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1.
We studied the hydrolysis of gas-phase carbon tetrachloride (CCl4), chloroform (CHCl3), and dichloromethane (CH2Cl2) over a metallic Fe surface for its application in combination with air stripping and soil vapour extraction. The effects of chlorocarbon concentration, type and preparation of the iron-containing material, humidity, and temperature on process performance are reported. The hydrolysis of chlorinated methane derivatives is catalysed by metallic iron resulting in a noticeable decrease of the reaction temperature. The reaction kinetics were found to be consistent with the Langmuir-Hinshelwood model.  相似文献   

2.
Bio-diffusion mixing rates (Db) were estimated from depth profiles of excess 210Pb and 137Cs in three sediment cores collected from Mumbai Harbour Bay (MHB) using a steady state vertical advection - diffusion model. The mean of 210Pb and 137Cs derived Db values along the studied area were obtained to be about 23 and 36 cm2y?1 respectively. These derived values were within the range of literature values reported for other equivalent environment internationally. The relatively higher Db values for 137Cs profiles demonstrated that particles have diffused more intensely within the surface layer of sediments over 1 year. Conversely, low Db values for 210Pb indicate slow mixing rates in the sediment profile which might be resulted from low 210Pb flux and diffusion of 222Rn to the seafloor. The significant differences between 210Pb and 137Cs derived Db values among cores indicate that there appeared to be as regional differences in sediment properties and local variability in the intensity of seafloor mixing. Furthermore, Db values also depend on differences in characteristic time and depth scales of radionuclides in cores, benthic fauna abundances, organic carbon flux to the sediments and primary production in overlying surface waters. Comparison of 210Pb derived Db values with those calculated from 137Cs distributions reveals better agreement for core 2 than core 1 and 3. The agreement may be fortuitous because 137Cs appears significantly deeper than 210Pb in all cores. It was also observed that Db values increases as sediment accumulation rate increases for both radionuclide.  相似文献   

3.
Photocatalytic oxidation using semiconductors is one of the advanced oxidation processes for degradation of organic pollutants in water and air. TiO2 is an excellent photocatalyst that can mineralize a large range of organic pollutants such as pesticides and dyes. The main challenge is to improve the efficiency of the TiO2 photocatalyst and to extend TiO2 light absorption spectra to the visible region. A potential solution is to couple TiO2 with a narrow band gap semiconductor possessing a higher conduction band such as bismuth oxide. Therefore, here we prepared Bi2O3/TiO2 heterojunctions by the impregnation method with different Bi/Ti ratio. The prepared composites have been characterized by UV–Vis diffused reflectance spectra and X-ray diffraction. The photocatalytic activity of the heterojunction has been determined from the degradation of orange II under visible and UV light. Results show that Bi2O3/TiO2 heterojunctions are more effective than pure TiO2-anatase under UV-A irradiation, with an optimum for the Bi/Ti ratio of 5 %, for the photocatalytic degradation of Orange II. However, the photocatalytic activity under irradiation at λ higher than 420 nm is not much improved. Under UV–visible radiation, the two semiconductors are activated. We propose a mechanism explaining why our products are more effective under UV–visible irradiation. In this case the charge separation is enhanced because a part of photogenerated electrons from the conduction band of TiO2 will go to the conduction band of bismuth oxide. In this composite, titanium dioxide is the main photocatalyst, while bismuth oxide acts as adsorbent photosensitizer under visible light.  相似文献   

4.
The NO/H2/O2 reaction was studied under oxidizing conditions in the 100-400 °C range over 0.1 wt% Pt supported on various metal oxides such as MgO, CeO2, SiO2, La2O3, CaO, Y2O3 and TiO2. The Pt/MgO and Pt/CeO2 catalysts showed good catalytic behaviours. Here, we find that the Pt/Mg-Ce-O catalyst, prepared from MgO and CeO2 by the sol-gel method, is a very active and selective catalyst towards N2 formation in the whole 100–400 °C range. This catalyst appears to be the most active, selective and stable one ever reported in the literature for the NO/H2/O2 reaction, even in the presence of 5%v H2O or 20 ppmv of SO2 in the feed stream.Selected article from the Regional Symposium on Chemistry and Environment, Krusevac, Serbia, June 2003, organised by Dr. Branimir Jovancicevic.  相似文献   

