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1.
This paper reports the effect of chimneys in reducing indoor air pollution in a lung cancer epidemic area of rural China. Household indoor air pollution concentrations were measured during unvented burning (chimneys blocked) and vented burning (chimneys open) of bituminous coal in Xuan Wei, China. Concentrations of particulate matter with an aerodynamic diameter of 10 μm or less (PM10) and of benzo[a]pyrene (BaP) were measured in 43 homes during normal activities. The use of chimneys led to significant decreases in indoor air concentrations of particulate matter with an aerodynamic diameter of 10 μm or less (PM10) by 66% and of benzo[a]pyrene (BaP) by 84%. The average BaP content of PM10 also decreased by 55% with the installation of a chimney. The reduction of indoor pollution levels by the installation of a chimney supports the epidemiology findings on the health benefits of stove improvement. However, even in the presence of a chimney, the indoor air concentrations for both PM10 and BaP still exceeded the indoor air quality standards of China. Movement up the energy ladder to cleaner liquid or gaseous fuels is probably the only sustainable indoor air pollution control measure.  相似文献   

2.
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   

3.
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   

4.
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   

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.
The condensation properties of polydisperse aged ultrafine carbon aerosols (particle diameter<1 μm) have been investigated by means of a variable supersaturation condensation nucleus counter. The critical supersaturation (Sc), as the point, where 50% of all particles have been activated and grew to droplets was compared to the median dry particle diameter for pure carbon aerosols, benzo[a]pyrene-tagged carbon aerosols and external mixtures of the carbon particles with sodium chloride and sulphuric acid aerosols. Additionally, ozone as oxidising gaseous compound was added in some of the experiments. Simple coagulation of pure and benzo[a]pyrene-tagged carbon particles resulted in only slightly lower values for Sc due to the increased median particle diameter. The formation of soluble functionalities on the particle surface, i.e. the coagulation with the soluble sodium chloride and sulphuric acid aerosols or the chemical decomposition of benzo[a]pyrene into polar, hydrophilic products due to the reaction with ozone resulted in significant lower values for Sc for the modified carbon aerosol. The necessary supersaturations for the increased hydrophilic particles dropped to atmospherically relevant values of 3% after 5 h reaction time (benzo[a]pyrene decomposition) and 15 h (coagulation with soluble particles), respectively.  相似文献   

7.
The reactivity of selected polycyclic aromatic hydrocarbons (PAH) adsorbed to various surfaces has been studied. PAH were adsorbed to silica, alumina or charcoal particles and exposed to ambient concentrations of NO2 in air in a fluidized bed reactor. The reaction products were analyzed by capillary gas chromatography and gas chromatograpy/mass spectrometry.The results show that silica is a more reactive surface than alumina. The charcoal used showed to be very adsorbtive and too little material was recovered for analyses. The reactivity of the PAH compounds studied decrease in the order perylene > benzo(a)pyrene > pyrene > chrysene > fluoranthene and phenanthrene. The relevance of these results to the assessment of the possible formation of nitro-PAH in the atmosphere is discussed.  相似文献   

8.
In the present study, photocatalytic reactions of nitrogen oxides (NOx = NO + NO2) were studied on commercial TiO2 doped facade paints in a flow tube photoreactor under simulated atmospheric conditions. Fast photocatalytic conversion of NO and NO2 was observed only for the photocatalytic paints and not for non-catalytic reference paints. Nitrous acid (HONO) was formed in the dark on all paints studied, however, it efficiently decomposes under irradiation only on the photocatalytic samples. Thus, it is concluded that photocatalytic paint surfaces do not represent a daytime source of HONO, in contrast to other recent studies on pure TiO2 surfaces. As main final product, the formation of adsorbed nitric acid/nitrate anion (HNO3/NO3?) was observed with near to unity yield. In addition, traces of H2O2 were observed in the gas phase only in the presence of O2. Formation of the greenhouse gas nitrous oxide (N2O) could be excluded. The uptake kinetics of NO, NO2 and HONO was very fast under atmospheric conditions (e.g. γ(NO + TiO2) > 10?5). Thus, the uptake on urban surfaces (painted houses, etc.) will be limited by transport. For a hypothetically painted street canyon, an average reduction of nitrogen oxide levels of ca. 5% is estimated. Since the harmful HNO3/NO3? is formed on the surface of the photoactive paints, whereas it is formed in the gas phase in the atmosphere, the use of photocatalytic paints may also help to reduce acid deposition, e.g. on plants, or nitric acid related health issues.  相似文献   

