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1.

Purpose

The aim of this study was to determine the mutual relations between polycyclic aromatic hydrocarbons (PAHs) originated from atmospheric emissions and enzymatic activity and humic substances in soils at differently urbanized area, on an example of the Lublin city, east Poland.

Materials and methods

The chosen areas represented three differently urbanized environments: old tenement houses and modern residential blocks, mixture of different building and rural landscape, and typical rural environment with smallholding farms, respectively. On each of the urban, suburban, and rural areas, one representative plot was chosen on fallow lands classified as luvisol derived from loess. The soil samples were collected from the top 25 cm layer. The following properties were determined: pH, organic carbon, total nitrogen, humic and fulvic acids, PAHs content (14 PAHs from US EPA list), and the activities of the following enzymes: dehydrogenases, acid phosphatase, alkane phosphatase, protease, and urease.

Results and discussion

Higher contents of organic C and total N were found in the rural soil samples. The share of humic acid was similar in all soils investigated, ranging from 19.38 to 25.27%, while fulvic acid values differ significantly between urban and rural areas. The urban soils indicated much lower share of fulvic acids (9.78–10.99%) than those of rural (29.02–29.32%). Consequently, the values of the CHA:CFA ratio of the urban soil were approximately two times higher than those of the rural soil. The results showed that both the rate of humification and the activity of dehydrogenases, acid phosphatase, alkaline phosphatase, and proteases in the soils increased in the following sequence: urban < suburban < rural.

Conclusions

The results showed that an increase of PAHs in the urbanized areas affect other soil properties. The phenanthrene/anthracene and fluoranthene/pyrene ratios pointed to coal combustion as the principal source of PAHs in the investigated soils. The PAH content in the urbanized area inhibit humification processes in the soil and the activity of dehydrogenases, acid phosphatase, alkaline phosphatase, and proteases.
  相似文献   

2.

Purpose

Little information is available heretofore on the gradient distribution of persistent organic pollutants in rhizosphere on a field scale. In this field study, we seek to explore the in situ distribution gradient of polycyclic aromatic hydrocarbons (PAHs) in rhizosphere soil proximal to the roots.

Materials and methods

Clover (Trifolium pratense L.) and hyssop (Hyssopus officinalis L.) grew in situ in the contaminated field soil near a petrochemical plant and were harvested when about 30 cm tall with mature roots. Rhizosphere soils of the plants were sampled including the rhizoplane, strongly adhering soil, and loosely adhering soil. Eleven EPA-priority PAHs were detected in each layer of rhizosphere soils in proximity to the root surface.

Results and discussion

The PAH concentrations followed the descending order of bulk soil, loosely adhering soil, strongly adhering soil, and rhizoplane soil in proximity to the root surface of clover and hyssop. The rhizosphere effect (R, in percent) on PAH distribution clearly decreased with increasing distance from the root, and a more significant decrease was observed for hyssop compared to clover. R values were generally lower for three- and four-ringed PAHs in the rhizosphere, which were more significant in loosely and strongly adhering rhizosphere layers.

Conclusions

Our field observations combined with previous potted studies demonstrated that PAH concentrations in rhizosphere soils increased with distance from the root. Results of this work provide new information on the fate of PAHs in rhizosphere.  相似文献   

3.

Purpose

Polycyclic aromatic hydrocarbons (PAHs) are largely accumulated in soils in China. The immobilized-microorganism technique (IMT) is a potential approach for abating soil contamination with PAHs. However, few studies about the application of IMT to contaminated soil remediation were reported. Due to recalcitrance to decomposition, biochar application to soil may enhance soil carbon sequestration, but few studies on the application of biochars to remediation of contaminated soil were reported. In this study, we illustrated enhanced bioremediation of soil having a long history of PAH contamination by IMT using plant residues and biochars as carriers.

Materials and methods

Two PAH-degrading bacteria, Pseudomonas putida and an unidentified indigenous bacterium, were selected for IMT. The extractability and biodegradation of 15 PAHs in solution and an actual PAH-contaminated soil amended with immobilized-bacteria materials were investigated under different incubation periods. The effects of carriers and the molecular weight of PAHs on bioremediation efficiency were determined to illustrate their different bio-dissipation mechanisms of PAHs in soil.