5.
Oxidation of aldehydes to carboxylic acids is a major reaction. Conventionally, this reaction is carried out with oxidants and metal catalysts, thus producing unwanted metal waste. Recently, aqueous media have been used as an alternative for toxic organic solvents. Here, we tested the clathrate-structured, neutral hydrogen peroxide adduct 4Na2SO4·2H2O2·NaCl for the oxidation of aldehydes to acids in aqueous solution. We found that various aromatic, heteroaromatic and aliphatic aldehydes were selectively oxidized to corresponding acids in 70–98% yields. This simple acid–base treatment allows to separate easily the acid product in high purity without any organic solvent. Moreover, the adduct is produced using 25% H2O2, with inexpensive sodium sulphate, Na2SO4, and sodium chloride, NaCl. The adduct is a non-toxic white crystalline solid, readily soluble in water, and easy to handle.  相似文献   

6.
Summary. Sequestration and processing of pyrrolizidine alkaloids (PAs) by leaf beetles of the genus Platyphora were investigated. Tracer experiments with labeled alkaloids were performed with P. eucosma feeding on Koanophyllon panamense (Asteraceae, tribe Eupatorieae). P. eucosma catalyzes the same reactions previously demonstrated for P. boucardi specialized to Prestonia portobellensis (Apocynaceae): (i) epimerization of rinderine to intermedine; (ii) esterification of retronecine yielding insect-specific PAs; (iii) efficient transport of the PAs as free bases into the defensive secretions. P. bella feeding on Tournefortia cuspidata (Boraginaceae) shows the same sequestration behavior and ability to synthesize the specific retronecine esters. P. ligata, a species phylogenetically closely related to the PA adapted species and clustering in the same clade, but feeding on a host plant devoid of PAs, feeds easily on PA treated host-plant leaves, but does not sequester or metabolize PAs. P. kollari a species clustering outside the PA clade refused to feed on its food-plant leaves painted with PAs. The results are discussed in relation to host-plant selection of the PA adapted species and the role of PAs in chemical defense. Received 20 September 2002; accepted 18 November 2002.  相似文献   

7.
N2O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N2O formation over Pt/BaO/Al2O3 catalyst. Three types of catalysts, Pt/BaO/Al2O3, Pt/Pd mechanical mixing catalyst (Pt/BaO/Al2O3 + Pd/Al2O3) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al2O3) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H2/CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H2-TPR techniques. In addition, temperature programmed reactions of NO with H2/CO were conducted to obtain further information about N2O formation mechanism. Compared with Pt/BaO/Al2O3, (Pt/BaO/ Al2O3 + Pd/Al2O3) produced less N2O and more NH3 during NO x storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al2O3 + Al2O3). Temperature programmed reactions of NO with H2/CO results showed that Pd/Al2O3 component in (Pt/BaO/Al2O3 + Pd/Al2O3) played an important role in NO reduction to NH3, and the formed NH3 could reduce NO x to N2 leading to a decrease in N2O formation. Most of N2O formed over (Pt-Pd/BaO/Al2O3 + Al2O3) was originated from Pd/BaO/Al2O3 component. H2-TPR results indicated Pd-Ba interaction resulted in more difficultto- reduce PdOx species over Pd/BaO/Al2O3, which inhibits the NO dissociation and thus drives the selectivity to N2O in NO reduction.
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8.
Highly symmetrical molecules such as CH4, CF4 or SF6 are known to be atmospheric pollutants and greenhouse gases. High-resolution spectroscopy in the infrared is particularly suitable for the monitoring of gas concentration and radiative transfers in the earth's atmosphere. This technique requires extensive theoretical studies for the modeling of the spectra of such molecules (positions, intensities and shapes of absorption lines). Here, we have developed powerful tools for the analysis and the simulation of absorption spectra of highly symmetrical molecules. These tools have been implemented in the spherical top data system (STDS) and highly-spherical top data system (HTDS) software available at http://www.u-bourgogne.fr/LPUB/shTDS.html. They include a compilation of modeled data obtained during the last 20 years. An overview of our latest results in this domain will be presented. Electronic Publication  相似文献   