9.
The bioaccumulation of two isomeric non-alternant non-priority polycyclic aromatic hydrocarbons (PAHs), namely cyclopenta[cd]pyrene and benzo[ghi]fluoranthene, was investigated in caged mussels (Mytilus galloprovincialis) exposed for 30 days in three sites of a coastal lagoon (Pialassa Baiona, Ravenna, Italy) contaminated by pyrogenic PAHs. The concentration of cyclopenta[cd]pyrene and benzo[ghi]fluoranthene increased from undetectable levels in reference mussels withdrawn from the Adriatic sea to 10-30 ng g(-1) dry weight in transplanted mussels. Other contaminants bioaccumulated by caged mussels included pyrene, fluoranthene and mercury. Whilst the isomer concentration ratio pyrene/fluoranthene in biota was comparable to that observed in sediments, the cyclopenta[cd]pyrene/benzo[ghi]fluoranthene ratio was much lower in mussels than in sediments. The lower sediment biota accumulation factor of cyclopenta[cd]pyrene with respect to that of benzo[ghi]fluoranthene was tentatively attributed to the greater biological activity of the former compound, which contains a reactive olefinic bond in the cyclopenta fused ring moiety. Given the higher mutagenic activity of cyclopenta[cd]pyrene with respect to other priority PAHs, its bioaccumulation from contaminated sediments may rise considerably the overall toxicity of PAH residues in exposed biota.  相似文献   

10.
The microbial degradation of 14C-pyrene and 14C-benzo[a]pyrene by a bacterial mixed culture was studied within a mixture of the PAHs phenanthrene, anthracene, pyrene, fluoranthene, and benzo[a]pyrene as sole carbon source in the different culture systems: (i) liquid medium, (ii) soil slurry (surface and grinding influence), and (iii) soil. The fate of these two labeled compounds was followed in these systems with an emphasis on mineralization to carbon dioxide, extractability, and adsorption to humic materials and formation of unextractable residual. Mineralization showed the most obvious differences: soil slurries achieved the best results both concerning the extent of mineralization and the time required. The highest extent of pyrene mineralization (54% within 21 days) was observed in soil slurries; in liquid media, pyrene mineralization was slower, but reached approximately the same extent (54% in 150 days); in soils, mineralization reached only 36% of added pyrene after 160 days. Benzo[a]pyrene was mineralized in a mixture of PAHs in soil slurries to an extent of 34% within 70 days, whereas mineralization in liquid medium and soil occurred in the range of 5% (70 days). Mineralization of benzo[a]pyrene in sand slurries was lower compared to soil slurries (19% in sand slurries vs. 32% in soil slurries within 50 days).  相似文献   

11.
Thirteen river waters and one humic lake water were characterized. The effects of dissolved organic matter (DOM) on the bioavailability of atrazine, pyrene and benzo[a]pyrene (B[a]P) was evaluated. Binding of the chemicals by DOM was analyzed with the equilibrium dialysis technique. For each of the water samples, 24 h bioconcentration factors (BCFs) of the chemicals were measured in Daphnia magna. The relationship between DOM and other water characteristics (including conductivity, water hardness and pH), and bioavailability of the chemicals was studied by performing several statistical analyses, including multiple regression analyses, to determine how much of the variation of BCF values could be explained by the quantity and quality of DOM. The bioavailability of atrazine was not affected by DOM or any other water characteristics. Although equilibrium dialysis showed binding of pyrene to DOM, the bioavailability of pyrene was not significantly affected by DOM. The bioavailability of B[a]P was significantly affected by both the quality and quantity of DOM. Multiple regression analyses, using the quality (ABS270 and HbA%) and quantity of DOM as variables, explained up to 70% of the variation in BCF of B[a]P in the waters studied.  相似文献   

12.
This work deals with the kinetic study of the reactions of ozone with pyrene, 1-hydroxypyrene and 1-nitropyrene, adsorbed on model particles. Experiments were performed at room temperature and atmospheric pressure, using a quasi-static flow reactor in the absence of light. Compounds were extracted from particles using pressurized fluid extraction (PFE) and concentration measurements were performed using gas chromatography/mass spectrometry (GC/MS). The pseudo-first order rate constants were obtained from the fit of the experimental decay of particulate polycyclic compound concentrations versus reaction time. Experiments were performed at three different O3 concentrations from which second order rate constants were calculated. The following rate constant values were obtained at 293 K: k(O3 + Pyrene) = (3.2 ± 0.7) × 10?16 cm3 molecule?1 s?1; k(O3 + 1OHP) = (7.7 ± 1.4) ×10 ?16 cm3 molecule?1 s?1; and k(O3 + 1NP) = (2.2 ± 0.5) × 10?17 cm3 molecule?1 s?1, for pyrene, 1-hydroxypyrene and 1-nitropyrene adsorbed on silica particles. The variation in the rate constants demonstrates the strong influence of the substituent (OH or NO2) on the heterogeneous reactivity of pyrene. The pyrene particulate concentration was also varied in order to check how this parameter may influence the experiments. Finally, oxidation products were investigated for all reactions and some were detected and identified for the first time for ozone heterogeneous reaction with pyrene adsorbed on particles.  相似文献   