Results and discussion

The IMT can considerably enhance the removal of PAHs. Carriers impose different effects on PAH bio-dissipation by amended soil with immobilized-bacteria, which can directly degrade the carrier-associated PAHs. The removal of PAHs from soil depended on PAH molecular weight and carrier types. Enhanced bio-dissipation by IMT was much stronger for 4- and 5-ring PAHs than for 3- and 6-ring ones in soil. Only P400 biochar-immobilized bacteria enhanced bio-dissipation of all PAHs in contaminated soil after a 90-day incubation.

Conclusions

Biochar can promote bioremediation of contaminated soil as microbial carriers of IMT. It is vital to select an appropriate biochar as an immobilized carrier to stimulate biodegradation. It is feasible to use adsorption carriers with high sorptive capabilities to concentrate PAHs as well as microorganisms and thereby enhance dissipation of PAHs and mitigate soil pollution.  相似文献   

4.

Purpose

The purpose of this study was to elucidate historical trends, spatial variations, and the sources of polycyclic aromatic hydrocarbons (PAHs) pollution in several Japanese lakes.

Materials and methods

The vertical distributions of PAHs in the core samples of sediments taken at several points in lakes Kasumigaura, Suwa, Kizaki, and Shinji were determined using a gas chromatograph equipped with a mass selective detector and combined with chronological information and the physical/elemental properties of the sediment.

Results and discussion

Seventeen related compounds (congeners) typically had concentration peaks at sediment depths corresponding to the 1960s to 1970s. In Lake Shinji and one bay of Lake Kasumigaura, there was a tendency for PAH concentrations to increase downstream; in contrast, another bay of Lake Kasumigaura showed the reverse trend. During big flood events, the fluxes of PAHs increased due to large inputs of particulate matter, although PAH concentrations were reduced. For the four study lakes and other similar lakes, PAH concentrations of surface sediments were approximately proportional to population densities in the respective watersheds, while the total input of PAHs to the lakes were correlated with their population and watershed area. The source apportionment analysis using isomer ratios for the congener profiles indicated that the principal sources of the PAHs in the lake sediments were gasoline and/or diesel engine exhausts and biomass burning.

Conclusions

The observed concentration peaks showed a deterioration of the chemical quality of atmospheric conditions around 1960?C1970 and a recent tendency for their amelioration. Between-lake differences suggest that the influence of human activity in the watersheds influences sediment PAH concentrations. The PAH sources were identified to be of pyrogenic origin.  相似文献   

5.

Purpose

A major challenge to phytoremediation of co-contaminated soils is developing strategies for efficient and simultaneous removal of multiple pollutants. A pot experiment was conducted to investigate the potential for enhanced phytoextraction of cadmium (Cd) by Sedum alfredii and dissipation of polycyclic aromatic hydrocarbons (PAHs) in co-contaminated soil by application of pig manure vermicompost (PMVC).

Materials and methods

Soil contaminated by Cd (5.53?mg?kg?1 DW) was spiked with phenanthrene, anthracene, and pyrene together (250?mg?kg?1 DW for each PAH). A pot experiment was conducted in a greenhouse with four treatments: (1) soil without plants and PMVC (Control), (2) soil planted with S. alfredii (Plant), (3) soil amended with PMVC at 5?% (w/w) (PMVC), and (4) treatment 2?+?3 (Plant?+?PMVC). After 90?days, shoot and root biomass of plants, Cd concentrations in plant and soil, and PAH concentrations in soil were determined. Abundance of PAH degraders in soil, soil bacterial community structure and diversity, and soil enzyme activities and microbial biomass carbon were measured.

Results and discussion

Application of PMVC to co-contaminated soil increased the shoot and root dry biomass of S. alfredii by 2.27- and 3.93-fold, respectively, and simultaneously increased Cd phytoextraction without inhibiting soil microbial population and enzyme activities. The highest dissipation rate of PAHs was observed in Plant?+?PMVC treatment. However, neither S. alfredii nor PMVC enhanced PAH dissipation when applied separately. Abundance of PAH degraders in soil was not significantly related to PAH dissipation rate. Plant?+?PMVC treatment significantly influenced the bacterial community structure. Enhanced PAH dissipation in the Plant?+?PMVC treatment could be due to the improvement of plant root growth, which may result in increased root exudates, and subsequently change bacterial community structure to be favorable for PAH dissipation.

Conclusions

This study demonstrated that remediation of Cd and PAHs co-contaminated soil by S. alfredii can be enhanced by simultaneous application of PMVC. Long-term evaluation of this strategy in co-contaminated field sites is needed.  相似文献   

6.

