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1.
Hu X  Zhao X  Hwang HM 《Chemosphere》2007,66(9):1618-1626
Laccase from Trametes versicolor was immobilized on nanoparticles and kaolinite by physical adsorption or chemical covalence in which the supporters were activated by cross-linked with glutaraldehyde. Thermal and pH stabilities of immobilized laccase on these different supporters were compared. The degradation efficiencies of these immobilized laccases on oxidation of benzo[a]pyrene (BaP) were also compared. The results showed that the immobilized laccases on nanoparticles were more stable in resisting pH and thermal changes. After 48h oxidation, laccase immobilized on kaolinite using the covalent coupling method showed a higher efficiency of oxidation with the BaP residue of 23% in the presence of 1mM HBT and with BaP residue of 37% in 1mM ABTS as the mediator. The results also exhibited a significant inhibition by 1% surfactant Tween 80. According to the HPLC analysis, the oxidation products including 1,6-benzo[a]pyrene quinone, 3,6-benzo[a]pyrene quinone and 6,12-benzo[a]pyrene quinone were identified.  相似文献   

2.
In order to study the enzymatic mechanisms involved in the successive steps of BaP degradation by a Deuteromycete fungus Fusarium solani, we developed an indirect approach by using inhibitors of enzymes. We used either specific inhibitors of peroxidases (i.e. salicylhydroxamic acid) and of cytochrome P-450 (i.e. piperonyl butoxyde) or inhibitors of both enzymes (i.e. potassium cyanide). Surprisingly, no expected decrease of BaP degradation was observed with most inhibitors tested. On the contrary, more BaP was degraded. Only butylated hydroxytoluene, which acts as a free radical scavenger, inhibited BaP degradation. The inhibition of these enzymes, which use H(2)O(2) as a cosubstrate, might have resulted in an increase of hydrogen peroxide availability in the fungal cultures. This enhancement could induce formation of reactive oxygen species (ROS) which might be the agents that initiate benzo[a]pyrene oxidation. This study proposed a hypothetic alternative metabolic pathway involved in PAH metabolism by Fusarium solani.  相似文献   

3.
Previous work in this laboratory has confirmed that the bacteria Mycobacterium sp. strain RJGII.135 and Sphingomonas yanoikuyae strain B1 and the green alga Selanastrum capricornutum strain UTEX 1648 degrade benzo[a]pyrene (BaP) to various BaP intermediates. S. capricornutum was first grown with BaP for 4 days. The organic extract of this media was then introduced into separate cultures of strain RJGII.135 and strain B1; separate cultures were grown with BaP for comparison. Cultures grown with BaP and those grown with the algal/BaP extract showed similar mineralization patterns. The quantity of total metabolites formed was greater in bacterial cultures grown with the algal/BaP extract than those grown with BaP alone. For strain RJGII.135, only 27% of the original BaP remained in cultures grown with the algal/BaP extract; 59% remained in cultures grown with BaP. For strain B1, only 6% of the original BaP remained in cultures grown with the algal/BaP extract; 38% remained in cultures grown with BaP. These results indicate that strategies utilizing organisms together may be necessary in being able to degrade large, recalcitrant polycyclic aromatic hydrocarbons (PAHs) such as BaP.  相似文献   

4.
The capacity of Phanerochaete chrysosporium grown on soil with added sugarcane baggase (BP) and pine sawdust (PS) to remove benzo(a)pyrene (BaP) was studied. A half factorial two-level experiment 2(4-1) was designed to determine the effect of: type of lignocellulosic material (BP and PS) for fungus growth, age of fungus (5 and 10d), amount of lignocellulosic material (10% and 15% w/w) and soil moisture content (water holding capacity of 45% and 56% w/w). Inoculum obtained at different ages showed that the capacity of P. chrysosporium to remove BaP depends on the lignocellulosic used and on inoculum age. Abiotic BaP removal was affected significantly (p<0.05) by inoculum age, type of lignocellulosic added and soil moisture content. The removal of BaP by lignocellulosic material was more effective by young inocula (71.97 mg BaP kg(-1) dry soil), with high percentage of added lignocellulosic (71.57 mg BaP kg(-1) dry soil) and at low soil moisture content (73.07 mg BaP kg(-1) dry soil). When fungus was grown on BP, maximum BaP removal rate was obtained at 5d of incubation (10.85 mg BaP d(-1)l(-1) and 50.12 mg BaP kg(-1) dry soil), while in PS maximum BaP removal was obtained at 10d of incubation (12.06 mg BaP d(-1)l(-1) and 39.94 mg BaP kg(-1) dry soil).  相似文献   

