Risk assessment of polycyclic aromatic hydrocarbons (PAHs) in sediments from a mixed-use reservoir

Although reservoirs in China are of great significance, very few studies on risk assessment have been reported for reservoirs. This study investigated distribution characteristics, cancer and ecological risks, and source diagnosis of 16 priority polycyclic aromatic hydrocarbons (PAHs) in sediments from Shitou Koumen Reservoir in Jilin Province, China. A total of 12 sediment samples were collected from the reservoir in August (wet season) 2014. Total PAH concentrations in sediment samples ranged from 1294.51 ng/g to 2755.35 ng/g with a mean concentration of 1757.54 ng/g. For individual PAHs, average concentration of Nap was the highest, 800.56 ng/g, while Acy, Fla, BkF, and DahA were undetected in sediment samples. Light PAHs (2–3 rings) accounting for 74.21% was a dominant PAH compositional pattern. Pearson correlation analysis was carried out; results showed that total PAHs was strongly correlated with the highly enriched sedimentary PAHs, and pH was a major factor in controlling PAH distribution. Lifetime cancer risk was employed to assess cancer risk; results indicated that the fish-culturing area was exposed to cancer risk. The molecular diagnostic ratios of isomeric PAHs were applied to identify possible PAH sources; primary PAH sources were identified as oil-related activities, burning agricultural wastes, vehicular emissions, and industrial discharges.     

Uncertainty-based dynamic multimedia human health risk assessment for polycyclic aromatic hydrocarbons (PAHs) in a land oil exploitation area

With the increasing development of the petrochemical industry and the growing demand for oil, polycyclic aromatic hydrocarbons (PAHs) pollutions in the environment, especially in petroleum exploitation areas, are caused by the discharge of waste from the petroleum extraction process into an environmental system. This study aims to develop a new health risk assessment approach based on interval dynamic multimedia fugacity (IDMF) model and uncertainty analysis that could analyze the human exposure risk level for PAH contamination. The developed IDM health risk assessment (IDMHRA) approach is applied to assess previous, current, and future risks at a case study site in Daqing, Heilongjiang, China, from 1985 to 2020 for model validation. The human health risk assessment results show that 11 PAHs (NAP, ANT, FLA, PYR, BaA, CHR, BbF, BkF, BaP, IPY, and DBA) in the study site require further remediation efforts in terms of their unacceptable non-carcinogenic and carcinogenic risk. The results of risk source analysis reveal that soil media is the main risk pathway as compared with other exposure pathways. It can be seen that remediation process for soil contamination in the study site is urgently demanded. The assessment results demonstrate that the developed IDMHRA approach provides an effective tool for decision-makers and environmental managers to make remediation decisions in contaminated sites.     

微生物降解多环芳烃(PAHs)的研究进展

从多环芳烃(PAHs)的降解菌株的筛选、降解机制以及PAHs污染的生物修复等方面介绍了微生物降解PAHs的最新研究进展。     

Multispecies and monoculture rhizoremediation of polycyclic aromatic hydrocarbons (PAHs) from the soil

In this study, we investigated the potential of multispecies rhizoremediation and monoculture rhizoremediation in decontaminating polycyclic aromatic hydrocarbon (PAH) contaminated soil Plant-mediated PAH dissipation was evaluated using monoplanted soil microcosms and soil microcosms vegetated with several different grass species (Brachiaria serrata and Eleusine corocana). The dissipation of naphthalene and fluorene was higher in the "multispecies" vegetated soil compared to the monoplanted and nonplanted control soil. The concentration of naphthalene was undetectable in the multispecies vegetated treatment compared to 96% removal efficiencies in the monoplanted treatments and 63% in the nonplanted control after 10 wk of incubation. Similar removal efficiencies were obtained for fluorene. However, there was no significant difference in the dissipation of pyrene in both the mono- and multispecies vegetated treatments. There also was no significant difference between the dissipation of PAHs in the monoplanted treatments with different grass species. Principle component analysis (PCA) and cluster analysis were used to evaluate functional diversity of the different treatments during phytoremediation of PAHs. Both PCA and cluster analysis revealed differences in the metabolic fingerprints of the PAH contaminated and noncontaminated soils. However, the differences in metabolic diversity between the multispecies vegetated and monoplanted treatments were not clearly revealed. The results suggest that multispecies rhizoremediation using tolerant plant species rather than monoculture rhizoremediation have the potential to enhance pollutant removal in moderately contaminated soils.     