Purpose

The assessing bias of rhizosphere effect on polycyclic aromatic hydrocarbons (PAHs) degradation in soils would come out from formation of nonextractable PAHs and extractability difference of various solvents. The aim of this study was to evaluate the role of rhizosphere effect in long-term PAHs polluted soils by using sequential extraction approach.

Material and methods

The scheme of sequential extraction included methanol/water extractable PAHs, butanol extractable PAHs, DCM extractable PAHs, humic acid-bound PAHs, crude humin-bound PAHs, and organic-C enriched humin-bound PAHs. PAHs in plant tissues were extracted by dichloromethane after saponifying. The correlations between PAHs in plant tissues and sequentially extracted fractions were generated by partial least squares regression.

Results and discussion

The profiles of sequentially extracted PAHs varied with plant species. The discrepancy of toxicity equivalency concentrations between rhizosphere and bulk soils was much more significant than that of total PAHs concentrations. In partial least squares regression models, the concentration of PAHs in plant tissues was correlated with fractions strongly associated with soil.

Conclusions

The novelty of this study is the evaluation of concentration and toxicity equivalency concentration of PAHs in rhizosphere of crops sampled in a field polluted with PAHs for long term. This study has highlighted more significant role of rhizosphere in cleanup of cancerogenic toxicity of soil than amount of PAHs in polluted soils.  相似文献   

7.

Purpose

The choice and timing of microorganisms added to soils for bioremediation is affected by the dominant bioavailable contaminants in the soil. However, changes to the concentration of bioavailable PAHs in soil are not clear, especially when several PAHs coexist. This study investigated the effects of PAH concentration and chemical properties on desorption in meadow brown soil after a 1-year aging period, which could reflect changes of PAH bioavailability during bioremediation.

Materials and methods

Based on the percentage of different molecular weights in a field investigation, high-level contaminated soil (HCS) and low-level contaminated soil (LCS) were prepared by adding phenanthrene (PHE), pyrene (PYR) and benzo(a)pyrene (BaP) to uncontaminated meadow brown soil. The concentrations of HCS and LCS were 250 mg?kg?1 (PHE, PYR, and BaP: 100, 100, and 50 mg?kg?1) and 50 mg?kg?1 (PHE, PYR, and BaP: 20, 20, and 10 mg?kg?1) respectively. The soils were aged for 1 year, after which desorption was induced by means of a XAD-2 adsorption technique over a 96-h period.

Results and discussion

The range of the rapidly desorbing fraction (F rap) for PHE, PYR, and BaP in HCS and LCS was from 1.9 to 27.8 %. In HCS, desorption of PYR was most difficult, and the rate constant of very slow desorption (K vs) of PYR was 8 orders of magnitude lower than that of BaP, which had similar very slow desorbing fractions (49.8 and 50.5 %, respectively). However, in LCS, desorption of PYR was the easiest; the Kvs of PYR was 8–10 orders of magnitude higher than those of PHE and BaP. In HCS, the time scale for release of 50 % of the PAHs was ranked as BaP?>?PYR?>?PHE, while in LCS this was BaP?>?PHE?>?PYR.

Conclusions

The combined effect of PAH concentrations and properties should be taken into account during desorption. The desorption of PAH did not always decrease with increasing molecular weight, and the desorption of four-ring PAHs might be special. These results are useful for screening biodegrading microbes and determining when they should be added to soils based on the dominant contaminants present during different periods, thus improving the efficiency of soil bioremediation.  相似文献   

8.

Purpose

Interestingly, soil is the component of the natural environment in which most hydrophobic organic pollution including polycyclic aromatic hydrocarbons (PAHs) gets accumulated. The aim of the present paper was to determine the effect of soil pollution with PAHs on the elemental composition, spectral properties, and hydrophobic and hydrophilic properties of humic acids. The research was performed on different types of soil samples that were artificially polluted with selected PAHs (anthracene, pyrene, fluorene and chrysene).

Materials and methods

The soil samples were polluted with selected PAHs in an amount corresponding to 10 mg PAHs kg?1. The PAHs-polluted soil samples were incubated for 180 and 360 days at a temperature of 20–25 °C and fixed moisture (50 % of field water capacity). Humic acids (HAs) were extracted from the soil samples prior to the incubation (additionally, soils not polluted with PAHs) and after 180 and 360 days of incubation. For isolated HAs, the following analyses were performed: elemental composition, UV–Vis and IR spectra, susceptibility to oxidation, and hydrophilic (HIL) and hydrophobic (HOB) properties were determined using high-performance liquid chromatography.