13.
The heterogeneous reactivity of nitrogen dioxide with pyrene and 1-nitropyrene (1NP) adsorbed on silica particles has been investigated using a fast-flow-tube in the absence of light. Reactants and products were extracted from particles using pressurised fluid extraction (PFE) and concentration measurements were performed using gas chromatography/mass spectrometry (GC/MS). The pseudo-first order rate constants were obtained from the fit of the experimental decay of particulate polycyclic compound concentrations versus reaction time. Experiments were performed at three different NO2 concentrations and second order rate constants were calculated considering the oxidant concentration. The following rate constant values were obtained at room temperature: k(NO2 + pyrene) = (9.3 ± 2.3) × 10?17 cm3 molecule?1 s?1 and k(NO2 + 1NP) = (6.2 ± 1.5) × 10?18 cm3 molecule?1 s?1, showing that the reactivity of 1NP was slower by a factor of 15 than that of pyrene. 1NP was identified as the only NO2-initiated oxidation product of pyrene and all the three dinitropyrenes were identified in the case of the 1NP reaction. The product quantification allowed showing that the kinetics of oxidation product formation was equal to that measured for parent compounds degradation, within uncertainties, confirming the validity of the reaction kinetics measurements.  相似文献   

14.
Abstract

The ozone (O3) sensitivity to nitrogen oxides (NOx, or nitric oxide [NO] + nitrogen dioxide [NO2]) versus volatile organic compounds (VOCs) in the Mexico City metropolitan area (MCMA) is a current issue of scientific controversy. To shed light on this issue, we compared measurements of the indicator species O3/NOy (where NOy represents the sum of NO + NO2 + nitric acid [HNO3] + peroxyacetyl nitrate [PAN] + others), NOy, and the semiempirically derived O3/NOz surrogate (where NOz surrogate is the derived surrogate NOz, and NOz represents NOx reaction products, or NOy – NOx) with results of numerical predictions reproducing the transition regimes between NOx and VOC sensitivities. Ambient air concentrations of O3, NOx, and NOy were measured from April 14 to 25, 2004 in one downwind receptor site of photo-chemically aged air masses within Mexico City. MCMA-derived transition values for an episode day occurring during the same monitoring period were obtained through a series of photochemical simulations using the Multiscale Climate and Chemistry Model (MCCM). The comparison between the measured indicator species and the simulated spatial distribution of the indicators O3/NOy, O3/NOz surrogate, and NOy in MCMA suggest that O3 in this megacity is likely VOC-sensitive. This is in opposition to past studies that, on the basis of the observed morning VOC/NOx ratios, have concluded that O3 in Mexico City is NOx-sensitive. Simulated MCMA-derived sensitive transition values for O3/NOy, hydrogen peroxide (H2O2)/HNO3, and NOy were found to be in agreement with threshold criteria proposed for other regions in North America and Europe, although the transition crossover for O3/NOz and O3/HNO3 was not consistent with values reported elsewhere. An additional empirical evaluation of weekend/weekday differences in average maximum O3 concentrations and 6:00- to 9:00-a.m. NOx and NO levels registered at the same site in April 2004 indirectly confirmed the above results. A preliminary conclusion is that additional reductions in NOx emissions in MCMA might cause an increase in presently high O3 levels.  相似文献   

15.
After intravenous injection of 3-hydroxybenzo (a) pyrene into rat, benzo (a) pyrene-diols were detected in urine, and in vitro experiment using isolated hepatocytes and sliced kidney also indicated the metabolism of 3-hydroxybenzo (a) pyrene to diol derivatives. THese results suggested the presence of unknown metabolic pathway of benzo (a) pyrene-phenols such as 3-hydroxybenzo (a) pyrene to diol derivatives both in vivo and in vitro.  相似文献   

16.
Diesel particulate matter poses a threat to human health, and in particular nitrated polycyclic aromatic hydrocarbons (NPAHs) found within and on the surface of these particles. Although diesel particulate filters (DPFs) have been designed and implemented to reduce these and other harmful diesel emissions, the particle loaded filters may act as a reaction chamber for the enhanced production of NPAHs from the nitration of PAHs with NO2.Focus is on the investigation of the heterogeneous reactions that occur on soot particles by exposing laboratory produced pyrene- or benzo(a)pyrene-coated spark discharge soot particles to varying concentrations of NO2 and temperatures while following the formation of products over time. The sole nitration product that was observed throughout the experiments with pyrene-coated soot was 1-nitropyrene (1-NPYR), which increased linearly with reaction time for all NO2 concentrations chosen (0.11, 1.0, 2.0, 4.0 ppm, m m?1). Resulting 1-NPYR formation rate increased exponentially with [NO2]. Throughout the 3-h experiments less than 10% of pyrene has been converted to 1-NPYR and the partial reaction order with regard to [NO2] was estimated to 1.52. Benzo(a)pyrene (BaP) was more reactive than pyrene. After 3 h reaction time almost 80% of the BaP has been converted to 6-NBaP.Highest 1-NPYR concentrations on particles were detected at 373 K, and at higher temperatures a considerable decrease in particulate 1-NPYR was observed. A similar trend was observed in a DPF simulation system (PM-Kat®-like) with BaP-coated soot. In this case, highest 6-NBaP concentration on particles was detected at 423 K. Backed by corroborating results from separate gas/solid-phase partition experiments with 1-NPYR and 6-NBaP, it is likely that the newly formed 1-NPYR and 6-NBaP became transferred from particle to gas phase at higher temperatures. Results from this study confirm the presence of 1-NPYR and 6-NBaP in particulate and gas phase under conditions encountered in DPFs, especially when operated at low temperature situations of the aftertreatment system.  相似文献   