5.
Benzo[a]pyrene degradation by Sphingomonas yanoikuyae JAR02   总被引:1,自引:0,他引:1  
Batch experiments were conducted to characterize the degradation of benzo[a]pyrene, a representative high molecular weight (HMW) polycyclic aromatic hydrocarbon (PAH), by Sphingomonas yanoikuyae JAR02. Concentrations up to the solubility limit (1.2 microg l(-1)) of benzo[a]pyrene were completely removed from solution within 20 h when the bacterium was grown on salicylate. Additional experiments with [(14)C]7-benzo[a]pyrene demonstrated 3.8% mineralization over 7 days when salicylate was present is solution, and one major radio-labeled metabolite was observed that accounted for approximately 10% of the initial radio-label. Further characterization of the radio-labeled metabolite using HPLC/MS and HPLC/MS/MS identified radio-labeled pyrene-8-hydroxy-7-carboxylic acid and unlabeled pyrene-7-hydroxy-8-carboxylic acid as novel ring-cleavage metabolites, and a benzo[a]pyrene degradation pathway was proposed. Results indicate that biostimulation of HMW PAH degradation by salicylate, a water-soluble, non-toxic substrate, has significant potential for in situ bioremediation.  相似文献   

6.
Effects of riboflavin on the phototransformation of benzo[a]pyrene   总被引:3,自引:0,他引:3  
Zhao X  Hu X  Hwang HM 《Chemosphere》2006,63(7):1116-1123
Riboflavin (Vitamin B2) is a natural dye-sensitizer habitually present in natural waters. Effects of riboflavin as photosensitizer on the transformation of benzo[a]pyrene (BaP) (10 microM) in the aqueous-organic solvent (water/acetonitrile/methanol 50/40/10) were investigated in this study. The photolysis half life of BaP in solution containing 50 microM riboflavin was 5 min, compared to 98 min in the absence of riboflavin. The rate of phototransformation of BaP increased as the concentration of riboflavin was raised from 10 microM to 100 microM under both natural sunlight and UVA irradiation. The half life of BaP in the presence of 50 microM riboflavin was 10.6 min and 43.1 min when exposed to visible range of natural sunlight and UVA irradiation respectively. Riboflavin decomposes under natural sunlight. Lumichrome, a principal photoproduct of riboflavin, was shown to photosensitize BaP under natural sunlight after photolysis of riboflavin. Our study indicated that other photoproducts from riboflavin, such as lumiflavin, were also involved in the phototransformation of BaP under sunlight when riboflavin diminished. The major photoproducts in the photolysis of BaP were identified as 1,6-benzo[a]pyrene-dione, 3,6-benzo[a]pyrene-dione, 6,12-benzo[a]pyrene-dione by using high performance liquid chromatography (HPLC). All these products were detected in the samples which were irradiated under different light sources and in the presence or absence of riboflavin. The possible phototransformation mechanism was discussed.  相似文献   

7.
Accumulation and elimination of polycyclic aromatic hydrocarbons (PAHs) were studied in the fungus Fusarium solani. When the fungus was grown on a synthetic medium containing benzo[a]pyrene, hyphae of F. solani contained numerous lipid vesicles which could be stained by the lipid-specific dyes: Sudan III and Rhodamine B. The fluorescence produced by Rhodamine B and PAH benzo[a]pyrene were at the same locations in the fungal hyphae, indicating that F. solani stored PAH in pre-existing lipid vesicles. A passive temperature-independent process is involved in the benzo[a]pyrene uptake and storage. Sodium azide, a cytochrome c oxidation inhibitor, and the two cytoskeleton inhibitors colchicine and cytochalasin did not prevent the transport and accumulation of PAH in lipid vesicles of F. solani hyphae. F. solani degraded a large range of PAHs at different rates. PAH intracellular storage in lipid vesicles was not necessarily accompanied by degradation and was common to numerous other fungi.  相似文献   