Results and discussion

The research demonstrated that introducing anthracene, fluorene, pyrene and chrysene to soil samples resulted in a change in some of the quality parameters of humic acids. However, the intensity and the direction of those changes were determined by soil properties. The changes of the parameters, once PAHs were introduced, that did not depend on the soil properties were ΔA 665u and ΔA 465u (susceptibility to oxidation at wavelengths of 465 and 665 nm) as well as HIL/ΣHOB. The same tendency in changes in the structure of humic acids, once PAHs were introduced, was also observed based on the Fourier transform infrared spectra pattern.

Conclusions

A single pollution of soils with PAHs that leads to changes in the quality parameters of humic acids shows that, as for the soils permanently exposed to pollution with those compounds, significant changes can occur in the properties of humic acids. As a result, it can lead to a change in the functions played by humic acids in the environment.  相似文献   

9.

Purpose

Polycyclic aromatic hydrocarbons (PAHs) are a class of organic compounds commonly found as soil contaminants. Fungal degradation is considered as an environmentally friendly and cost-effective approach to remove PAHs from soil. Acenaphthylene (Ace) and Benzo[a]anthracene (BaA) are two PAHs that can coexist in soils; however, the influence of the presence of each other on their biodegradation has not been studied. The biodegradation of Ace and BaA, alone and in mixtures, by the white rot fungus Pleurotus ostreatus was studied in a sandy soil.

Materials and methods

Experimental microcosms containing soil spiked with different concentrations of Ace and BaA were inoculated with P. ostreatus. Initial (t 0) and final (after 15 days of incubation) soil concentrations of Ace and BaA were determined after extraction of the PAHs.

Results and discussion

P. ostreatus was able to degrade 57.7% of the Ace in soil spiked at 30 mg kg?1 dry soil and 65.8% of Ace in soil spiked at 60 mg kg?1 dry soil. The degradation efficiency of BaA by P. ostreatus was 86.7 and 77.4% in soil spiked with Ace at 30 and 60 mg kg?1 dry soil, respectively. After 15 days of incubation, there were no significant differences in Ace concentration between soil spiked with Ace and soil spiked with Ace + BaA, irrespective of the initial soil concentration of both PAHs. There were also no differences in BaA concentration between soil spiked with BaA and soil spiked with BaA + Ace.

Conclusions

The results indicate that the fungal degradation of Ace and BaA was not influenced by the presence of each other’s PAH in sandy soil. Bioremediation of soils contaminated with Ace and BaA using P. ostreatus is a promising approach to eliminate these PAHs from the environment.  相似文献   

10.

Purpose

Obtaining a better understanding of the concentrations and origins of polycyclic aromatic hydrocarbons (PAHs) in the sediments Taihu Lake, China, is of paramount importance for the environmental protection and remediation of this lake. To investigate temporal and spatial variations in PAH concentrations, composition and possible source categories, 29 sediment samples were collected from Taihu Lake during both the flooding and dry seasons of the lake.

Materials and methods

Fifteen US Environmental Protection Agency priority PAHs were detected in 58 surface sediments (29 for each season) by gas chromatograph/mass selective detection, following extraction by accelerated solvent extraction.

Results and discussion

The concentrations of the total and individual PAHs in the flooding season were higher than those in the dry season, suggesting that high levels of fishing activity may be an important contributor to PAH pollution in the flooding season. The fractions of high molecular weight PAHs in the flooding season ranged from 63?% to 71?% and were higher than those in the dry season (which ranged from 52?% to 65?%). These results indicate that vehicle exhaust may be a more important pollutant source in the flooding season than in the dry season. Diagnostic ratios, principal component analysis and hierarchical cluster analysis were used to study possible source categories in the different seasons. Consistent results were obtained for all techniques. Seasonal and spatial variations were also investigated by the coefficient of divergence method. The results of previous studies support the conclusion of source identification.

Conclusions

Vehicle emissions were the dominant contributor to PAHs in the flooding season, while PAHs in the dry season sediments may have come from multiple sources. The findings of this study may provide a theoretical basis for seasonal PAH control strategies for Taihu Lake.  相似文献   

11.