17.
The removal of pyrene and benzo(a)pyrene from contaminated water by sequential and simultaneous ozonation-bioremediation techniques was investigated. During the sequential treatment, ozonation using 0.5 or 2.5 mg/L ozone was used as a pretreatment process, whereas, during the simultaneous treatment process, ozonation of hydrocarbon-contaminated water at a predetermined duration using 0.5 mg/L ozone was made in the presence of microbial biomass. Ozonation was not beneficial for the removal of pyrene. However, despite a decreased specific biodegradation rate, ozonation improved the overall elimination of benzo(a)pyrene during both treatment processes. The overall removal of benzo(a)pyrene increased from 23 to 91% after exposure of the water to 0.5 mg/L ozone for 30 minutes during the simultaneous treatment process and further to 100% following exposure to 2.5 mg/L ozone for 60 minutes during the sequential treatment mode, demonstrating the benefits of combined ozonation-biological treatment for the removal of polycyclic aromatic hydrocarbons.  相似文献   

18.
The fate of spiked anthracene, pyrene and benzo[a]pyrene in soil with or without sewage sludge compost was assessed during a 6-month bioremediation process simulating landfarming. Bioassays and physico-chemical analyses were employed to monitor toxicity change in soil samples and elutriates through ten sampling campaigns. Pearson product-moment correlation coefficient was determined to measure the strength of relationship between bioassays and physico-chemical analyses. The PAH dissipation in soil was enhanced after the first water addition, and the remaining amounts at the end of the experiment were positively correlated to the number of benzene rings and the presence of sewage sludge compost. Toxicity of soil elutriates to Daphnia magna was evident at early stages, originating exclusively from sewage sludge compost amendment. The lettuce root elongation was continuously inhibited by elutriates for all the treatments including control soil, probably due to high salinity or to unaddressed leachable phytotoxic compounds that were present in the experimental soil. The newly developed direct solid-phase chronic toxicity test using ostracod (Heterocypris incongruens) succeeded in evaluating the soil-bound PAH toxicity, as PAHs could not be detected in elutriates.  相似文献   

19.
The livers of soles (Solea senegalensis) injected with subacute doses of cadmium (Cd), benzo[a]pyrene (B[a]P), or their combination, were screened for alterations to cytosolic protein expression patterns, complemented by cytological and histological analyses. Cadmium and B[a]P, but not combined, induced hepatocyte apoptosis and Kupfer cell hyperplasia. Proteomics, however, suggested that apoptosis was triggered through distinct pathways. Cadmium and B[a]P caused upregulation of different anti-oxidative enzymes (peroxiredoxin and glutathione peroxidase, respectively) although co-exposure impaired induction. Similarly, apoptosis was inhibited by co-exposure, to which may have contributed a synergistic upregulation of tissue metalloproteinase inhibitor, β-actin and a lipid transport protein. The regulation factors of nine out of eleven identified proteins of different types revealed antagonistic or synergistic effects between Cd and B[a]P at the prospected doses after 24 h of exposure. The results indicate that co-exposure to Cd and B[a]P may enhance toxicity by impairing specific responses and not through cumulative damage.  相似文献   

20.
A saturated solution of pyrene in water was not toxic to the fish , even in the presence of ultraviolet light. A survival curve possessing one minimum, and therefore defining two LC50 values, was obtained when fish placed in water containing increasing amounts of a pyrene solution in dimethylsulfoxide were exposed to ultraviolet light after a short incubation period. The phototoxicity was linked to the presence of undissolved pyrene. A normal survival curve with only one LC50 value was found when pyrene was solubilized with the surfactant Tween-20. Practically no phototoxicity was produced when the pyrene mixtures were filtered before use, or when a saturated aqueous solution of pyrene was used. Piperonyl butoxide, present at a concentration where it was not toxic, synergized the toxicity of pyrene . The environmental significance of this observation may be considerable.  相似文献   

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