8.
The constancy, both temporal and spatial, of the profile of polycyclic aromatic hydrocarbons (PAHs) relative to benzo[a]pyrene (BaP) is a prerequisite to using the BaP-indicator approach in the carcinogenic risk assessment for PAHs. The principal aim of this study was to provide a contribution to validate this approach, by studying the variability of the profile at a typical urban site through a multi-year data set and by comparing the profiles available for different cities. Seven carcinogenic PAHs (benz[a]anthracene, benzo[b+j+k]fluoranthenes, BaP, indeno[1,2,3-cd]pyrene, dibenz[a,h]anthracene) were determined in PM10 24-h samples collected every third day at a road site; moreover, benzo[e]pyrene was determined as a reference PAH due to its stability. The profile was found stable from year to year. Besides, it was similar to those recently found in other European cities (observed differences within a factor of four) and to those elaborated from earlier (1970s–1980s) investigations. The substantial similarity of profiles, both temporal (on an annual basis) and spatial, supports the validity of the BaP-indicator approach. Large PAH-to-PAH differences were, however, found in the seasonal pattern of profile: they were explained by the different atmospheric degradability of PAHs, whose effect is enhanced under the meteoclimatic conditions typical of the European Mediterranean countries. PAH annual means showed a slight declining trend since 1994. In the last sampling year, mean concentration of BaP was 1.2 ng m−3. Within-year differences among monthly averaged PAH concentrations were observed, as large as up to 44-fold for BaP, underlining the need for whole-year monitoring.  相似文献   

9.
研究了非离子型表面活性剂Triton X-100(TX-100)和Tween80(TW-80)对苯并[a]芘的增溶特性及对苯并[a]芘高效降解菌Bacillus pumilus strain Bap9生长的影响,结果表明,2种表面活性剂对苯并[a]芘均有良好的增溶效果,均能作为碳源和能源被菌株Bap9所利用,TX-100增溶能力和增殖能力相对更强;不同浓度的TX-100对菌株降解苯并[a]芘的影响不同,当浓度为1 000 mg/L时,对降解的促进作用最强,可将苯并[a]芘降解率提高20.8%;在苯并[a]芘降解过程中,TX-100亦能作为碳源被菌株Bap9利用,不产生二次污染,因此可用于苯并[a]芘污染环境的生物修复。  相似文献   

10.
BACKGROUND: A climate-controlled pot experiment was conducted to investigate the effects of planting alfalfa and applying organic fertilizer on the dissipation of benzo[a]pyrene from an aged contaminated agricultural soil. RESULTS: Short-term planting of alfalfa inhibited the dissipation of benzo[a]pyrene from the soil by 8.9%, and organic fertilizer enhanced benzo[a]pyrene removal from the soil by 11.6% compared with the unplanted and unfertilized treatments, respectively. No significant interaction was observed between alfalfa and organic fertilizer on benzo[a]pyrene dissipation. Sterilization completely inhibited the removal of benzo[a]pyrene from the soil indicating that its degradation by indigenous microorganisms may have been the main mechanism of dissipation. Furthermore, significant positive relationships were observed between benzo[a]pyrene removal and the contents of soil ammonium nitrogen, nitrate nitrogen, and total mineral nitrogen at the end of the experiment, suggesting that competition between plants and microorganisms for nitrogen may have inhibited benzo[a]pyrene dissipation in the rhizosphere of alfalfa and the addition of organic fertilizer may facilitate microbial degradation of benzo[a]pyrene in the soil.  相似文献   

