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1.
J Hazard Mater ; 471: 134437, 2024 Jun 05.
Article En | MEDLINE | ID: mdl-38691934

Crude oil is a hazardous pollutant that poses significant and lasting harm to human health and ecosystems. In this study, Moesziomyces aphidis XM01, a biosurfactant mannosylerythritol lipids (MELs)-producing yeast, was utilized for crude oil degradation. Unlike most microorganisms relying on cytochrome P450, XM01 employed two extracellular unspecific peroxygenases, MaUPO.1 and MaUPO.2, with preference for polycyclic aromatic hydrocarbons (PAHs) and n-alkanes respectively, thus facilitating efficient crude oil degradation. The MELs produced by XM01 exhibited a significant emulsification activity of 65.9% for crude oil and were consequently supplemented in an "exogenous MELs addition" strategy to boost crude oil degradation, resulting in an optimal degradation ratio of 72.3%. Furthermore, a new and simple "pre-MELs production" strategy was implemented, achieving a maximum degradation ratio of 95.9%. During this process, the synergistic up-regulation of MaUPO.1, MaUPO.1 and the key MELs synthesis genes contributed to the efficient degradation of crude oil. Additionally, the phylogenetic and geographic distribution analysis of MaUPO.1 and MaUPO.1 revealed their wide occurrence among fungi in Basidiomycota and Ascomycota, with high transcription levels across global ocean, highlighting their important role in biodegradation of crude oil. In conclusion, M. aphidis XM01 emerges as a novel yeast for efficient and eco-friendly crude oil degradation.


Biodegradation, Environmental , Glycolipids , Mixed Function Oxygenases , Petroleum , Surface-Active Agents , Petroleum/metabolism , Surface-Active Agents/metabolism , Surface-Active Agents/chemistry , Glycolipids/metabolism , Mixed Function Oxygenases/metabolism , Mixed Function Oxygenases/genetics , Polycyclic Aromatic Hydrocarbons/metabolism , Polycyclic Aromatic Hydrocarbons/chemistry , Alkanes/metabolism
2.
Bull Environ Contam Toxicol ; 112(5): 76, 2024 May 11.
Article En | MEDLINE | ID: mdl-38733550

Traffic-related particulate matter emissions have been considerably reduced due to stringent regulations in Europe. However, emission of diesel-powered vehicles still poses a significant environmental threat, affecting rural ecosystems and agriculture. Several studies have reported that polycyclic aromatic hydrocarbons (PAHs), a group of potentially toxic organic compounds, can accumulate in crops and vegetables. In our study, white mustard (Sinapis alba L.) plants were experimentally treated with an extract of diesel exhaust. PAH concentrations were measured in the different plant compartments (stems, leaves and seeds), bioconcentration factors (BCFs) were also calculated. Significant accumulation was measured in the leaves and seeds, stems showed lower accumulation potential. All plant matrices showed high tendency to accumulate higher molecular weight PAHs, BCF was the highest in the 6-ring group. The fact that considerable accumulation was experienced in the seeds might show the risk of cultivating crops nearby roads highly impacted by traffic-related emissions.


Air Pollutants , Environmental Monitoring , Polycyclic Aromatic Hydrocarbons , Seeds , Seeds/chemistry , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/metabolism , Air Pollutants/analysis , Sinapis , Vehicle Emissions/analysis , Particulate Matter/analysis
3.
Sci Total Environ ; 929: 172362, 2024 Jun 15.
Article En | MEDLINE | ID: mdl-38649047

Pollution-induced declines in fishery resources restrict the sustainable development of fishery. As a kind of typical environmental pollutant, the mechanism of polycyclic aromatic hydrocarbons (PAHs) facilitating fishery resources declines needs to be fully illustrated. To determine how PAHs have led to declines in fishery resources, a systematic toxicologic analysis of the effects of PAHs on aquatic organisms via food-web bioaccumulation was performed in the Pearl River and its estuary. Overall, PAH bioaccumulation in aquatic organisms was correlated with the trophic levels along food-web, exhibiting as significant positive correlations were observed between PAHs concentration and the trophic levels of fishes in the Pearl River Estuary. Additionally, waterborne PAHs exerted significant direct effects on dietary organisms (P < 0.05), and diet-borne PAHs subsequently exhibited significant direct effects on fish (P < 0.05). However, an apparent block effect was found in dietary organisms (e.g., zooplankton) where 33.49 % of the total system throughput (TST) was retained at trophic level II, exhibiting as the highest PAHs concentration, bioaccumulation factor (BAF), and biomagnification factor (BMF) of ∑15PAHs in zooplankton were at least eight-fold greater than those in fishes in both the Pearl River and its estuary, thereby waterborne PAHs exerted either direct or indirect effects on fishes that ultimately led to food-web simplification. Regardless of the block effect of dietary organisms, a general toxic effect of PAHs on aquatic organisms was observed, e.g., Phe and BaP exerted lethal effects on phytoplankton Chlorella pyrenoidosa and zooplankton Daphnia magna, and decreased reproduction in fishes Danio rerio and Megalobrama hoffmanni via activating the NOD-like receptors (NLRs) signaling pathway. Consequently, an assembled aggregate exposure pathway for PAHs revealed that increases in waterborne PAHs led to bioaccumulation of PAHs in aquatic organisms along food-web, and this in turn decreased the reproductive ability of fishes, thus causing decline in fishery resources.