9.
The great fecundity and very high larval mortality of most marine invertebrates and fish make possible substantial variance in the number of offspring contributed by adults to subsequent generations. The reproductive success of such organisms may thus resemble a sweepstakes lottery, in which a minority of progenitors succeeds in replacing an entire population, while the majority fails to procreate. One specific prediction of this hypothesis, that genetic diversity of newly settled cohorts should be less than that of the adult population, is tested in the present study. Microsatellite DNA markers were examined in naturally spawned juvenile European flat oysters Ostrea edulis (L.), collected over a 12-day period in 1993 from the western Mediterranean Sea, near Sète, France (43°32′N, 3°56′E) and grown out for a period of up to 10 months. Variation in these juveniles was compared to that in a pooled sample of adults collected in 1994 from two locations (Thau Lagoon and Port St. Louis) that had statistically homogeneous allelic frequencies. Though nearly twice as large as the pooled adult sample, the juvenile sample had only 60% of the adult allelic diversity. Analyses of linkage disequilibrium and kinship, as well as estimation of the effective number of parents, suggested that 10–20 adults produced this juvenile cohort. This observation supports the hypothesis of sweepstakes reproductive success and suggests that partial inbreeding may occur even in species with large populations and dispersing planktonic larvae. Electronic Supplementary Material Supplementary material is available to authorised users in the online version of this article at .  相似文献   

10.
Chromium oxide and manganese oxide promoted ZrO2-CeO2 catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NO x with NH3. A series of characterization including X-ray diffraction (XRD), high-resolution transmission electron microscope (HR-TEM), Brunauer–Emmett–Teller (BET) surface area analysis, H2 temperatureprogrammed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS) were used to evaluate the influence of the physicochemical properties on NH3-SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO2-CeO2 binary oxide for the low temperature NH3-SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO2 and H2O. Cr-Zr-Ce mixed oxide exhibited>80% NO x conversion at a wide temperature window of 100°C–300°C. In situ DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence of Cr6 +. The present mixed oxide can be a candidate for the low temperature abatement of NO x .
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11.
Microgrowth patterns and the oxygen isotope composition of juvenile, shallow-marine bivalve mollusk shells of Phacosoma japonicum (Reeve) in Japan were analyzed and cross-calibrated with environmental parameters. Mark-and-recovery experiments indicate that a pair of two microgrowth lines and two microgrowth increments is produced every lunar day. This finding makes it possible to assign exact calendar dates to each portion of the shell. Average daily growth rates decrease by 61% from age two to three and 55% from age three to four. The length of the growing season and the growth rate are mainly controlled by temperature: shell growth ceases below 14.2°C (age two) and 16.8°C (age four) and is most rapid between 24.6°C and 27.2°C. Based on local temperature cycles, the growing season is longest in Seto Inland Sea, central Honshu (from May to November) and shortest at Hakodate Bay, North Japan (from June to October). The annual oxygen isotope profiles of the shells reflect the temperature cycle and the varying amounts of freshwater added to the seawater by precipitation. The most negative '18O values of -3.15‰ occur during the rainy season, i.e. during the monsoon and typhoon seasons. Growth rates are only slightly affected by salinity changes. Strongly reduced growth rates during the second half of the year at Seto Inland Sea and to a lesser extent at Tokyo Bay are explained by nutrient deprivation. Our study provides the basis for the use of P. japonicum in high-resolution ecological studies and environmental reconstructions.  相似文献   

