 23m layer of compacted clay subsoil, are compared to effective flux density values that are based on breakthrough time distributions for water and Br− tracer over the same area. Results suggest that both water and tracer move at similar rates, but considerably faster than expected, on the basis of flux density alone, and that only a small fraction of the total pore space is involved in active transport. The ramifications of these findings are explored against the background of effective porosity, degree of compaction, and observed changes in bulk density with time. 相似文献
15.
H. -W. Jacobi R. Weller A. E. Jones P. S. Anderson O. Schrems 《Atmospheric environment (Oxford, England : 1994)》2000,34(29-30)
Because investigations of PAN at higher southern latitudes are very scarce, we measured surface PAN concentrations for the first time in Antarctica. During the Photochemical Experiment at Neumayer (PEAN'99) campaign mean surface PAN mixing ratios of 13±7 pptv and maximum values of 48 pptv were found. When these PAN mixing ratios were compared to the sum of NOx and inorganic nitrate they were found to be equal or higher. Low ambient air temperatures and low PAN concentrations caused a slow homogeneous PAN decomposition rate of approximately 5×10−2 pptv h−1. These slow decay rates were not sufficient to firmly establish the simultaneously observed NOx concentrations. In addition, low concentration ratios of [HNO3]/[NOx] imply that the photochemical production of NOx within the snow pack can influence surface NOx mixing ratios in Antarctica. Alternate measurements of PAN mixing ratios at two different heights above the snow surface were performed to derive fluxes between the lower troposphere and the underlying snow pack using calculated friction velocities. Most of the concentration differences were below the precision of the measurements. Therefore, only an upper limit for the PAN flux of ±1×1013 molecules m−2 s−1 without a predominant direction can be estimated. However, PAN fluxes below this limit can still influence both the transfer of nitrogen compounds between atmosphere and ice, and the PAN budget in higher southern latitudes. 相似文献
16.
E. Martínez J. Albaladejo A. Notario E. Jimnez 《Atmospheric environment (Oxford, England : 1994)》2000,34(29-30)
The atmospheric reaction of the methylthiyl radical (CH3S) with O3 was investigated as a function of temperature (259–381 K), in the pressure range of 25–300 Torr, using the technique of laser photolysis/laser-induced fluorescence. The resulting Arrhenius expression, with an uncertainty of ±2σ, was k1(T=259–381 K)=(1.02±0.30)×10−12 exp[(432±77) K/T] cm3 molecule−1 s−1. The obtained rate constant k1 was independent of pressure over the limited range employed. Our results are compared with the previous studies carried out, at single temperature and as a function of temperature, by different techniques. 相似文献
17.
C. Wagner G. Schuster J.N. Crowley 《Atmospheric environment (Oxford, England : 1994)》2009,43(32):5001-5008
The interaction of N2O5 with dispersed samples of Arizona Test Dust (ATD), Calcite (CaCO3) and quartz (SiO2) was investigated at varying relative humidity using an aerosol flow reactor. Reactive uptake coefficients, γ, obtained at close to zero relative humidity were (4.8 ± 0.7) × 10−3 for CaCO3, (8.6 ± 0.6) × 10−3 for Quartz and (9.8 ± 1.0) × 10−3 for ATD. In the case of calcite, evidence was obtained for an enhanced rate of uptake at relative humidities above ≈ 50%. The results are compared to literature values obtained using bulk substrates and to previous aerosol uptake data on Saharan dust. 相似文献
18.