Purpose

Thaumarchaeota is an ecologically relevant archaeal phylum which may significantly contribute to global nitrogen cycling. Thaumarchaeotal abundance, composition, and activity can be changed by soil pH and pollutants such as toxic metals. This study aims to examine the responses of thaumarchaeotal community to soil pH variation and polycyclic aromatic hydrocarbon (PAH) pollution which may co-occur in agricultural soils.

Materials and methods

Field soil samples were collected from agricultural land impacted by both acidification and PAH contamination. Thaumarchaeotal abundance and composition were assessed using molecular approaches targeting 16S rRNA or amoA genes and were linked to environmental factors by correlation and canonical correspondence analysis (CCA). To evaluate the short-term responses of Thaumarchaeota to PAHs, additional soil microcosms amended with either three selected PAHs were established. Changes in thaumarchaeotal communities during the incubation were monitored.

Results and discussion

A significant correlation between thaumarchaeotal gene abundance and soil pH was observed within field samples, with the I.1a-associated group enriched when pH <5.0. CCA suggests that the community variation was primarily related to soil pH. In contrast, the effects of PAHs were minimal. In soil microcosms, high concentrations of PAHs persisted after the 4-week incubation. Independent of the PAHs added, thaumarchaeotal amoA abundance slightly increased and the compositions were stable at the end of the incubation. This might be associated with the pollutants bioavailability and potential microbe-PAH interactions in the soil.

Conclusions

Soil pH variation strongly shapes the agricultural soil thaumarchaeotal community, whereas PAH effects appear to be marginal even in the presence of high concentrations of pollutants. The complicated interaction between soil matrix, pollutants, and Thaumarchaeota requires further study.
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12.

Purpose

Enhancing desorption of hydrophobic organic contaminants from soils is a promising approach for the effective remediation of soils contaminated with organic compounds. The desorption efficiency of chemical reagent, such as surfactant, should be evaluated. In this study, the effect of mixed anionic–nonionic surfactants sodium dodecylbenzene sulfonate (SDBS)–Tween 80 on the distribution of polycyclic aromatic hydrocarbons in soil–water system was evaluated.

Materials and methods

Batch desorption experiments were employed to evaluate the distribution of polycyclic aromatic hydrocarbons (PAHs) and surfactants in soil–water system. PAHs and SDBS were determined by high-performance liquid chromatography, Tween 80 by spectrophotometry, and total organic carbon with a carbon analyzer.

Results and discussion

Sorption of PAHs to soil was increased at low surfactant concentration due to the effective partition phase on soil formed by sorbed surfactants. The mixture of anionic and nonionic surfactants decreased the sorption of surfactants to soil, increasing the effective surfactant concentration in solution and thus decreasing the sorption of PAHs on soil. Anionic–nonionic mixed surfactant showed better performance on desorption of PAHs from soil than single surfactant. The greatest desorption efficiency was achieved with low proportions of SDBS (SDBS/Tween80?=?1:9).

Conclusions

SDBS–Tween 80 mixed surfactant showed the highest desorption rate with low proportion of SDBS, which indicated that the addition of relative low amount of anionic surfactant could significantly promote the desorption efficiency of PAHs by nonionic surfactants. Results obtained from this study did provide useful information in surfactant-enhanced remediation of soil and subsurface contaminated by hydrophobic organic compounds.  相似文献   

13.

Purpose

This study addresses the feasibility of a flotation technique, using a lab-scale flotation cell, to simultaneously remove both metals and polyaromatic hydrocarbons (PAHs) from fine sediment fractions (<250 μm) that are potentially contaminated with copper (Cu).

Materials and methods

A multiple flotation process with three consecutive flotation stages was performed on three sediments (13S, 14B, and 24A) with different particle size distributions, Cu and PAH concentrations, and organic matter contents.

Results and discussion

Flotations performed under selected conditions allowed for significant removal of both Cu (61–70 %) and PAHs (75–83 %) with acceptable froth recoveries of approximately 23–29 %. Removal rates for arsenic, lead, and zinc were 48–61, 40–48, and 32–36 %, respectively. Flotation selectivity of Cu was greatly influenced by the contents of fine particles and organic matter of the sediments. The maximum flotation selectivity was obtained for the 53–125-μm size fraction. The high flotation selectivity of Cu (2.5–3.2) and PAHs (3.0–3.6) demonstrated the feasibility of flotation to treat soils or sediments containing both organic and inorganic pollutants.