The unique aromatic catabolic genes in sphingomonads degrading polycyclic aromatic hydrocarbons (PAHs)

Many members of the sphingomonad genus isolated from different geological areas can degrade a wide variety of polycyclic aromatic hydrocarbons (PAHs) and related compounds. These sphingomonads such as Sphingobium yanoikuyae strain B1, Novosphingobium aromaticivorans strain F199, and Sphingobium sp. strain P2 have been found to possess a unique group of genes for aromatic degradation, which are distantly related with those in pseudomonads and other genera reported so far both in sequence homology and gene organization. Genes for aromatics degradation in these sphingomonads are complexly arranged; the genes necessary for one degradation pathway are scattered through several clusters. These aromatic catabolic gene clusters seem to be conserved among many other sphingomonads such as Sphingobium yanoikuyae strain Q1, Sphingomonas paucimobilis strain TNE12, S. paucimobilis strain EPA505, Sphingobium agrestis strain HV3, and Sphingomonas chungbukensis strain DJ77. Furthermore, some genes for naphthalenesulfonate degradation found in Sphingomonas xenophaga strain BN6 also share a high sequence homology with their homologues found in these sphingomonads. On the other hand, protocatechuic catabolic gene clusters found in fluorene-degrading Sphingomonas sp. strain LB126 appear to be more closely related with those previously found in lignin-degrading S. paucimobilis SYK-6 than the genes in this group of sphingomonads. This review summarizes the information on the distribution of these strains and relationships among their aromatic catabolic genes.     

Biodegradation of selected UV-irradiated and non-irradiated polycyclic aromatic hydrocarbons (PAHs)

Biodegradation of UV-irradiated anthracene, pyrene,benz[a]anthracene,and dibenz[a,h]anthracene was comparedto that of the non-irradiated samples, individuallyand in synthetic mixtures with enrichment cultures.Combined treatment was repeated for individual anthraceneand for the PAH mixture with Sphingomonas sp.strain EPA 505 and Sphingomonas yanoikuyae.Enrichment culture studies were performed on the PAHmixtures in the presence of the main photoproduct ofanthracene, pure 9,10-anthracenedione. Photochemicallypretreated creosote solutions were also subjected tobiodegradation and the results were compared tothose of the non-irradiated solutions. The primaryinterest was on 16 polycyclic aromatic hydrocarbons(PAHs) listed as priority pollutants by European Union(EU) and the United States Environmental ProtectionAgency (USEPA). Irradiation accelerated thebiodegradation onset for anthracene, pyrene, andbenz[a]anthracene when they were treatedindividually. The biodegradation of irradiatedpyrene started with no lag phase andwas complete by 122 h whereas biodegradation of thenon-irradiated sample had a lag of 280 h andresulted in complete degradation by 720 h. Biodegradation ofPAHs was accelerated in synthetic mixtures, especiallyin the presence of pure 9,10-anthracenedione.In general, irradiation had no effect on the biodegradation of PAHsincubated in synthetic mixtures or with pure cultures. Undercurrent experimental conditions, the UV-irradiation invariablyreduced the biodegradation of PAHs in creosote. Based onthe results of the present and previous photochemical-biologicalstudies of PAHs, the influence of the photochemical pretreatmenton the biodegradation is highly dependent on the compoundsbeing treated and other process parameters.     

