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Polycyclic aromatic hydrocarbon removal from subsurface soil mediated by bacteria and archaea under methanogenic conditions: Performance and mechanisms
2022
Gou, Yaling | Song, Yun | Yang, Sucai | Yang, Yan | Cheng, Yanan | Li, Jiabin | Zhang, Tengfei | Cheng, Yanjun | Wang, Hongqi
In situ anoxic bioremediation is an easy-to-use technology to remediate polycyclic aromatic hydrocarbon (PAH)-contaminated soil. Degradation of PAHs mediated by soil bacteria and archaea using CO₂ as the electron acceptor is an important process for eliminating PAHs under methanogenic conditions; however, knowledge of the performance and mechanisms involved is poorly unveiled. In this study, the effectiveness and efficiency of NaHCO₃ (CO₂) as an electron acceptor to stimulate the degradation of PAHs by bacteria and archaea in highly contaminated soil were investigated. The results showed that CO₂ addition (EC2000) promoted PAH degradation compared to soil without added CO₂ (EC0), with 4.18%, 9.01%–8.05%, and 6.19%–12.45% increases for 2-, 3- and 4-ring PAHs after 250 days of incubation, respectively. Soil bacterial abundances increased with increasing incubation time, especially for EC2000 (2.90 × 10⁸ g⁻¹ soil higher than EC0, p < 0.05). Different succession patterns of the soil bacterial and archaeal communities during PAH degradation were observed. According to the PCoA and ANOSIM results, the soil bacterial communities were greatly (ANOSIM: R = 0.7232, P = 0.001) impacted by electron acceptors, whereas significant differences in the archaeal communities were not observed (ANOSIM: R = 0.553, P = 0.001). Soil bacterial and archaeal co-occurrence network analyses showed that positive correlations outnumbered the negative correlations throughout the incubation period for both treatments (e.g., EC0 and EC2000), suggesting the prevalence of coexistence/cooperation within and between these two domains rather than competition. The higher complexity, connectance, edge, and node numbers in EC2000 revealed stronger linkage and a more stable co-occurrence network compared to EC0. The results of this study could improve the knowledge on the removal of PAHs and the responses of soil bacteria and archaea to CO₂ application, as well as a scientific basis for the in situ anoxic bioremediation of PAH-contaminated industrial sites.
Afficher plus [+] Moins [-]The longitudinal biomonitoring of residents living near the waste incinerator of Turin: Polycyclic aromatic hydrocarbon metabolites after three years from the plant start-up
2022
Iamiceli, A.L. | Abate, V. | Bena, A. | De Filippis, Sp | De Luca, S. | Iacovella, N. | Farina, E. | Gandini, M. | Orengia, M. | De Felip, E. | Abballe, A. | Dellatte, E. | Ferri, F. | Fulgenzi, Ar | Ingelido, A.M. | Ivaldi, C. | Marra, V. | Miniero, R. | Crosetto, L. | Procopio, E. | Salamina, G.
The waste-to-energy (WTE) incinerator plant located in the Turin area (Italy) started to recover energy from the combustion of municipal solid waste in 2013. A health surveillance program was implemented to evaluate the potential health effects on the population living near the plant. This program included a longitudinal biomonitoring to evaluate temporal changes of some environmental pollutants, including polycyclic aromatic hydrocarbons (PAHs), in residents living in areas near the Turin incinerator (exposed group, E) compared to those observed in subjects living far from the plant (not exposed group, NE). Ten monohydroxy-PAHs (OH-PAHs), consisting in the principal metabolites of naphthalene, fluorine, phenanthrene, and pyrene, were analyzed in urines collected from the E and NE subjects after one (T₁) and three years (T₂) of plant activity and compared with those determined in the same cohort established before the plant start-up (T₀). Spearman correlation analysis was undertaken to explore possible associations between OH-PAHs and personal characteristics, lifestyle variables, and dietary habits. A linear mixed model (LMM) approach was applied to determine temporal trends of OH-PAHs observed in the E and NE subjects and to evaluate possible differences in trend between the two groups. Temporal trends of OH-PAHs determined by LMM analysis demonstrated that, at all times, the E group had concentrations lower than those assessed in the NE group, all other conditions being equal. Moreover, no increase in OH-PAH concentrations was observed at T₁ and T₂ either in E or in NE group. Significant positive correlations were found between all OH-PAHs and smoking habits. Regarding variables associated to outdoor PAH exposure, residence near high traffic roads and daily time in traffic road was positively correlated with 1-hydroxynaphthalene and 1-hydroxypyrene, respectively. In conclusion, no impact of the WTE plant on exposure to PAHs was observed on the population living near the plant.