Conclusions

Overall, the flotation results showed a high selectivity for both Cu and PAHs and demonstrated the feasibility of flotation to treat media contaminated with organic and inorganic contaminants.  相似文献   

14.

Purpose

Understanding the fate and behavior of polycyclic aromatic hydrocarbon (PAH) sources in aquatic systems is important for the efficiency of control policies. In this work, a new approach??organic carbon-normalized sediment?Cpore water partition coefficients of PAH source contributions (logK??Osource)??was developed to study the sediment?Cpore water partition of PAH source contributions. The focus of this study was the Yellow River, which is the second largest river in China and one of the largest rivers in the world.

Materials and methods

Sixteen priority US Environmental Protection Agency PAHs were analyzed in 14 surface sediments and 11 pore water samples. Principal component analysis?Cmultiple linear regression (PCA-MLR) and Unmix models were employed to estimate the source contributions of PAHs in sediments and pore water samples. Finally, logK??Osource values were calculated according to the modeled source contributions of PAHs.

Results and discussion

??PAHs (sum of the 16 PAH concentrations) in 14 sediment samples and 11 pore water samples from the Yellow River were 1,415?±?726?ng?g?1 dry weight (dw) and 123?±?57.4???g?l?1, respectively. The source apportionment results indicate the following: (1) for sediment samples, the contributions to ??PAHs from vehicular emissions, coal combustion, and petrogenic sources were 41.07?C61.05, 38.83?C45.56, and 11.18?C14.92?%, respectively, and (2) for pore water samples, vehicular emissions were the most significant contributor (45.51?C69.39?%), followed by petrogenic sources (29.80?C34.22?%) and coal combustion (7.35?C21.59?%). Coal combustion had the highest logK??Osource values (4.15?C4.26) among the three categories, followed by vehicular emissions (3.51?C3.57) and petrogenic sources (3.30?C3.43).

Conclusions

The possible categories of PAH sources identified by hierarchical cluster analysis, PCA-MLR, and Unmix models were consistent, indicating that vehicular emissions, coal combustion, and petrogenic sources were three important categories. The logK??Osource values indicate that contributions from coal combustion had a higher partition for the sediment phase compared with the other two source categories.  相似文献   

15.

Purpose

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous and persistent contaminants in aquatic bed sediments. A better understanding of their in-bed fate and transport is therefore key in minimising the risk to the environment over time through various remediation and monitoring strategies. Since ecological effects and risks are related to contaminant concentrations, this study developed CoReTranS, a predictive model that simulates one-dimensional organic contaminant reaction and transport in bed sediments.

Materials and methods

CoReTranS was benchmarked against analytical solutions of simplified reactive transport models and validated using a published study of marsh sediments contaminated with petroleum-derived hydrocarbons from Wild Harbour, West Falmouth, MA, USA.

Results and discussion

The CoReTranS model effectively predicted the vertical distribution of PAHs in the Wild Harbour sediments as confirmed by the modelling results from the published study. The CoReTranS model was also used to interpret results from a published study of PAH-contaminated fjord sediments from Kitimat Arm in British Columbia, Canada. Specific insights into the post-depositional fate and transport of selected PAHs in the Kitimat fjord sediments were obtained by comparing the measured concentration-depth profiles with the numerical results from the CoReTranS model. Key parameters such as effective diffusivity of contaminants and burial velocities of sediment particles were shown to possibly account for the predicted concentrations-depth profiles in the Kitimat fjord sediments.

Conclusions

As demonstrated, CoReTranS can simulate reactive transport models in order to predict PAH concentration profiles in porewater under site-specific conditions. The information derived from the use of the CoReTranS model highlighted practical application of such information by engineers to site-specific risk assessment and remediation.  相似文献   

16.

Purpose

Combined pollution by polycyclic aromatic hydrocarbons (PAHs) and heavy metals are commonly found in industrial soils. This study aims to investigate the effect of the coexistence of heavy metals on the sorption of PAHs to soils. We focused specifically on the relationship of the sorption capacity with the estimation of the binding energy between PAHs and heavy metals.

Materials and methods

The sorption of typical PAHs (naphthalene, phenanthrene, and pyrene) to soils coexisting with heavy metals (Cu(II), Pb(II), and Cr(III)) was characterized in batch sorption experiments. The binding energy between PAHs and heavy metals in aqueous solution was estimated by quantum mechanical (QM) method using density functional theory (DFT) at the M06-2x/def2svp level of theory.