11.
In this study, airborne particulates were collected at three sites, two in a downtown area and the other in a suburban area of Kanazawa, Japan in each season for 7 years. Two polycyclic aromatic hydrocarbons (PAHs), pyrene (Py) and benzo[a]pyrene (BaP) and four nitropolycyclic aromatic hydrocarbons (NPAHs), 1-nitropyrene (NP) and 1,3-, 1,6-, and 1,8-dinitropyrenes (DNP) were determined by high-performance liquid chromatography with fluorescence and chemiluminescence detection. At the downtown sites, the mean concentration of each DNP was about two orders of magnitude lower than that of 1-NP and more than three orders of magnitude lower than those of Py and BaP. This tendency reflected the composition of PAHs and NPAHs in diesel-engine exhaust particulates. Concentrations of these PAHs and NPAHs were higher at the downtown sites than at the suburban site, suggesting the dilution of these compounds during the transportation from the downtown to the suburban area. The concentration ratios of NPAHs to PAHs were larger at the downtown sites than at the suburban site. Studies using UV light and sunlight showed that degradation of NPAHs was faster than that of PAHs. Thus, the lower concentrations of NPAHs in the suburban sites may be due to their being photodegraded faster than PAHs during the atmospheric transportation from the downtown area to the suburban area.  相似文献   

12.
The ethoxy resorufin dealkylase (EROD) inducing potency of 10 polycyclic aromatic hydrocarbons (PAHs) is measured in the H4IIE in vitro bioassay and the results are compared to those reported in literature. The selected PAHs varied considerably in their potency to induce EROD activity. Anthracene (Ant) and phenanthrene (Phe) showed consistently no response. Naphthalene (Nap) showed no or a very weak response on EROD activity. Fluoranthene (Fla) and benzo[g,h,i]perylene (BghiP) showed weak responses at the highest doses. The other PAHs, including indeno[1,2,3-cd]pyrene (IP), benz[a]anthracene (BaA), benzo[a]pyrene (BaP), chrysene (Chr) and benzo[k]fluoranthene (BkF), showed full bell shaped dose-response curves. BaP EROD induction equivalency factors (BaP-1EF) were calculated and increased in the order Ant approximately Phe < Fla < Nap < BghiP < IP < BaA < BaP < Chr < BkF. Comparison of BaP-IEFs based on 50% effect concentration (EC50) or lowest effect concentration (LEC), yielded a significant relationship between both methods described by the equation log(BaPIEF(EC50) = 0.55 x log(BaPIEF(LEC)) + 0.07 (r2 = 0.913). BaP-IEFs as derived from our measurements and as reported in literature and measured in other in vitro assays deviated up to a factor of 17 among the different studies, but the potency rankings were comparable. For the PAH mixture as on average present in the human diet an overall tetrachlorodibenzo-p-dioxin (TCDD)-IEF of 1 x 10(-4) was estimated. The total PAH based TCDD induction equivalents (IEQ) intake then was calculated 300 pg/day, which is approximately 2 times higher then the PHAH based TCDD-EQ intake reported for humans.  相似文献   

13.
An innovative process that combines soil electrokinetic remediation and liquid electrochemical oxidation for the degradation of organic compounds present in a polluted soil was developed and evaluated by using benzo[a]pyrene spiked kaolin. In order to increase benzo[a]pyrene solubility during electrokinetic treatment, the addition of a co-solvent or surfactant, such as ethanol or Brij 35, as flushing solution was tested. The research carried out demonstrated the influence of the desorption agent employed on benzo[a]pyrene remediation from the kaolin matrix. Thus, if the flushing solution was ethanol at 40%, there was no presence of contaminant in either chamber. On the contrary, when a solution of surfactant Brij 35 was used, benzo[a]pyrene was transported towards the cathode chamber, where it was collected. Moreover, the extent of this recovery depends on the pH profile on the soil. When no pH control was used, around 17% of initial contaminant was detected in the cathode chamber; however, when pH control was applied, the recovery of benzo[a]pyrene could be higher than 76%, when the pH control in the anode chamber was set at 7.0.In order to obtain the total degradation of mobilised benzo[a]pyrene from the contaminated soil, the liquid collected by electrokinetic remediation was oxidised by electrochemical treatment. This oxidation was accomplished via an electrochemical cell with a working volume of 0.4 L, and graphite as electrode material. The benzo[a]pyrene was almost totally degraded in 1 d, reaching a degradation of about 73% in 16 h.  相似文献   