12.
The cDNA sequence coding for tauropine dehydrogenase (TaDH) [belonging to the family of opine dehydrogenases] has been determined. Using the demosponge Suberites domuncula, we describe for the first time the tauropine dehydrogenase gene (of length 2,992 kb) from a eukaryote, consisting of two introns flanked by three exons. Moreover, two allelic variants have been identified, which are present in the different specimens either in a homozygotic or in a heterozygotic way; the data suggest an intermediary type of heritance. Phylogenetic analyses indicate that S. domuncula TaDH is only distantly related to the opine dehydrogenases from marine invertebrates; rather it comprises high sequence similarity to bacterial ornithine cyclodeaminases (OCD). In addition, expression studies revealed that the steady-state level of TaDH dropped drastically in animals, which had been exposed to elevated aeration. Antibodies raised against the recombinant sponge TaDH were used to demonstrate that S. domuncula expresses high levels of this enzyme in almost all cells. If tissue samples were kept under additional aeration no immuno-signals could be identified. A strong accumulation of the enzyme was seen around the bacteria, existing in bacteriocytes, indicating that under aerobic conditions the bacteria might produce taurine. These data suggest involvement of the sponge TaDH in the final step of the glycolytic pathway, more specifically, in regeneration of NAD(+) under anaerobic conditions. Furthermore, potential mutual influences between bacteria and sponge are discussed, claiming a horizontal gene transfer of the gene from a bacterium to the sponge. The following sequences from Suberites domuncula have been deposited (EMBL/GenBank): the cDNA encoding the tauropine [(carboxyethyl)-taurine/derived from sulfhydryl-amino acids] dehydrogenase (SD_TaDH) under AM712888; the corresponding gene under AM712889; and the fragments of the sponge-associated bacteria comprising the opine dehydrogenase domain: SUBDO_BAC1 (AM712890), SUBDO_BAC2 (AM712891), SUBDO_BAC3 (AM712892), SUBDO_BAC5 (AM712894), SUBDO_BAC6 (AM712895), SUBDO_BAC7 (AM712896), SUBDO_BAC8 (AM712897) and SUBDO_BAC9 (AM712898).  相似文献   

13.
In this work, Er3+:YAlO3/TiO2 composite was synthesized by a ultrasonic dispersion and liquid boil method. The Er3+:YAlO3/TiO2 composite and pure TiO2 powder were characterized by XRD. The degradation of different organic dyes was used to evaluate the photocatalytic activity of the Er3+:YAlO3/TiO2 composite. It is found that the photocatalytic activity of Er3+:YAlO3/TiO2 composite is much higher than that for the similar system with only TiO2. Moreover, this Er3+:YAlO3/TiO2 composite provides a new way to take advantage of TiO2 in sewage treatment aspects using solar light.  相似文献   

14.
This study devised a staging system for, and monitored, the gonad development of the limpet species Patella vulgata and Patella ulyssiponensis on the South West coast of Ireland using histological techniques. Maturation began in the males of both species in January and in the females it began in March. There was no statistical difference in gonad development between sexes and between species. Spawning in the male P. vulgata occurred from September to December 2003 and in September and October 2004. In female P. vulgata spawning occurred from October to December 2003, no spawning of females was observed in 2004. In male P. ulyssiponensis spawning occurred in November and December 2003 and from September 2004 to December 2004. Spawning was observed from November 2003 to January 2004 and in September 2004 in female P. ulyssiponensis. Sex ratios also varied between the species and between months sampled. Nevertheless more males were observed in both species.  相似文献   

15.
We have discovered that HNO3 and related species are released from the TiO2 surface into air in the TiO2 photocatalytic oxidation of NO2 (1 ppm) under continuous UV light illumination (1 mW cm−2) by dehumidifying the outlet gas of the reaction and analyzing the recovered condensate liquid by ion chromatography. The origin of the HNO3 recovered in the dehumidifier could not be explained by a simple desorption of HNO3 overproduced on the TiO2 surface. The produced HNO3 must be activated on the TiO2 surface and causing the unidentified reaction.  相似文献   

16.
The photodegradation of Acid blue 74 in aqueous solution employing a H2O2/ultraviolet system in a photochemical reactor was investigated. The kinetics of decolorization were studied by application of a kinetic model. The results show that the reaction of decolorization followed pseudo-first order kinetics. We demonstrate that there is an optimum H2O2 concentration, at which the rate of the decolorization reaction is maximum. Irradiation at 253.7 nm of the dye solution in the presence of H2O2 results in complete discoloration after ten minutes of treatment.  相似文献   

