Characteristics,sources, and in situ phytoremediation of polycyclic aromatic hydrocarbon in rural dumpsites

Purpose

Without precaution to deal with gas emissions and leachate generation, dumpsites have become a severe environmental problem in many developing countries. The objectives of this study were to investigate the pollution status of polycyclic aromatic hydrocarbons (PAHs) in dumpsite soil in rural areas of China and to verify phytoremediation effectiveness with Sedum alfredii Hance and alfalfa (Medicago sativa L.) under complex pollution conditions in PAH-contaminated soil.

Materials and methods

In this study, we collected soil cores from four dumpsites in rural areas of North China (Hebei Province) for analysis, and correspondingly conducted an in situ phytoremediation experiment using Sedum alfredii Hance and alfalfa (Medicago sativa L.) at one of these sites, monitoring the total PAH concentration in soil.

Results and discussion

Results showed generally moderate pollution by PAHs in soil samples from dumpsites with pockets of heavy pollution. PAH concentrations in dumpsite soil ranged from 827 to 1101 ng/g (dry weight). High-molecular-weight PAHs were present in higher proportions at oldest dumpsite in operation. Certain molecular ratios of PAHs can be used to diagnose the source of PAHs in soil, and it indicated that the main sources were combustion of domestic coal and biomass, as well as the automobile exhaust and kitchen exhaust. A 17-month in situ phytoremediation experiment resulted in the effective removal of PAHs in the Sedum alfredii and alfalfa plots, with total PAH concentrations decreasing by 82.4% and 81.3%, respectively. Furthermore, PAH concentrations in plants correlated to plant growth conditions.

Conclusions

This study indicated that the soils of the dumpsites were generally moderately polluted by PAHs, and some parts of the area were heavily polluted. Both Sedum alfredii and alfalfa absorbed PAHs from soil, and PAH concentrations in these two plants correlated to the growth conditions of the plants. Phytoremediation can effectively be used for PAH removal in open dumpsites.

     

1-Hydroxypyrene in milk and urine as a bioindicator of polycyclic aromatic hydrocarbon exposure of ruminants

Urinary 1-hydroxypyrene (1-OH-pyrene) is now largely considered to be a valuable biomarker of exposure of man and animals to pyrene and other polycyclic aromatic hydrocarbons (PAHs). However, from a practical and agronomic standpoint, the question remains whether such biomarking capability still holds when 1-OH-pyrene is analyzed in milk produced by ruminants. To assess this hypothesis, four goats were daily submitted to three different amounts of pyrene oral ingestion, together with phenanthrene and benzo(a)pyrene (1, 7, and 49 mg/day during 1 week each). An HPLC-fluorometric analysis of 1-OH-pyrene in milk revealed a perfect correlation between pyrene doses and 1-OH-pyrene detected in milk, thus fully confirming the biomarking capability of 1-OH-pyrene and providing information on its transfer coefficient toward milk. Transfer equations such as the ones found in the present study could be used as a valuable and practical risk assessment tool in (i) the accurate monitoring of exposure of ruminants to pyrene and (ii) the evaluation of occupational and environmental exposure of ruminants to PAH mixtures.     

柴油机多环芳香烃类污染物的测量方法

采用聚四氟乙烯滤膜及XAD-2吸附管采集、超声和索氏提取、气-质联用（GC/MS）分析等方法对柴油机排气中多环芳香烃类污染物进行了定性、定量分析。结果表明,在试验浓度范围内,多环芳香烃（PAHs）各组分的浓度与峰面积的线性关系良好,线性相关系数在0.99以上。线性范围较宽,为0.0125～80 μg/mL。该方法样品采集效率较高,样品提取效率均在95%以上。方法重复性较好,相对标准偏差低于15%,滤膜样品的回收率为70.1%～95.9%,吸附剂样品的回收率为77.0%～102.6%。灵敏度高,检出限在0.04 μg/m3以下。该方法适用于柴油机排气中PAHs含量的快速分析。     