The main objective of the present study was to investigate possible links between biomarkers and swimming performance in the estuarine fish Pomatoschistus microps acutely exposed to metals (copper and mercury). In independent bioassays, P. microps juveniles were individually exposed for 96 h to sub-lethal concentrations of copper or mercury. At the end of the assays, swimming performance of fish was measured using a device specially developed for epibenthic fish (SPEDE). Furthermore, the following biomarkers were measured: lipid peroxidation (LPO) and the activity of the enzymes acetylcholinesterase (AChE), lactate dehydrogenase (LDH), glutathione S-transferases (GST), 7-ethoxyresorufin-O-deethylase (EROD), superoxide dismutase (SOD), catalase (CAT), glutathione reductase (GR) and glutathione peroxidase (GPx). LC50s of copper and mercury (dissolved throughout metal concentrations) at 96 h were 568 μg L−1 and 62 μg L−1, respectively. Significant and concentration-dependent effects of both metals on swimming resistance and covered distance against water flow were found at concentrations equal or higher than 50 μg L−1 for copper and 3 μg L−1 for mercury (dissolved throughout metal concentrations). These results indicate that SPEDE was efficacious to quantify behavioural alterations in the epibenthic fish P. microps at ecologically relevant concentrations. Significant alterations by both metals on biomarkers were found including: inhibition of AChE and EROD activities, induction of LDH, GST and anti-oxidant enzymes, and increased LPO levels, with LOEC values ranging from 25 to 200 μg L−1 for copper and from 3 to 25 μg L−1 for mercury (dissolved throughout metal concentrations). Furthermore, significant and positive correlations were found between some biomarkers (AChE and EROD) and behavioural parameters, while negative correlations were found for others (LPO, anti-oxidant enzymes and LDH) suggesting that disruption of cholinergic function through AChE inhibition, decreased detoxification capability due to EROD inhibition, additional energetic demands to face chemical stress, and oxidative stress and damage may contribute to decrease the swimming performance of fish. Since a reduced swimming capability of fish may reduce their ability to capture preys, avoid predators, and interfere with social and reproductive behaviour, the exposure of P. microps to copper and/or mercury concentrations similar to those tested here may decrease the fitness of wild populations of this species. 相似文献
19.
Alejandro Moncayo-Lasso Janeth Sanabria Csar Pulgarin Norberto Benítez 《Chemosphere》2009,77(2):296-300
Bacteria inactivation and natural organic matter oxidation in river water was simultaneously conducted via photo-Fenton reaction at “natural” pH (6.5) containing 0.6 mg L−1 of Fe3+ and 10 mg L−1 of H2O2. The experiments were carried out by using a solar compound parabolic collector on river water previously filtered by a slow sand filtration system and voluntarily spiked with Escherichia coli. Fifty five percent of 5.3 mg L−1 of dissolved organic carbon was mineralized whereas total disinfection was observed without re-growth after 24 h in the dark. 相似文献
20.
Andreas C. Scheinost Regina Kirsch Dipanjan Banerjee Alejandro Fernandez-Martinez Harald Zaenker Harald Funke Laurent Charlet 《Journal of contaminant hydrology》2008,102(3-4):228
The long-lived radionuclide 79Se is one of the elements of concern for the safe storage of high-level nuclear waste, since clay minerals in engineered barriers and natural aquifer sediments strongly adsorb cationic species, but to lesser extent anions like selenate (SeVIO42−) and selenite (SeIVO32−). Previous investigations have demonstrated, however, that SeIV and SeVI are reduced by surface-associated FeII, thereby forming insoluble Se0 and Fe selenides. Here we show that the mixed FeII/III (hydr)oxides green rust and magnetite, and the FeII sulfide mackinawite reduce selenite rapidly (< 1 day) to FeSe, while the slightly slower reduction by the FeII carbonate siderite produces elemental Se. In the case of mackinawite, both S−II and FeII surface atoms are oxidized at a ratio of one to four by producing a defective mackinawite surface. Comparison of these spectroscopic results with thermodynamic equilibrium modeling provides evidence that the nature of reduction end product in these FeII systems is controlled by the concentration of HSe−; Se0 forms only at lower HSe− concentrations related to slower HSeO3− reduction kinetics. Even under thermodynamically unstable conditions, the initially formed Se solid phases may remain stable for longer periods since their low solubility prevents the dissolution required for a phase transformation into more stable solids. The reduction by Fe2+-montmorillonite is generally much slower and restricted to a pH range, where selenite is adsorbed (pH < 7), stressing the importance of a heterogeneous, surface-enhanced electron transfer reaction. Although the solids precipitated by the redox reaction are nanocrystalline, their solubility remains below 6.3 × 10− 8 M. No evidence for aqueous metal selenide colloids nor for Se sorption to colloidal phases was found. Since FeII phases like the ones investigated here should be ubiquitous in the near field of nuclear waste disposals as well as in the surrounding aquifers, mobility of the fission product 79Se may be much lower than previously assumed. 相似文献