Sorption of polycyclic aromatic hydrocarbons (PAHs) by dietary fiber extracted from wheat bran

The unintentional ingestion of carcinogenic xenobiotic substances leads to the high risk of cancer. Dietary fiber (DF) may protect against cancer by sorbing such chemicals. To this end, the sorption of four polycyclic aromatic hydrocarbons (PAHs) to DF extracted from wheat bran (WB) was studied. The strong affinity of PAHs to DF and WB indicated the effective binding of PAHs, and their distribution coefficients (K_d) positively increased with the increase in hydrophobicity of the PAHs. The DF had much higher K_d values for all PAHs compared to those of the unprocessed WB. The DF extraction process removed hydrophilic residues, such as starch, from WB, and increased the roughness of DF surface. Loss of hydrophilic components from WB to DF led to much higher affinity of DF with PAHs than WB. The results indicate that the DF can effectively sorb and remove xenobiotics, thereby having the potential to lower carcinogenic risk to humans.     

Cumulative exposure assessment for trace-level polycyclic aromatic hydrocarbons (PAHs) using human blood and plasma analysis

Humans experience chronic cumulative trace-level exposure to mixtures of volatile, semi-volatile, and non-volatile polycyclic aromatic hydrocarbons (PAHs) present in the environment as by-products of combustion processes. Certain PAHs are known or suspected human carcinogens and so we have developed methodology for measuring their circulating (blood borne) concentrations as a tool to assess internal dose and health risk. We use liquid/liquid extraction and gas chromatography–mass spectrometry and present analytical parameters including dynamic range (0–250 ng/ml), linearity (>0.99 for all compounds), and instrument sensitivity (range 2–22 pg/ml) for a series of 22 PAHs representing 2–6-rings. The method is shown to be sufficiently sensitive for estimating PAHs baseline levels (typical median range from 1 to 1000 pg/ml) in groups of normal control subjects using 1-ml aliquots of human plasma but we note that some individuals have very low background concentrations for 5- and 6-ring compounds that fall below robust quantitation levels.     

土壤－植物系统中多环芳烃和重金属的行为研究

对土壤中多环芳烃和重金属的行为研究表明,与对照相比,０—２０ｃｍ以上表土层存在多环芳烃和重金属积累,２０ｃｍ以下土层未发现积累;与春、秋两次采样结果相比,土壤中多环芳烃的含量有所下降,表明土壤微生物对多环芳烃有一定降解作用,且其降解程度与土壤－植物系统的生态结构有关．菲在地下水中检出浓度较高,表明这一污染物有向下迁移的可能性．此外,柳树对土壤中重金属Ｃｄ的积累有明显的削减与净化作用．本研究表明,严格限制污水中多环芳烃和重金属的污染负荷以及设计合理的生态结构是避免多环芳烃和重金属在土壤中积累的关键．     

Binding of polycyclic aromatic hydrocarbons (PAHs) to teleost aryl hydrocarbon receptors (AHRs)

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous, environmental contaminants that pose a potential risk to fish populations. Both field and laboratory studies suggest that exposure of the early life stages of fish to PAH can mimic the embryotoxic effects of the planar halogenated hydrocarbons (PHHs), the most potent of which is 2,3,7,8-tetrachlorodibenzo-p-dioxin. PHH toxicity is mediated by the aryl hydrocarbon receptor (AHR) and PHH potency is predicted by its AHR-binding affinity and CYP1A induction potency. However, the role of the AHR, if any, in mediating the developmental effects of PAH to fish remains unknown. In this study we looked at the AHR binding affinity of a test set of PAH that had been previously ranked for their potency for inducing teleost CYP1A. PAH that induced CYP1A inhibited [3H]TCDD binding to in vitro-expressed AHRs from rainbow trout and the AHR expressed in PLHC-1 fish hepatoma cells. Generally, the relative rank order for AHR binding affinity predicted the rank order of these same PAH for inducing CYP1A reported in other studies. There was a strong, positive relationship between binding to the PLHC-1 AHR (stimulus) and the EC50s for CYP1A induction (response) in whole juvenile trout and in RTL-W1 cells, but EC50s were much higher than expected for a 1:1 stimulus/response relationship. These data show that the ability of PAH to bind to teleost AHR predicts PAH potency for CYP1A induction. If PAH toxicity is receptor-mediated and predicted by induction potencies, we will have a powerful mechanistic-based tool for rapidly assessing the risk of toxicity to fish of PAH from any source.     