Afficher plus [+] Moins [-]Laccase production by Pleurotus ostreatus using cassava waste and its application in remediation of phenolic and polycyclic aromatic hydrocarbon-contaminated lignocellulosic biorefinery wastewater
2022
Kumar, Vaidyanathan Vinoth | Venkataraman, Swethaa | Kumar, P Senthil | George, Jenet | Rajendran, Devi Sri | Shaji, Anna | Lawrence, Nicole | Saikia, Kongkona | Rathankumar, Abiram Karanam
The treatment of contaminants from lignocellulosic biorefinery effluent has recently been identified as a unique challenge. This study focuses on removing phenolic contaminants and polycyclic aromatic hydrocarbons (PAHs) from lignocellulosic biorefinery wastewater (BRW) applying a laccase-assisted approach. Cassava waste was used as a substrate to produce the maximum yield of laccase enzyme (3.9 U/g) from Pleurotus ostreatus. Among the different inducers supplemented, CuSO₄ (0.5 mM) showed an eight-fold increase in enzyme production (30.8 U/g) after 240 h of incubation. The catalytic efficiency of laccase was observed as 128.7 ± 8.47 S⁻¹mM⁻¹ for syringaldazine oxidation at optimum pH 4.0 and 40 °C. Laccase activity was completely inhibited by lead (II) ion, mercury (II) ion, sodium dodecyl sulphate, sodium azide and 1,4 dithiothretiol and induced significantly by manganese (II) ion and rhamnolipid. After treating BRW with laccase, the concentrations of PAHs and phenolic contaminants of 1144 μg/L and 46160 μg/L were reduced to 96 μg/L and 16100 μg/L, respectively. The ability of laccase to effectively degrade PAHs in the presence of different phenolic compounds implies that phenolic contaminants may play a role in PAHs degradation. After 240 h, organic contaminants were removed from BRW in the following order: phenol >2,4-dinitrophenol > 2-methyl-4,6-dinitrophenol > 2,3,4,6-tetrachlorophenol > acenaphthene > fluorine > phenanthrene > fluoranthene > pyrene > anthracene > chrysene > naphthalene > benzo(a)anthracene > benzo(a)pyrene > benzo(b)fluoranthene > pentachlorophenol > indeno(1,2,3-cd)pyrene > benzo(j) fluoranthene > benzo[k]fluoranthène. The multiple contaminant remediation from the BRW by enzymatic method, clearly suggests that the laccase can be used as a bioremediation tool for the treatment of wastewater from various industries.
Afficher plus [+] Moins [-]Opposite selection effects of nZVI and PAHs on bacterial community composition revealed by universal and sphingomonads-specific 16S rRNA primers
2022
Sheng, Dong | Chen, Minjie | Chen, Qiqi | Huang, Yili
Next-generation sequencing method employing the sphingomonads-specific and universal 16s rRNA primers were applied to analyze the response of soil bacterial community to continuous stress of nanoscale zero-valent iron (nZVI) and/or polycyclic aromatic hydrocarbons (PAHs) under suspended conditions. The group specific primer greatly improves taxonomic resolution, the overall OTU numbers increased from 12 by universal primer to 42 by sphingomonads-specific primer. It was found that nZVI and PAHs had opposite selection effects on bacterial community composition, furthermore, the abundance of Sphingopyxis was positively related to nZVI while negatively related to PAHs, whereas abundances of Sphingobium and Sphingosinicella were positively related to PAHs (p < 0.01). The improved taxonomic resolution helps identify the potential keystone taxa, which provides valuable information for future bioremediation technology such as synthetic microbiome.
Afficher plus [+] Moins [-]The association of co-exposure to polycyclic aromatic hydrocarbon and phthalates with blood cell-based inflammatory biomarkers in children: A panel study
2022
Zhao, Lei | Liu, Miao | Liu, Linlin | Guo, Wenting | Yang, Huihua | Chen, Shuang | Yu, Jie | Li, Meng | Fang, Qin | Lai, Xuefeng | Yang, Liangle | Zhang, Xiaomin
The association of co-exposure to polycyclic aromatic hydrocarbons (PAHs) and phthalates (PAEs) with blood cell-based inflammatory biomarkers is largely unknown. We conducted a panel study of 144 children aged 4–12 years, with up to 3 repeated visits across 3 seasons. For each visit, we collected the first-morning urine for 4 consecutive days and fasting blood on the day of physical examination. We developed a gas chromatography/tandem mass spectrometry method to detect the metabolites of 10 PAHs (OH-PAHs) and 10 PAEs (mPAEs) in urine samples. We employed linear mixed-effects models to evaluate the individual associations of each OH-PAH and mPAE with blood cell-based inflammatory biomarkers over different lag times. Bayesian kernel machine regression (BKMR) and quantile g-computation were used to evaluate the overall associations of OH-PAHs and mPAEs mixtures with blood cell-based inflammatory biomarkers. After multiple adjustments, we found positive associations of summed hydroxylphenanthrene (∑OHPHE), summed OH-PAHs, and mono-n-butyl phthalate with inflammatory biomarkers such as neutrophil count, neutrophil-to-lymphocyte ratio, platelet-to-lymphocyte ratio, and the systemic immune-inflammation index (SII) at lag 0 (the day of physical examination). Each 1% increase in ∑OHPHE was related to a 0.18% (95% confidence interval: 0.10%, 0.25%) increase in SII, which was the strongest among the above associations. The results of BKMR and quantile g-computation suggested that co-exposure to PAHs and PAEs mixture was associated with an elevated white blood cell count, neutrophil count, neutrophil-to-lymphocyte ratio, platelet-to-lymphocyte ratio, and SII, to which ∑OHPHE and 1-hydroxypyrene (1-OHPYR) might be the major contributors. In addition, gender and age modified the associations of ∑OHPHE and 1-OHPYR with inflammatory biomarkers, where girls and younger children were more susceptible. In conclusion, co-exposure to PAHs and PAEs was associated with elevated inflammation in children, in which ∑OHPHE and 1-OHPYR might play important roles.