Results and discussion

Sorption capacity and nonlinearity of the PAHs to the soils were enhanced by the coexisting heavy metals. The extent of increment was positively associated with the hydrophobicity of the PAHs and the electronegativity and radius of the metal cations: Cr(III)?>?Pb(II)?>?Cu(II). The cation-π interaction was revealed as an important noncovalent binding force. There was a high correlation between the binding energies of the PAHs and K f (K f adjusted after normalizing the equilibrium concentration (C e) by the aqueous solubility (C s)) (R 2?>?0.906), indicating the significant role of the cation-π interactions to the improved PAH sorption to soils.

Conclusions

In the presence of heavy metals, the sorption capacities of naphthalene, phenanthrene, and pyrene to soils were enhanced by 21.1–107 %. The improved sorption capacity was largely contributed from the potent interactions between PAHs and heavy metals.
  相似文献   

17.

Purpose

Heavy metals often occur as co-contaminants with polycyclic aromatic hydrocarbons (PAHs) and reportedly have adverse effects on biodegradation. In this study, the development of 14C-phenanthrene mineralisation in soil co-contaminated with aged or freshly added Al or Fe amendment was assessed.

Materials and methods

14C-phenanthrene mineralisation was assessed using respirometry; respirometers incorporated a Teflon-lined screw-capped CO2 trap containing 1-M NaOH within a glass scintillation vial. The production of 14CO2 was assessed by the addition of Ultima Gold liquid scintillation fluid to the CO2 traps and subsequent liquid scintillation counting. Enumeration of phenanthrene-degrading bacteria was achieved by counting the colony forming unit count using the spread plate method.

Results and discussion

This investigation considered the effects of Al and Fe (50, 100, 250 and 500 mg/kg) on 14C-phenanthrene biodegradation in soil over 63-day contact time. Fresh Al amendments at lower concentrations (50 and 100 mg/kg) stimulated phenanthrene catabolism (p <0.05) at t?=?21 and 42 days which may reflect an ‘Arndt–Schulz’ effect, but phenanthrene catabolism was significantly reduced (p <0.05) in 500 mg/kg aged Al this could be due to Al toxicity to phenanthrene degraders. Phenanthrene mineralisation was stimulated in the highest Fe concentration (500 mg/kg) in aged and fresh Fe amendments at t?=?21 days. This could be because Fe is an essential requirement for microbial growth.

Conclusions

The impact of Al or Fe on the catabolism of 14C-phenanthrene was dependent on incubation time and Al was more toxic than Fe to soil PAH catabolic activity. This could be because Al is a non-essential microbial requirement. Bioremediation of soils co-contaminated with PAH and heavy metal is a complex problem; therefore, studies on the impact of metals on PAHs biodegradation highlight the risks and biodegradation potential in contaminated soil.  相似文献   

18.
Purpose

The purpose of this study is to study the major sources, concentrations, and distributions of polycyclic aromatic hydrocarbons (PAHs) in three different types of green space in Shanghai. In addition, we will quantitatively assess the burden of PAHs in the soil, as well as the potential carcinogenic risk of PAHs in humans. These results will provide valuable information for soil remediation and human health risk management.

Materials and methods

A total of 166 surface soil samples were collected in parks, greenbelts, and woodlands. Soils were extracted using accelerated solvent extraction (ASE). PAHs were analyzed by gas chromatography-mass spectrometry (GC-MS). The positive matrix factorization (PMF) model was used to identify major PAH emission sources and quantitatively assess their contributions to PAHs. The incremental lifetime cancer risk (ILCR) was used to quantify the potential health risk of PAHs.

Results and discussion

The average concentrations of ∑15 PAHs are 227?±?95 ng g?1, 1632?±?251 ng g?1, and 1888?±?552 ng g?1 in the woodland, park, and greenbelt soils, respectively. The PMF results show that biomass (33%), coal (21%), vehicles (17%), natural gas (14%), oil (9%), and coke (7%) are the dominant sources of PAHs in the park soils. Diesel (40%), tire debris (30%), biomass (15%), gasoline (9%), and oil (5%) are the main sources in the greenbelt soils. Biomass (48%), vehicles (37%), and coal (15%) are the main sources in the woodland soils. The ILCRs of adults and children who are exposed to PAHs in soils range from 9.53?×?10?8~1.42?×?10?5.