Aerobic bacterial degradation of polycyclic aromatic hydrocarbons (PAHs) and its kinetic aspects

Aerobic bacterial degradation of PAHs is reviewed. Particular attention is paid to its kinetic aspects (rate and specificity). The general concepts of PAH biodegradation in nature and the role of aerobic bacteria in this process are described. The problem of PAH bioavailability and the mechanism of PAH penetration through bacterial cell wall are discussed. The key role of the reaction of PAH hydroxylation in controlling the rate and specificity of PAH biodegradation process is substantiated. The effects of competitive inhibition, intermediate inhibition, cross induction, and cometabolism are considered. The importance of microbial communities for PAH biodegradation in natural ecosystems is shown. The review contains the list of 138 references.     

Effectiveness of phytoremediation as a secondary treatment for polycyclic aromatic hydrocarbons (PAHs) in composted soil

A greenhouse study was conducted over a 12-month period to investigate the fate of polycyclic aromatic hydrocarbons (PAHs) in soil using phytoremediation as a secondary treatment. The soil was pretreated by composting for 12 weeks, then planted with tall fescue (Festuca arundinacea), annual ryegrass (Lolium multiflorum), and yellow sweet clover (Melilotus officinalis). Two sets of unvegetated controls also were evaluated, one fertilized and one unfertilized. Total PAH concentrations decreased in the tall fescue, annual ryegrass, and yellow sweet clover treatments by 23.9%, 15.3%, and 9.1%, respectively, whereas the control was reduced by less than 5%. The smaller two- and most of the three-ringed compounds--naphthalene, acenaphthylene, acenaphthene, fluorene, and anthracene--were not found in detectable concentrations in any of the treatments. The most probable number analysis for microbial PAH degraders did not show any statistically significant differences among treatments. There were significant differences among treatments (p < 0.05) for the residual concentrations of five of the target PAHs. Root surface area measurements indicated that tall fescue and annual ryegrass both had significantly higher root surface area than yellow sweet clover, although the two species were not significantly different from each other. The tall fescue treatment resulted in the highest root and shoot biomass, followed by annual ryegrass and yellow sweet clover, and also had the highest percent of contaminant removal after 12 months. These results imply a positive relationship between plant biomass development and PAH biodegradation.     

Health risk assessment of atmospheric polycyclic aromatic hydrocarbons over the Central Himalayas

Carcinogenic risk assessments of polycyclic aromatic hydrocarbons (PAHs) in four sites from the Central Himalayas (Bode, Lumbini, Pokhara, and Dhunche) were performed. Lifetime Average Daily Dose (LADD), Lifetime lung cancer risk (LLCR) and Incremental lifetime cancer risk (ILCR) were calculated in order to evaluate the cancer risk. PAHs levels were converted to BaP equivalent concentrations (B[a]Peq), and models of health risk assessment were applied. B[a]Peq concentrations exceeded the standard limited value (1 ng/m³) in all the four sites. The human health risk assessment (HHRA) demonstrated high carcinogenic risk on residents of Bode and Lumbini. Further, LLCR in all sites were over the acceptable range (1.15E-03, 7.90E-04, 1.40E-04 and 9.96E-05, respectively); however, ILCR ranking exhibited acceptable range in Lumbini, Pokhara, and Dhunche (7.10E-06, 1.26E-06, and 8.95E-07). The risk variation among the sites is due to the difference in pollution status. The study shows health risk due to atmospheric PAHs via inhalation prevails all the seasons throughout, differing only seasonally; nevertheless, the concentration and carcinogenic risk decreased remarkably from south-north transect of the central Himalaya. Keeping some uncertainties aside, this study provides noble insights and helps to formulate new advance assessment on the carcinogenic risk of atmospheric PAHs over the Central Himalayas.     