Enchytraeid worms retard polycyclic aromatic hydrocarbon degradation in a coniferous forest soil

In this study the fate of naphthalene, fluorene and pyrene were investigated in the presence and absence of enchytraeid worms. Microcosms were used, which enabled the full fate of ¹⁴C-labelled PAHs to be followed. Between 60 and 70% of naphthalene was either mineralised or volatilised, whereas over 90% of the fluorene and pyrene was retained within the soil. Mineralisation and volatilisation of naphthalene was lower in the presence of enchytraeid worms. The hypothesis that microbial mineralisation of naphthalene was limited by enchytraeids because they reduce nutrient availability, and hence limit microbial carbon turnover in these nutrient poor soils, was tested. Ammonia concentrations increased and phosphorus concentrations decreased in all microcosms over the 56 d experimental period. The soil nutrient chemistry was only altered slightly by enchytraeid worms, and did not appear to be the cause of retardation of naphthalene mineralisation. The results suggest that microbial availability and volatilisation of naphthalene is altered as it passes through enchytraeid worms due to organic material encapsulation.     

Anthropogenic trace elements and polycyclic aromatic hydrocarbon levels in sediment cores from two lakes in the Adirondack acid lake region

Sediment cores were taken from the remote Sagamore and Woods Lakes in New York State's Adirondack acid lake region and analyzed for 3 to 7 ring polycyclic aromatic hydrocarbons (PAHs) and Ag, Al, As, Be, Cd, Cr, Cu, Hg, Ni, Ph, Se, Sn, TI, V, and Zn. With the exception of perylene, all of the parental PAHs, e.g. those without sidechains, and several of the metals, Pb, As, and Cd, were found to be significantly increased in the sediments of both lakes compared to their natural integrated deposits (ng cm^?2) and their background concentrations (μg g^?1 or ng g^?1 dry wt). Although the concentrations were generally much higher in Woods Lake, the total anthropogenic integrated depositions were about the same in both lakes for most of the metals and the 3 to 4 ring PAHs. The prime source of most of the 3 to 7 ring PAHs and trace elements measured is ascribed to anthropogenic combustion. Anthropogenically derived materials decreased in concentration with depth to baseline levels in sediment layers estimated by¹³⁷Cs analyses to be ～30 yr old, while biogenic or crustal derived species remained constant or fluctuated with core depth.     

Effects of pH and polycyclic aromatic hydrocarbon pollution on thaumarchaeotal community in agricultural soils

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.

     

拟南芥对多环芳烃菲胁迫的早期响应

选用模式植物拟南芥及3环的多环芳烃菲为材料, 研究了抗氧化酶和膜保护系统的早期响应及胁迫下相关基因mRNA的差异表达, 结果表明: 菲胁迫12 h时, 拟南芥叶片超氧化物歧化酶(SOD)及过氧化物酶(POD)活性明显高于对照, 清除超氧阴离子自由基()及过量H2O2的机制已启动.胁迫72 h时H2O2含量出现累积现象, 但膜系统仍未受到膜脂过氧化作用的明显伤害.随着胁迫时间的延长, 拟南芥的光合作用无论在mRNA水平还是细胞水平都受到影响.本研究揭示了氧化胁迫响应是植物对多环芳烃胁迫的重要早期应激反应.     

Simulation of polycyclic aromatic hydrocarbon remobilization in typical active regions of river system under hydrodynamic conditions

Purpose  

In an aquatic environment, hydrodynamic condition is a ubiquitous natural process, and the contaminated sediments will act as a potential pollution source once they are remobilized into the overlying water. In this study, remobilization behavior of polycyclic aromatic hydrocarbons (PAHs) under simulated hydrodynamic conditions was studied. Additionally, an adjusted prediction model with addictive consideration of surface properties was developed to exhibit the distribution of PAHs in hydrodynamic system.     