Aquatic Organisms , Bioaccumulation , Environmental Monitoring , Food Chain , Polycyclic Aromatic Hydrocarbons , Water Pollutants, Chemical , Water Pollutants, Chemical/toxicity , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/metabolism , Animals , Aquatic Organisms/drug effects , Fishes/metabolism , Estuaries , Rivers/chemistry , China
4.
Environ Microbiol Rep ; 16(2): e13197, 2024 Apr.
Article En | MEDLINE | ID: mdl-38600035

Many microbial genes involved in degrading recalcitrant environmental contaminants such as polycyclic aromatic hydrocarbons (PAHs) have been identified and characterized. However, all molecular mechanisms required for PAH utilization have not yet been elucidated. In this work, we demonstrate the proposed involvement of lasso peptides in the utilization of the PAH phenanthrene in Sphingomonas BPH. Transpositional mutagenesis of Sphingomonas BPH with the miniTn5 transposon yielded 3 phenanthrene utilization deficient mutants, #257, #1778, and #1782. In mutant #1782, Tn5 had inserted into the large subunit of the naph/bph dioxygenase gene. In mutant #1778, Tn5 had inserted into the B2 protease gene of a lasso peptide cluster. This finding is the first report on the role of lasso peptides in PAH utilization. Our studies also demonstrate that interruption of the lasso peptide cluster resulted in a significant increase in the amount of biosurfactant produced in the presence of glucose when compared to the wild-type strain. Collectively, these results suggest that the mechanisms Sphingomonas BPH utilizes to degrade phenanthrene are far more complex than previously understood and that the #1778 mutant may be a good candidate for bioremediation when glucose is applied as an amendment due to its higher biosurfactant production.


Phenanthrenes , Polycyclic Aromatic Hydrocarbons , Polycyclic Aromatic Hydrocarbons/metabolism , Biodegradation, Environmental , Phenanthrenes/metabolism , Peptides/genetics , Glucose
5.
Int J Mol Sci ; 25(8)2024 Apr 13.
Article En | MEDLINE | ID: mdl-38673911

One of the most significant challenges in human health risk assessment is to evaluate hazards from exposure to environmental chemical mixtures. Polycyclic aromatic hydrocarbons (PAHs) are a class of ubiquitous contaminants typically found as mixtures in gaseous and particulate phases in ambient air pollution associated with petrochemicals from Superfund sites and the burning of fossil fuels. However, little is understood about how PAHs in mixtures contribute to toxicity in lung cells. To investigate mixture interactions and component additivity from environmentally relevant PAHs, two synthetic mixtures were created from PAHs identified in passive air samplers at a legacy creosote site impacted by wildfires. The primary human bronchial epithelial cells differentiated at the air-liquid interface were treated with PAH mixtures at environmentally relevant proportions and evaluated for the differential expression of transcriptional biomarkers related to xenobiotic metabolism, oxidative stress response, barrier integrity, and DNA damage response. Component additivity was evaluated across all endpoints using two independent action (IA) models with and without the scaling of components by toxic equivalence factors. Both IA models exhibited trends that were unlike the observed mixture response and generally underestimated the toxicity across dose suggesting the potential for non-additive interactions of components. Overall, this study provides an example of the usefulness of mixture toxicity assessment with the currently available methods while demonstrating the need for more complex yet interpretable mixture response evaluation methods for environmental samples.