Genome-to-function characterization of novel fungal P450 monooxygenases oxidizing polycyclic aromatic hydrocarbons (PAHs)

Fungi, particularly the white rot basidiomycetes, have an extraordinary capability to degrade and/or mineralize (to CO₂) the recalcitrant fused-ring high molecular weight (?4 aromatic-rings) polycyclic aromatic hydrocarbons (HMW PAHs). Despite over 30 years of research demonstrating involvement of P450 monooxygenation reactions in fungal metabolism of HMW PAHs, specific P450 monooxygenases responsible for oxidation of these compounds are not yet known. Here we report the first comprehensive identification and functional characterization of P450 monooxygenases capable of oxidizing different ring-size PAHs in the model white rot fungus Phanerochaete chrysosporium using a successful genome-to-function strategy. In a genome-wide P450 microarray screen, we identified six PAH-responsive P450 genes (Pc-pah1-Pc-pah6) inducible by PAHs of varying ring size, namely naphthalene, phenanthrene, pyrene, and benzo(a)pyrene (BaP). Using a co-expression strategy, cDNAs of the six Pc-Pah P450s were cloned and expressed in Pichia pastoris in conjunction with the homologous P450 oxidoreductase (Pc-POR). Each of the six recombinant P450 monooxygenases showed PAH-oxidizing activity albeit with varying substrate specificity towards PAHs (3-5 rings). All six P450s oxidized pyrene (4-ring) into two monohydroxylated products. Pc-Pah1 and Pc-Pah3 oxidized BaP (5-ring) to 3-hydroxyBaP whereas Pc-Pah4 and Pc-Pah6 oxidized phenanthrene (3-ring) to 3-, 4-, and 9-phenanthrol. These PAH-oxidizing P450s (493-547 aa) are structurally diverse and novel considering their low overall homology (12-23%) to mammalian counterparts. To our knowledge, this is the first report on specific fungal P450 monooxygenases with catalytic activity toward environmentally persistent and highly toxic HMW PAHs.     

Ecological risk assessment of polycyclic aromatic hydrocarbons in surface sediments from the middle and lower reaches of the Yellow River,China

In this research, ecological risks for eight individual polycyclic aromatic hydrocarbons (PAHs) and ∑PAH₈ in surface sediments from middle and lower reaches of Yellow River are evaluated using overlapping areas of probability density curves and margin of safety (MOS), based on the toxicity data and the exposure concentrations of PAHs in sediments collected from 23 sites. In the overlapping areas of probability density curves, the risk of Ant and Pyr are the highest, then the risk level is in the order of Flua > Nap > Phe > BaP > Flu > Ace. The values of MOS₁₀ present that Pyr (4.62 × 10^?4), Ant (5.60 × 10^?3), and Flua (6.4 × 10^?3) have a significantly high ecological risk level, while Nap and Phe have middle-level ecological risk. As for Ace, BaP, and Flu, they pose limited risk to the ecological system with MOS₁₀ greater than 1.0. The ∑PAH₈ (2.66 × 10^?5) is a higher risk level than that of any individual PAHs, where the probabilities of ∑PAH₈ in excess of the 10th percentile of the toxicity data were 86%.     

Human health risk assessment and source diagnosis of polycyclic aromatic hydrocarbons (PAHs) in the corn and agricultural soils along main roadside in Changchun,China

This work was to investigate distribution characteristics, human health risk assessment, and possible sources of 16 priority polycyclic aromatic hydrocarbons (PAHs) in corn and surface soils of farmlands along main roadside in Changchun City, Jilin Province, China. Total concentrations of 16 PAHs ranged from 1572.4 to 4390.2 µg/kg with a mean value of 2954.9 µg/kg in soils and from 219.9 to 627 µg/kg with a mean value of 362µg/kg in corn. Light-molecular-weight PAHs (2–3 rings) concentration was dominant in soils, accounting for 51%, whereas high-molecular-weight PAHs (5–6 rings) concentration was highest in corn, accounting for 48%. The results of plant concentration factor indicated that high-molecular-weight PAHs have greater mobility. To evaluate potential risk to human health, hazard index (HI) and risk index (RI) were employed. The values of HI for corn and soils were both smaller than 1, indicating that exposure of PAHs posed no or little potential risk to local residents. The fact that values of RI for corn and soils were smaller than 1 × 10^–4 suggested that exposure of PAHs posed no or little cancer risk to local residents. The possible sources of PAHs in corn and soils were both identified as mixture patterns of pyrogenic and petrogenic sources.     