湛江市区不同利用类型土壤的PAHs污染特征和来源

首次对湛江市表层土壤PAHs污染进行研究,并根据利用类型对其进行分类讨论。虽然湛江市的环境质量在全国名列前茅,但研究显示随着重化工业的快速发展,湛江市土壤已受到一定程度的PAHs污染,∑PAHs的平均含量达491.1ng.g-1,低于珠三角的发达城市,而高于中等城市,特别是某些工业区污染严重,超过荷兰相关标准;与其它城市一样,湛江市土壤PAHs的组分构成以4环和5环为主,占∑PAHs的65.1%。∑PAHs的变化趋势为旧厂址>市区工业区>交通>郊区工业区>休闲>农业,市区>郊区;3环组分比重随市中心距离的增大而增加,4环和5环则相反,6环差异较小。农业和郊区工业高比重的3环组分可能与市区石油源PAHs的大气输送有关。已搬迁工厂高含量∑PAHs表明PAHs在土壤的积累影响是长期的,而休闲区178.7 ng.g-1的∑PAHs则表明解决PAHs的污染问题必须解决污染源问题。利用4种PAHs比值判断湛江市土壤PAHs的来源主要是石油源、石化燃烧和煤、柴等生物燃烧源的混合源,与湛江市社会经济情况相符。     

Molecular comparison of cultivable protozoa from a pristine and a polycyclic aromatic hydrocarbon polluted site

We compared the abundance and diversity of cultivable protozoa (flagellates and amoebae) in a polycyclic aromatic hydrocarbon (PAH) polluted soil and an unpolluted control, by isolating and cultivating clonal strains. The number of cultivable protozoa was higher in the polluted soil; however, the polluted soil displayed an impoverished community, dominated by certain taxa, such as Acanthamoeba sp. We isolated a total of 31 protozoan strains to characterize them morphologically and by 18S rRNA gene sequence analysis. This approach, i.e. combining morphological and molecular information had the advantage of providing quantitative data, information on morphology but also an accurate positioning of the isolates in 18S rRNA trees.     

Polycyclic aromatic hydrocarbons in spanish olive oils: relationship between benzo(a)pyrene and total polycyclic aromatic hydrocarbon content

Samples of Spanish virgin olive oils (VOOs) from different categories, origins, varieties, and commercial brands were analyzed by HPLC with a programmable fluorescence detector to determine the content of nine heavy polycyclic aromatic hydrocarbons (PAHs): benzo(a)anthracene, chrysene, benzo(e)pyrene, benzo(b)fluoranthene, benzo(k)fluoranthene, benzo(a)pyrene, dibenzo(a,h)anthracene, benzo(g,h,i)perilene, and indeno(1,2,3-c,d)pyrene. Samples of olive pomace and crude olive pomace oils were also investigated. Benzo(a)pyrene concentrations were below the allowed limit in the European Union (2 microg/kg) in 97% of the VOO samples. Only those samples coming from contaminated olive fruits or obtained in oil mills with highly polluted environments exceeded this value. High correlation coefficients (<0.99) were obtained between the contents of benzo(a)pyrene and the sum of the nine PAHs for all of the analyzed categories, suggesting that benzo(a)pyrene could be used as a marker of the content of these nine PAHs in olive oils.     

Effect of roasting conditions on the polycyclic aromatic hydrocarbon content in ground Arabica coffee and coffee brew