Epithelial Cells , Polycyclic Aromatic Hydrocarbons , Humans , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/metabolism , Epithelial Cells/metabolism , Epithelial Cells/drug effects , Oxidative Stress/drug effects , DNA Damage/drug effects , Models, Biological , Air Pollutants/toxicity , Cells, Cultured , Bronchi/metabolism , Bronchi/cytology , Bronchi/drug effects , Biomarkers
6.
Chemosphere ; 356: 141931, 2024 May.
Article En | MEDLINE | ID: mdl-38614391

Chlorella vulgaris was cultivated for 15 days in 10 different treatments under mixotrophic and heterotrophic conditions, using wastewater from oil and poultry industries as the culture medium. The blends were made with produced water (PW), sterilized produced water (PWs), sterilized poultry wastewater (PoWs), sterilized seawater (SWs), and the addition of sodium nitrate to evaluate cell growth in treatments and the removal of PAHs. The heterotrophic condition showed more effective removal, having an initial concentration of 3.93 µg L-1 and a final concentration of 0.57 µg L-1 of total PAHs reporting 83%, during phycoremediation of (PW) than the mixotrophic condition, with an initial concentration of 3.93 µg L-1 and a final concentration of 1.96 and 43% removal for the PAHs. In the heterotrophic condition, the blend with (PWs + SWs) with an initial concentration of 0.90 µg L-1 and a final concentration of 0.32 µg L-1 had 64% removal of total PAHs compared to the mixotrophic condition with 37% removal having an initial concentration of 0.90 µg L-1 and a final concentration of 0.56 µg L-1. However, the best result in the mixotrophic condition was obtained using a blend of (PWs + PoWs) that had an initial cell concentration of 1.18 × 105 cells mL-1 and reached a final cell concentration of 4.39 × 105 cells mL-1, an initial concentration of 4.76 µg L-1 and a final concentration of 0.37 µg L-1 having a 92% total removal of PAHs. The biostimulation process increased the percentage of PAHs removal by 45% (PW) in the mixotrophic condition. This study showed that it is possible to allow an environmental remediation strategy that significantly reduces effluent toxicity and generates high value-added biomass in contaminated effluents rich in nutrients and carbon, based on a circular bioeconomy model.


Biodegradation, Environmental , Chlorella vulgaris , Microalgae , Polycyclic Aromatic Hydrocarbons , Wastewater , Water Pollutants, Chemical , Polycyclic Aromatic Hydrocarbons/metabolism , Chlorella vulgaris/metabolism , Chlorella vulgaris/growth & development , Water Pollutants, Chemical/metabolism , Wastewater/chemistry , Microalgae/metabolism , Heterotrophic Processes , Waste Disposal, Fluid/methods
7.
Fungal Biol ; 128(2): 1675-1683, 2024 Apr.
Article En | MEDLINE | ID: mdl-38575240

Polycyclic aromatic hydrocarbons (PAHs) are widely present in the environment, causing increasing concern because of their impact on soil health, food safety and potential health risks. Four bioremediation strategies were examined to assess the dissipation of PAHs in agricultural soil amended with sewage sludge over a period of 120 days: soil-sludge natural attenuation (SS); phytoremediation using maize (Zea mays L.) (PSS); mycoremediation (MR) separately using three white-rot fungi (Pleurotus ostreatus, Phanerochaete chrysosporium and Irpex lacteus); and plant-assisted mycoremediation (PMR) using a combination of maize and fungi. In the time frame of the experiment, mycoremediation using P. chrysosporium (MR-PH) exhibited a significantly higher (P < 0.05) degradation of total PAHs compared to the SS and PSS treatments, achieving a degradation rate of 52 %. Both the SS and PSS treatments demonstrated a lower degradation rate of total PAHs, with removal rates of 18 % and 32 %, respectively. The PMR treatments showed the highest removal rates of total PAHs at the end of the study, with degradation rates of 48-60 %. In the shoots of maize, only low- and medium-molecular-weight PAHs were found in both the PSS and PMR treatments. The calculated translocation and bioconversion factors always showed values < 1. The analysed enzymatic activities were higher in the PMR treatments compared to other treatments, which can be positively related to the higher degradation of PAHs in the soil.


Pleurotus , Polycyclic Aromatic Hydrocarbons , Soil Pollutants , Biodegradation, Environmental , Soil , Sewage , Polycyclic Aromatic Hydrocarbons/metabolism , Soil Pollutants/analysis , Soil Pollutants/metabolism , Pleurotus/metabolism , Zea mays
8.
Water Res ; 256: 121627, 2024 Jun 01.
Article En | MEDLINE | ID: mdl-38642539