14.
A microcosm experiment was conducted to investigate the dissipation of available benzo[a]pyrene (BaP) in soils co-contaminated with cadmium (Cd) and pyrene (PYR) during aging process. The available residue of BaP in soil was separated into desorbing and non-desorbing fractions. The desorbing fraction contributed more to the dissipation of available BaP than the non-desorbing fraction did. The concentration of bound-residue fraction of BaP was quite low across all treatments. Within the duration of this study (250 days), transformation of BaP from available fractions to bound-residue fraction was not observed. Microbial degradation was the dominant mechanism of the dissipation of available BaP in the soil. The dissipation of available BaP was significantly inhibited with the increment in Cd level in the soil. The addition of PYR (250 mg kg?1) remarkably promoted the dissipation of available BaP without reducing Cd availability in the soil. The calculated half-life of available BaP in the soil prolonged with the increment in Cd level; however, the addition of PYR shortened the half-life of available BaP by 13.1, 12.7, and 32.8 % in 0.44, 2.56, and 22 mg Cd kg?1 soils, respectively. These results demonstrated that the inhibiting effect of Cd and the promoting effect of PYR on the dissipation of available BaP were competitive. Therefore, this study shows that the bioremediation process of BaP can be more complicated in co-contaminated soils.  相似文献   

15.
Benzo[a]pyrene, a high molecular weight (HMW) polycyclic aromatic hydrocarbon (PAH) was removed from solution by Sphingomonas yanoikuyae JAR02 while growing on root products as a primary carbon and energy source. Plant root extracts of osage orange (Maclura pomifera), hybrid willow (Salix albaxmatsudana), or kou (Cordia subcordata), or plant root exudates of white mulberry (Morus alba) supported 15-20% benzo[a]pyrene removal over 24 h that was similar to a succinate grown culture and an unfed acetonitrile control. No differences were observed between the different root products tested. Mineralization of (14)C-7-benzo[a]pyrene by S. yanoikuyae JAR02 yielded 0.2 to 0.3% (14)CO(2) when grown with plant root products. Collectively, these observations were consistent with field observations of enhanced phytoremediation of HMW PAH and corroborated the hypothesis that co-metabolism may be a plant/microbe interaction important to rhizoremediation. However, degradation and mineralization was much less for root product-exposed cultures than salicylate-induced cultures, and suggested the rhizosphere may not be an optimal environment for HMW PAH degradation by Sphingomonas yanoikuyae JAR02.  相似文献   

16.
Ishii S  Hisamatsu Y  Inazu K  Kobayashi T  Aika K 《Chemosphere》2000,41(11):1809-1819
In order to clarify the contribution of nitrated products to the direct-mutagenic activity of products of the reactions of benzo[a]pyrene in NO2-air under various conditions, heterogeneous reactions of BaP deposited on filter in the air containing 10 ppm of NO2 have been conducted in dark or under photoirradiation. The reaction products have been analyzed by gas chromatography and mutagenicity of the products fractionated by preparative HPLC was assayed for Salmonella typhimurium strains TA98 and YG1024 in the absence of S9 mix. 3,6-dinitrobenzo[a]pyrene and 1,3-dinitrobenzo[a]pyrene, which are strong direct-acting mutagens, largely contributed to the total direct-acting mutagenicity of the dark reaction products in NO2-air. On the other hand, both the dark reaction in the presence of O3 and the photoreaction in NO2-air resulted in the formation of much smaller amounts of nitrobenzo[a]pyrenes than that observed in the dark reaction in the absence of O3. These results show that the contribution of other direct-acting mutagens to the total direct-acting mutagenicity of the products in these reactions should be considered. Benzo[a]pyrene lactones were identified in a highly mutagenic fraction of the products of the dark reaction in the presence of O3 and photoreaction and a nitrobenzo[a]pyrene lactone was also identified in a highly mutagenic fraction of the dark reaction products in the presence of O3. Nitrated oxygenated benzo[a]pyrene derivatives such as nitrobenzo[a]pyrene lactone were considered to largely contribute to direct-acting mutagenicity of the products of the dark reaction in the presence of O3 and photoreaction.  相似文献   