Adsorption of polycyclic aromatic hydrocarbons (PAHs) by soil particles: influence on biodegradability and biotoxicity

Summary Polycyclic aromatic hydrocarbon (PAH) biodegradation was investigated in contaminated soils from two different industrial sites under simulated land treatment conditions. Soil samples from a former impregnation plant (soil A) showed high degradation rates of PAHs by the autochthonous microorganisms, whereas PAHs in material of a closed-down coking plant (soil B) were not degraded even after inoculation with bacteria known to effectively degrade PAHs. As rapid PAH biodegradation in soil B was observed after PAHs were extracted and restored into the extracted soil material, the kind of PAH binding in soil B appears to completely prevent biodegradation. Sorption of PAHs onto extracted material of soil B follows a two-phase process (fast and slow); the latter is discussed in terms of migration of PAHs into soil organic matter, representing less accessible sites within the soil matrix. Such sorbed PAHs are suggested to be non-bioavailable and thus non-biodegradable. By eluting soil B with water, no biotoxicity, assayed as inhibition of bioluminescence, was detected in the aqueous phase. When treating soil A analogously, a distinct toxicity was observed, which was reduced relative to the amount of activated carbon added to the soil material. The data suggest that sorption of organic pollutants onto soil organic matter significantly affects biodegradability as well as biotoxicity.     

Gene regulation in the marine diatom Thalassiosira pseudonana upon exposure to polycyclic aromatic hydrocarbons (PAHs)

Diatoms are eukaryotic algae, which can be found worldwide in oceans and freshwaters. These organisms are ecologically relevant due to their key role in the global carbon cycle, contributing to about 25% to the global primary production [Falciatore, A., Bowler, C., 2002. Revealing the molecular secrets of marine diatoms. Annu. Rev. Plant Biol. 53, 109-130]. We investigated the effects of three polycyclic aromatic hydrocarbons (PAHs, pyrene, fluoranthene, and benzo[a]pyrene), either as single compound or as mixture, at molecular level. Dose-response curves for growth inhibition were determined and four concentrations eliciting from "no effect" up to a severe growth inhibition were chosen for further investigation to detect alterations at gene expression level by Real-Time PCR. Among the eight selected genes, two were strongly influenced by the PAH treatment. lacsA, which is involved in the fatty acid metabolism, was found to be strongly up-regulated by all single PAHs, as well as by the mixture. sil3, involved in the formation of the silica shell, was repressed by a factor up to three even at low PAH concentrations not eliciting any growth inhibition. For other genes, involved e.g. in photosynthesis, a slight down-regulation was detected. Based on the effects at gene expression level it can be assumed that PAHs impair the fatty acid metabolism and silica shell formation.     

两种植物条件下土壤中矿物油和多环芳烃（PAHs）的生物修复研究

选择苜蓿草和水稻为供试植物,以污染物水平、有机以、专性细菌和真菌为调控因子,进行土壤中矿物油和PAHs的生物修复研究,结果表明,投肥对苜蓿草土壤中矿物油降解有促进作用,但对水稻土壤中矿物油降解无明显作用,投肥均使苜蓿草和水稻土壤中多环芒烃总量（11种列于美国EPA黑名单上的多环芳烃）降解率提高,这一降解促进效果在水稻土壤中好于苜蓿草土壤,有机肥量与苜蓿草根际土著真菌、细菌数量明显呈正相关,但仅与水稻根际土著细菌数量呈明显正相关,两种土壤中实测真菌和细菌总数均与试验投加专性真菌和细菌量无关,水稻土和苜蓿草土壤中3环多环芳烃的降解随投肥量增大而降解率提高,其在水稻土蓑中的效果好于苜蓿草土壤,投肥怪4环多环芳烃的降解并未产生有效作用。     

多环芳烃在土壤中的行为

多环芳烃（PAHs)在土壤中达到吸附平衡时存在“快”和“慢”两个吸附过程,植物能够从土壤中吸收低分子量的PAHs并向植物的地上部分迁移转化,但PAHs在植物体内主要的累积方式是植物地上部分的空气污染,微生物对PAHs的降解依然是去除PAHs的主要方式,主要通过微生物产生的酶的作用,本文详细分析了影响PAHs生物去除的各种因素。