Roasting is a critical process in coffee production as it enables the development of flavor and aroma. At the same time, roasting may lead to the formation of nondesirable compounds, such as polycyclic aromatic hydrocarbons (PAHs). In this study, Arabica green coffee beans from Cuba were roasted under controlled conditions to monitor PAH formation during the roasting process. Roasting was performed in a pilot spouted bed roaster, with the inlet air temperature varying from 180 to 260 degrees C, using both dark (20 min) and light (5 min) roasting conditions. Several PAHs were determined in both roasted coffee samples and green coffee samples. Also, coffee brews, obtained using an electric coffee maker, were analyzed for final estimation of PAH transfer coefficients to the infusion. Formation of phenanthrene, anthracene, and benzo[a]anthracene in coffee beans was observed at temperatures above 220 degrees C, whereas formation of pyrene and chrysene required 260 degrees C. Low levels of benzo[g,h,i]perylene were also noted for dark roasting under 260 degrees C, with simultaneous partial degradation of three-cycle PAHs, suggesting that transformation of low molecular PAHs to high molecular PAHs occurs as the roasting degree is increased. The PAH transfer to the infusion was quite moderate (<35%), with a slightly lower extractability for dark-roasted coffee as compared to light-roasted coffee.     

The correlation between in-situ,real-time aerosol photoemission intensity and particulate polycyclic aromatic hydrocarbon concentration in combustion aerosols

Aerosol photoemission (APE) has been found to be an excellent surrogate measure of particulate PAH concentration in combustion aerosols under a variety of laboratory and field conditions. Samples of oil stove, automobile exhaust, and urban air particulate matter were concurrently analyzed for aerosol photoemission intensity and particulate PAH concentration. In-situ, real-time analysis of the particulate matter was performed by UV-induced electron photoemission. Two photon energies, 4.9 and 6.7 eV, were chosen for irradiation. The latter energy was more sensitive and less selective. Particulate PAH concentrations were determined by collecting the particulate matter on a filter, solvent extracting the filter, and analyses of the extracts by gas chromatography / mass spectroscopy. Linear correlations (0.84≤r²≤1.00) were observed between aerosol photoemission intensities and the sum of particulate PAH concentrations for laboratory and field studies under a wide variety of conditions. The studies performed to date cover a dynamic range of three orders of magnitude (1 to 1000 ng / m³). The time resolution is in the order of a few seconds.     

Assessment of polycyclic aromatic hydrocarbon content of smoked fish by means of a fast HPLC/HPLC method

Polycyclic aromatic hydrocarbon (PAH) concentrations in smoked food can reach levels hazardous for the human health, especially when the smoking procedure is carried out under uncontrolled conditions. In this work a simple and rapid method for the determination of PAHs in smoked fish samples is described. PAHs were extracted from the insoluble samples (together with fat substances) by homogenization with acidified chloroform. The fat extract was then submitted to a first LC sample preparation step (performed on a large silica column) to isolate PAHs from triglycerides. After reconcentration, the PAH fraction was finally injected into the reverse-phase analytical column. The proposed method, which presents good characteristics of recoveries and repeatability, was also used to analyze PAH content of some smoked trout samples packed under vacuum.     

Composition,distribution and sources of polycyclic aromatic hydrocarbons in sediments of the western harbour of alexandria,egypt

Aim and Background  Little data are available on the levels of polycyclic aromatic hydrocarbons (PAHs) in the sediments of the Mediterranean Sea Coast of Egypt in general and the Alexandria coastal zone in particular. It was therefore deemed necessary to set up a monitoring programme to determine the current concentrations of PAHs in bottom sediments, and to identify any area where high concentrations of these potential hazardous contaminants were present in the Western Harbour of Alexandria. Methods  The composition, distribution and the source of PAHs in surficial sediments of the harbour were investigated. To document the spatial PAH input, surficial sediment samples from 23 locations throughout the harbour were analysed. as]Results and Discussion The total PAH load determined in the surficial sediment samples ranged from 8 to 131150 ng g¹ dry wt, generally with most of the samples having total concentrations of PAHs greater than 5000 ng g¹ dry weight. The highest concentration of total PAHs was recorded in sediments of the inner harbour. Ratio values of specific compounds such as phenanthrene to anthracene, fluoranthrene to pyrene, methyl-phen-anthrene to phenanthrene, methyl-dibenzothiophenes to dibenzothiophenes, alkylated to non-alkylated and high molecular weight to low molecular weight PAH, were calculated to evaluate the possible source of PAH contamination in the harbour sediments. Conclusions  Two main sources of PAH in the study area have been found: pyrolytic and petrogenic. Interferences of rather petrogenic and pyrolytic PAH contaminations were noticed for most samples. The dominant sources of PAH appear to be the combustion processes through run-off, industrial and sewage discharges, and atmospheric input. The concentrations of PAHs were generally above levels expected to cause adverse biological effects. Recommendations and outlook  Information from this study and any other relevant studies should be useful in designing future strategies for environmental protection and management of the harbour.     