17.
研究了非离子型表面活性剂Triton X-100(TX-100)和Tween80(TW-80)对苯并[a]芘的增溶特性及对苯并[a]芘高效降解菌Bacillus pumilus strain Bap9生长的影响,结果表明,2种表面活性剂对苯并[a]芘均有良好的增溶效果,均能作为碳源和能源被菌株Bap9所利用,TX-100增溶能力和增殖能力相对更强;不同浓度的TX-100对菌株降解苯并[a]芘的影响不同,当浓度为1 000 mg/L时,对降解的促进作用最强,可将苯并[a]芘降解率提高20.8%;在苯并[a]芘降解过程中,TX-100亦能作为碳源被菌株Bap9利用,不产生二次污染,因此可用于苯并[a]芘污染环境的生物修复。  相似文献   

18.
The capabilities of selected strains from genera Lactobacillus and Bifidobacterium to produce extracellular bioactive compounds with antimutagenic properties against benzo[a]pyrene (BaP) and sodium azide (SA) were tested as a function of growth phase. The bacterial supernatants from exponential and stationary phases were characterized with different patterns of antimutagenic activity against the two mutagens. All lactobacilli exhibited either no effect or low antimutagenicity against BaP during exponential growth. Higher antimutagenic activities of lactobacilli supernatants were observed in the stationary phase against SA as well. An exception was Lactobacillus sakei 23K which expressed a relatively low percent of inhibition of mutagenesis (PI = 28.14 +/- 7.41) in the exponential phase and no antimutagenic activity in the stationary phase. Of the bifidobacteria, only Bifidobacterium adoleascentis ATCC 15703 exhibited higher antimutagenecity against BaP in the exponential phase. The same bacterial supernatants however, did not possess any antimutagenicity against SA in either the exponential or stationary phases. B. bifidum ATCC 11863 did not express any significant differences in its activity against either BaP or SA in the exponential or stationary phases. Only B. breve ATCC 15700 expressed a high antimutagenic effect against SA in the stationary phase but exhibited no effect during exponential growth. Overall, bacterial antimutagenic responses were associated with growth phase and type of mutagen.  相似文献   

19.
Chelating sorbents with diethylenetriaminepenta(methylene-phosphonic acid) (DTPMPA) and ethylenediaminetetraacetic acid ligands immobilized on zirconia matrix were prepared and subsequently saturated with Cu(II). All the Cu chelates catalyzed decomposition of H(2)O(2) yielding highly reactive hydroxyl radicals. All of them were also able to catalyze degradation of polycyclic aromatic hydrocarbons (anthracene, benzo[a]pyrene and benzo[b]fluoranthene). The most effective DTPMPA-based catalysts G-32 and G-35 (10 mg ml(-1) with 100 mmol H(2)O(2)) caused almost complete decomposition of 15 ppm anthracene and benzo[a]pyrene during a five day catalytic cycle at 30 degrees C. Anthracene-1,4-dione was the main product of anthracene oxidation by all catalysts. The catalysts were active in several cycles without regeneration.  相似文献   

20.
《Chemosphere》1986,15(6):675-685
Five polycyclic aromatic hydrocarbons (PAH), pyrene (PY), fluoranthene (FL), benz(a)anthracene (BaA), benzo(a)pyrene (BaP), and benzo(e)pyrene (BeP) adsorbed on glass fiber (GF) and Teflon impregnated glass fiber (TIGF) filters and on ambient particulate organic matter (POM) were exposed to ozone (50–300 ppb) passively in a 360-liter Teflon chamber and actively in a flow system. The influence of ozone concentration, exposure time and relative humidity (RH) on the degree of degradation of these PAH was established. The most reactive PAH both on filters and in ambient POM were PY, BaA and BaP. Up to 50–80% of these PAH degraded in 3-hr exposures to 200 ppb of ozone at ∼1% RH; in a flow system, most of the degradation occurred within the first 10 minutes of exposure. With the exception of BaP, the degradation of the PAH tested on GF and TIGF filters were much lower at 50% RH than at 1% RH, whether they were exposed to ozone in an active or passive mode. Interestingly, RH did not significantly affect the reactivity of PAH present in ambient POM passively exposed to ozone. Our results show that PAH are susceptible to ozone degradation under many typical atmospheric conditions.  相似文献   

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