Conclusion

In three types of green space in Shanghai, the dominant PAHs are high–molecular weight (HMW) compounds (≥?4 rings). This may be due to the proximity of the sampling site to emission sources. In addition, low–molecular weight (LMW) PAHs (with 2–3 rings) are relatively unstable, and these compounds are prone to volatilization and degradation. Source identification indicates that biomass combustion is the most dominant PAH source in the park and woodland soils, while vehicles are the dominant PAH source in the greenbelt soils. The ILCRs of adults and children indicate potential health risks, and children have a greater health risk than adults.

  相似文献   

19.

Purpose

During the late 1950s and early 1960s, industrial waste material highly enriched with various contaminants (e.g., heavy metals, polycyclic aromatic hydrocarbons (PAHs)) was dumped in the inner Bay of Mecklenburg, western Baltic Sea. Between 2002 and 2004, a research program was initiated using chemical analysis in combination with bioanalytical techniques to assess the extent and variability in contamination at this dump site (DS). The data were compared to a reference area (RS) with similar environmental conditions, which is representative of the western Baltic Sea.

Materials and methods

Twelve PAHs were investigated to assess their ecological hazard, as they were identified as major pollutants in the dumped material. In addition to analyzing the actual PAH contamination status in the sediments, PAHs measured in the soft tissue of Arctica islandica were also used as an indicator of contaminant bioaccumulation. A biotest battery was applied to determine the toxic effects of contaminants in the sediment.

Results and discussion

Significantly elevated PAH concentrations (sum of 12 PAHs) of ~3,000 ng g?1 dw and higher bioaccumulation factors (BAFs) were determined in the soft body tissue of A. islandica collected at DS (t test, p?=?0.025). The results also showed that the sediment PAH contamination was significantly higher at DS (1,952–5,466 ng g?1 dw) than at RS (1,384–2,315 ng g?1 dw). The results revealed a major heterogeneity in the PAH concentration at DS due to an attempt to cover the toxic material with clean clay. This resulted in a more heterogeneous distribution of the dump material rather than covering it up completely. However, not all relevant contaminants were included in this study, not only because it is too costly to determine them all but also because unidentified contaminants present at concentrations below the limit of detection cannot be measured. Bioassays were used to fill this gap in the hazard assessment in a cost-effective way by investigating the possible effects of sediment contamination on benthic organisms. The results showed a high variability and magnitude of growth and luminescence inhibition. Bacterial contact tests with marine organisms showed a high toxicity response (>80 % inhibition) from DS sediments. In contrast, the luminescent bacteria test (Vibrio fischeri) showed equivalent effects of sediments from both DS and RS.

Conclusions

The spatial distribution of toxicity in DS, the bioaccumulation in mussels and the analytical evidence of PAH pollution clearly show that the dumped material still represents a potential risk even after 60 years.  相似文献   

20.

Purpose

The emerging recycling of electronic and electric waste (e-waste) is causing critical levels of soil pollution in those relatively poor towns surrounding the central cities, which have been involved in recycling activities for quite some time. Agricultural soil is of great importance due to its direct impact on food and human health. The objective of this study was to provide a systematic investigation of the contamination in agricultural soil for a range of inorganic compounds (Cr, Cd, Pb, Zn, Cu, and Ni) and organic compounds (PAHs and PCBs) in town A, an emerging e-waste recycling town in China.

Materials and methods

A total of 20 agricultural soil samples were collected from three sampling locations throughout town A. Levels of inorganic compounds (Cr, Cd, Pb, Zn, Cu, and Ni) and organic compounds (PAHs and PCBs) were determined by AAS, GC/MS, and GC/electron capture detector, respectively. Data was processed with SPSS 13 and Arcview 3.3 GIS software.

Results and discussion

The findings demonstrate that agricultural soil was contaminated to various extents by inorganic and/or organic pollutants. Comparison among the three sampling areas indicated that the soil was highly contaminated in the agricultural area near e-waste recycling workshops. Moreover, the contaminants (Cu, Pb, PAHs, and PCBs) may be connected through a common source as found in the Pearson correlations and cluster analysis.

Conclusions

There exists a heightened sense of awareness concerning the hazardous implications of current emerging e-waste recycling issues in the agricultural soil of those areas close to the central city in Taizhou.  相似文献   

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