Availability of polycyclic aromatic hydrocarbons in aging soils

Purpose  

The soil contamination by hydrophobic organic contaminants (HOCs), such as polycyclic aromatic hydrocarbons (PAHs), poses great threats to human health and ecological security and attracts worldwide concerns. The total HOC concentrations overestimate its available fraction to the soil biota. Increased understanding of the availabilities of PAHs in soil environment will have considerable benefits for their risk assessment and be very instructive to food safety and remediation strategies in contaminated sites. However, the availability of PAHs in aging soils and particularly the correlations of the availabilities with their forms in soils have yet to be elucidated. In this work, the availabilities of PAHs in aging soils were evaluated using a sequential mild extraction technique.     

Effect of exposure to soil-bound polycyclic aromatic hydrocarbons on milk contaminations of parent compounds and their monohydroxylated metabolites

The aim of this study was to determine the transfer kinetics of soil-bound polycyclic aromatic hydrocarbons to milk in lactating cows. Soil (500 g/day) fortified with fluorene (104 microg/g dry soil), phenanthrene (82 microg/g), pyrene (78 microg/g), and benzo[a]pyrene (33 microg/g) was administered to three dairy cows via a rumen cannulas for 28 consecutive days. Parent compounds and their major metabolites in milk were measured using gas chromatography-mass spectrometry. Secretion of parent compounds in milk did not increase significantly (P > 0.05) over the control values measured before supply. Target monohydroxylated metabolites were not detected in control samples, but 2-hydroxy fluorene, 3-hydroxy phenanthrene, and 1-hydroxy pyrene were present in milk by the second day of dosing. The highest concentrations of metabolites in milk (31-39 ng/mL) were for 1-hydroxy pyrene at days 7 and 14 of dosing. The observed plateaus for 3-hydroxy phenanthrene and 2-hydroxy fluorene were lower (respectively, 0.69 and 2.79 ng/mL) but significantly increased in comparison to the control samples. Contrarily, 3-hydroxy benzo[a]pyrene was not detected in milk at any sampling time. These results suggested a notable metabolism of the parent compounds after their extraction from soil during the digestive transfer. Thus, the metabolization of fluorene and pyrene can lead to higher concentrations of metabolites than of parent compounds in milk. Despite the absence of a significant transfer of parent PAHs to milk, the appearance of metabolites raises the questions of their impact on human health.     

Seasonal variations of concentrations, profiles and possible sources of polycyclic aromatic hydrocarbons in sediments from Taihu Lake, China

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.     

Distribution of polycyclic aromatic hydrocarbons in the soil-plant system

The content and composition of the polycyclic aromatic hydrocarbons (PAHs) in the conjugated systems of [arable soil]-[above-ground plant organs] in background (reference) and contaminated regions were studied. The coefficients of the biological uptake of PAHs by plants (K _bPAH) were determined for different PAH concentrations in the soil. Correlations of the PAH accumulation rate in plants with the physicochemical properties of the PAHs—the solubility, hydrophobicity, volatility, and chemical activity (polarizability and ionization potential)—were revealed. The high accuracy, sensitivity, and information value of the standardized parameters K _b were shown (with K _bPAH as an example) for the quantitative study of the accumulation mechanisms of substances by plants compared to the average arithmetic values of their concentrations in the plants.