Afficher plus [+] Moins [-]Legacy PAHs in effluent receiving river sediments near a large petroleum products depot in Enugu, Nigeria: Human health risks and economic cost of pollution
2022
Ugochukwu, Uzochukwu C. | Chukwuone, Nnaemeka Andegbe | Jidere, Chika | Agu, Chizoba | Kurumeh, Leonard | Ezeudu, Obiora Boniface
This study assessed the human health risk of exposure to legacy PAHs in the Nwaenebo River sediments that received effluents for over two decades from the Nigeria National Petroleum Corporation (NNPC) petroleum product Depot in Emene, Enugu, Nigeria. The study went further to estimate economic costs of the sediment PAHs pollution based on the human health risk of exposure. The human health risks were determined by estimating carcinogenic and mutagenic risks via Benzo[a]pyrene total potential equivalent (BaP TPE) and mutagenic equivalent quotient (MEQ). The economic costs of the sediment pollution comprised costs due to mortality and those due to morbidity and were estimated using the value of statistical lives (VSLs) and cost of illness (CoI), respectively. The study, with an appropriate selection of sampling points established that the NNPC petroleum Depot was responsible for the Nwaenebo River sediment PAHs pollution with ƩPAHs concentration 14.3–163 mg/kg. The carcinogenic and mutagenic risks varied from 1.3*10^-5 to 4.7*10^-5 and 1.4*10^-5 to 6.0*10^-5 respectively. Based on risk threshold of 10^-6, these risks were high. The long term economic costs of pollution of the sediments by the PAHs were estimated at 60.5 million USD and 0.46 million USD for mortality and morbidity costs, respectively.
Afficher plus [+] Moins [-]Human health risks estimations from polycyclic aromatic hydrocarbons in serum and their hydroxylated metabolites in paired urine samples
2021
Yang, Ziying | Guo, Chongshan | Li, Qin | Zhong, Yi | Ma, Shengtao | Zhou, Jinhua | Li, Xiaotong | Huang, Rende | Yu, Yingxin
Polycyclic aromatic hydrocarbons (PAHs) are compounds with two or more benzene rings whose hydroxylated metabolites (OH-PAHs) are excreted in urine. Human PAH exposure is therefore commonly estimated based on urinary OH-PAH concentrations. However, no study has compared PAH exposure estimates based on urinary OH-PAHs to measurements of PAH levels in blood samples. Estimates of PAH exposure based solely on urinary OH-PAHs may thus be subject to substantial error. To test this hypothesis, paired measurements of parent PAHs in serum and OH-PAHs in urine samples from 480 participants in Guangzhou, a typical developed city in southern China, were used to investigate differences in the estimates of human PAH exposure obtained by sampling different biological matrices. The median PAH concentration in serum was 4.05 ng mL⁻¹, which was lower than that of OH-PAHs in urine (8.33 ng mL⁻¹). However, serum pyrene levels were significantly higher than urinary levels of its metabolite 1-hydroxypyrene. Concentrations of parent PAHs in serum were not significantly correlated with those of their metabolites in urine with the exception of phenanthrene, which exhibited a significant negative correlation. Over 28% of the participants had carcinogenic risk values above the acceptable cancer risk level of 10⁻⁶. Overall, estimated human exposure and health risks based on urinary 1-hydroxypyrene levels were only 13.6% of those based on serum pyrene measurements, indicating that estimates based solely on urine sampling may substantially understate health risks due to PAH exposure.