17.
Short-term (3 h) changes in concentration of chlorophylls and their derivatives in stage V Pseudodiaptomus euryhalinus and their fecal material were followed by HPLC during a 24 h experiment. Copepodites were fed with the prasinophyte Tetraselmis suecica. Intact chlorophyll a and b were found in animals and fecal material and had similar dynamics of accumulation over time. The extent of transformation of chlorophyll a and b to colorless compounds was different with chlorophyll a being more extensively degraded. Additionally, several chlorophyll derivatives (pheophytin and pyropheophytin-like pigments) were found. Pyropheophytin a was the most abundant followed by pheophytin b, pheophytin a, and pheophorbide a. Relative amounts of pheopigments were different in copepodites and fecal material, and pheophytin a, pheophorbide a, and pheophytin b concentrations were low and variable. The amount of ingested chlorophyll recovered as chlorophyll a and its derivatives in fecal and copepodite pools was generally low (<5%), with one exception occurring after 9 h, when it accounted for >70%. These data suggest individual pheopigments are produced at different rates and that chemical or enzymatic mechanisms in the gut of copepodites act on the two chlorophylls in different ways.  相似文献   

18.
Adult rock hyrax (Procavia capensis) and bush hyrax (Heterohyrax brucei) allocate much of their surface activity to being vigilant for vertebrate predators. Individuals of the two species associate for thermoregulatory basking on rock outcrops (koppies) and, in the Matobo National Park, Zimbabwe, frequently constitute heterospecific groups that produce offspring synchronously. Exposure to predators during basking is thought to put a high premium on vigilance, particularly during the presence of dependent offspring in nurseries. We predicted, therefore, an increase in the association of the two species of hyraxes when offspring were present because this would lead to larger groups, thus enhancing the ability to detect predators. Koppie aggregations of hyraxes were classified as homospecific or heterospecific according to basking group composition. Heterospecific association increased when offspring were present, and heterospecific groups were larger than homospecific ones. Fifty-one percent of nurseries were heterospecific for adults/subadults. During the pre-weaning phase (<2 months after birth), 85% of P. capensis and 65% of H. brucei juveniles were in nurseries of heterospecific basking groups. Heterospecific groups had more offspring than homospecific groups. Juvenile mortality is most evident after young are weaned and heterospecific associations break down. Heterospecific aggregation, through increased group size, may result in a higher probability of avoiding predators, thereby reducing the vulnerability of young.  相似文献   

19.
Although the flow dynamics of pure liquid drops in other liquids has been well researched, little attention has been paid to the impacts of impurities. Hence, most of research is not directly applicable to the real world. To address this gap, we conducted numerical experiments simulating the rise of pure and contaminated drops. It was selected to study liquid CO2 drops contaminated with SO2 under high pressure because such mixtures mimic potential scenarios in which drops may leak from carbon capture and storage (CCS) facilities or pipelines. First, numerical simulation experiments were performed to validate our method by comparing our results with previous research on pure drops. Second, the validated numerical approach was applied to simulations of contaminated drops to investigate how contaminants affect rising drops. The results show that the SO2 contamination caused changes in deformation, breakup phenomena, rising velocities, surrounding flow fields and drag coefficients. Most importantly, the contamination resulted in the formation of smaller “child drops”; such breakup is not observed in pure CO2 drops. The formation of child drops in turn affects the streamlines, patterns and areas of wakes behind the contaminated drops. The addition of contaminants also enhances the dissolution rate, which is affected by the contaminant concentration and by the flow dynamics of the rising drop. Our results would improve understanding the rise of impure CO2 drops, such as drops potentially leaked by future CCS operations.  相似文献   

20.
The transformation of the fungicide carbendazim (methyl-2 benzimidazole carbamate) induced by hydroxyl radical generated by the UV photolysis of H2O2 has been studied in dilute aqueous solution. The efficient reaction of hydroxyl radicals with carbendazim led to the rapid degradation of carbendazim. The study of reaction kinetics yielded a second order rate constant of 2.2±0.3 109 M−1 s−1 for HO· radicals with carbendazim. This value is in agreement with a high reactivity of HO· radicals with carbendazim. Most degradation products were identified by high performance liquid chromatography mass spectrometry (HPLC-MS). In the presence of hydrogenocarbonate and carbonate ions, hydroxyl radicals were quenched and in turn carbonate radicals CO3 ·− were formed. Carbonate radicals are indeed known to react efficiently with compounds containing electron-rich sites such as nitrogen or sulfur atoms. The use of a kinetic modelling software gave evidence for the occurrence of such reactions with carbendazim. The second order rate constant of carbonate radical with carbendazim was equal to 6±2 106 M−1 s−1. Electronic Publication  相似文献   

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