Afficher plus [+] Moins [-]Polycyclic aromatic hydrocarbon contamination along roads based on levels on vehicle window films
2021
Zhang, Weiwei | Su, Penghao | Tomy, Gregg T. | Sun, Dan | Yin, Fang | Chen, Lisu | Ding, Yongsheng | Li, Yifan | Feng, Daolun
Vehicular emissions are known to be major contributors of airborne polycyclic aromatic hydrocarbons (PAHs) in cities. In order to assess the long-term contamination of PAHs along roads, we collected organic films from vehicle windows (26 private cars and 4 buses, in Shanghai, China) and used mathematical models to convert the film-bound PAH concentrations to the airborne PAH concentrations. The field measurements of airborne PAHs revealed that the partitioning and Level III fugacity model was suitable to estimate the airborne concentrations of high and low volatile PAHs (expect for naphthalene), respectively. The total airborne PAH concentrations along roads in Shanghai ranged from 0.83 to 3.37 μg m⁻³ and the incremental lifetime cancer risks (ILCRₜₒₜₐₗ) by exposure to PAHs along roads were greater than the USEPA lower guideline of 10⁻⁶, indicating non-negligible carcinogenic risks to drivers and passengers, especially via ingestion processes. This study provided a practicable method to investigate long-term air contamination of PAHs in vehicles and along roads based on film-bound PAH on vehicle windows. In addition, it was also possible to investigate the health risk in vehicles as a result of exposure to PAHs. Comparisons of PAHs between roads and shipping lanes also facilitated the delineation of vehicular and shipping PAH inventories.A capsule that summarizes the main finding of the work: Investigating film-bound PAH on vehicle windows is a practicable pathway to investigate the long-term contamination of PAHs in vehicles and along roads. This method can not only simplify the sampling processes, but the model calculations. The results also enabled investigations into ILCR in vehicles and specified source apportionment of traffic PAHs.
Afficher plus [+] Moins [-]Targeting the right parameters in PAH remediation studies
2021
Davin, Marie | Colinet, Gilles | Fauconnier, Marie-Laure
Contaminated land burdens the economy of many countries and must be dealt with.Researchers have published thousands of documents studying and developing soil and sediment remediation treatments. Amongst the targeted pollutants are the polycyclic aromatic hydrocarbons (PAHs), described as a class of persistent organic compounds, potentially harmful to ecosystems and living organisms.The present paper reviews and discusses three scientific trends that are leading current PAH-contaminated soil/sediment remediation studies and management.First, the choice of compounds that are being studied and targeted in the scientific literature is discussed, and we suggest that the classical 16 US-EPA PAH compounds might no longer be sufficient to meet current environmental challenges.Second, we discuss the choice of experimental material in remediation studies. Using bibliometric measures, we show the lack of PAH remediation trials based on co-contaminated or aged-contaminated material.Finally, the systematic use of the recently validated bioavailability measurement protocol (ISO/TS 16751) in remediation trials is discussed, and we suggest it should be implemented as a tool to improve remediation processes and management strategies.
Afficher plus [+] Moins [-]Characterization of polycyclic aromatic compounds in historically contaminated soil by targeted and non-targeted chemical analysis combined with in vitro bioassay
2021
Titaley, Ivan A. | Lam, Monika M. | Bülow, Rebecca | Enell, Anja | Wiberg, Karin | Larsson, Maria
Soil samples from a contaminated site in Sweden were analyzed to identify the presence of 78 polycyclic aromatic compounds (PACs) using gas chromatography coupled with mass spectrometry (GC-MS). The target analysis revealed large contributions not only from polycyclic aromatic hydrocarbons (PAHs), but also from alkylated- and oxygenated-PAHs (alkyl- and oxy-PAHs, respectively), and N-heterocyclics (NPACs). PAC profiles indicated primarily pyrogenic sources, although contribution of petrogenic sources was also observed in one sample as indicated by a high ratio of alkylated naphthalene compared to naphthalene. The aryl hydrocarbon receptor (AhR)-activity of the soil extracts was assessed using the H4IIe-pGudluc 1.1 cells bioassay. When compared with the calculated total AhR-activity of the PACs in the target list, 35–97% of the observed bioassay activity could be explained by 62 PACs with relative potency factors (REPs). The samples were further screened using GC coupled with Orbitrap™ high resolution MS (GC-HRMS) to investigate the presence of other PACs that could potentially contribute to the AhR-activity of the extracts. 114 unique candidate compounds were tentatively identified and divided into four groups based on their AhR-activity and environmental occurrence. Twelve substances satisfied all the criteria, and these compounds are suggested to be included in regular screening in future studies, although their identities were not confirmed by standards in this study. High unexplained bio-TEQ fractions in three of the samples may be explained by tentatively identified compounds (n = 35) with high potential of being toxic. This study demonstrates the benefit of combining targeted and non-targeted chemical analysis with bioassay analysis to assess the diversity and effects of PACs at contaminated sites. The applied prioritization strategy revealed a number of tentatively identified compounds, which likely contributed to the overall bioactivity of the soil extracts.
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