The complex composition of coal chemical wastewater (CCW), marked by numerous highly toxic aromatic compounds, induces the destabilization of the biochemical treatment system, leading to suboptimal treatment efficacy. In this study, a biochemical treatment system was established to efficiently degrade aromatic compounds by quantitatively regulating the dosage of co-metabolized substrates (specifically, the chemical oxygen demand (COD) Glucose: COD Sodium acetate = 3:1, 1:3, and 1:1). The findings demonstrated that the system achieved optimal performance under the condition that the ratio of COD Glucose to COD Sodium acetate was 3:1. When the co-metabolized substrate was added to the system at an optimal ratio, examination of pollutant removal and cumulative effects revealed that the removal efficiencies for COD and total organic carbon (TOC) reached 94.61 % and 86.40 %, respectively. The removal rates of benzene series, nitrogen heterocyclic compounds, polycyclic aromatic hydrocarbons, and phenols were 100 %, 100 %, 63.58 %, and 94.12 %, respectively. Research on the physiological response of microbial cells showed that, under optimal ratio regulation, co-metabolic substrates led to a substantial rise in microbial extracellular polymeric substances (EPS) secretion, particularly extracellular proteins. When the system reached the end of its operation, the contents of loosely bound EPS (LB-EPS) and tightly bound EPS (TB-EPS) for proteins in the optimal group were 7.12 mg/g-SS and 152.28 mg/g-SS, respectively. Meanwhile, the ratio of α-Helix / (ß-Sheet + Random coil) and the proportion of intermolecular interaction forces were also increased in the optimal group. At system completion, the ratio of α-Helix / (ß-Sheet + Random coil) reached 0.717 (LB-EPS) and 0.618 (TB-EPS), respectively. Additionally, the proportion of intermolecular interaction forces reached 74.83 % (LB-EPS) and 55.03 % (TB-EPS). An in-depth analysis of the metabolic regulation of microorganisms indicated that the introduction of optimal ratios of co-metabolic substrates contributed to a noteworthy upregulation in the expression of Catechol 2,3-dioxygenase (C23O) and Dehydrogenase (DHA). The expression levels of C23O and DHA were measured at 0.029 U/mg Pro·g MLSS and 75.25 mg TF·(g MLSS·h)-1 (peak value), respectively. Correspondingly, enrichment of aromatic compound-degrading bacteria, including Thauera, Saccharimonadales, and Candidatus_Competibacter, occurred, along with the upregulation of associated functional genes such as Catechol 1,2-dioxygenase, Catechol 2,3-dioxygenase, Protocatechuate 3,4-dioxygenase, and Protocatechuate 4,5-dioxygenase. Considering the intricate system of multiple coexisting aromatic compounds in real CCW, this study not only obtained an optimal ratio for carbon source addition but also enhanced the efficient utilization of carbon sources and improved the capability of the system to effectively degrade aromatic compounds. Additionally, this paper established a theoretical foundation for metabolic regulation and harmless treatment within the biochemical treatment of intricate systems, exemplified by real CCW.


Biodegradation, Environmental , Carbon , Coal , Wastewater , Wastewater/chemistry , Carbon/metabolism , Waste Disposal, Fluid/methods , Water Pollutants, Chemical/metabolism , Biological Oxygen Demand Analysis , Polycyclic Aromatic Hydrocarbons/metabolism
9.
FEMS Microbiol Ecol ; 100(5)2024 Apr 10.
Article En | MEDLINE | ID: mdl-38650065

The overall impact of a crude oil spill into a pristine freshwater environment in Canada is largely unknown. To evaluate the impact on the native microbial community, a large-scale in situ model experimental spill was conducted to assess the potential role of the natural community to attenuate hydrocarbons. A small volume of conventional heavy crude oil (CHV) was introduced within contained mesocosm enclosures deployed on the shoreline of a freshwater lake. The oil was left to interact with the shoreline for 72 h and then free-floating oil was recovered using common oil spill response methods (i.e. freshwater flushing and capture on oleophilic absorptive media). Residual polycyclic aromatic hydrocarbon (PAH) concentrations returned to near preoiling concentrations within 2 months, while the microbial community composition across the water, soil, and sediment matrices of the enclosed oligotrophic freshwater ecosystems did not shift significantly over this period. Metagenomic analysis revealed key polycyclic aromatic and alkane degradation mechanisms also did not change in their relative abundance over the monitoring period. These trends suggest that for small spills (<2 l of oil per 15 m2 of surface freshwater), physical oil recovery reduces polycyclic aromatic hydrocarbon concentrations to levels tolerated by the native microbial community. Additionally, the native microbial community present in the monitored pristine freshwater ecosystem possesses the appropriate hydrocarbon degradation mechanisms without prior challenge by hydrocarbon substrates. This study corroborated trends found previously (Kharey et al. 2024) toward freshwater hydrocarbon degradation in an environmentally relevant scale and conditions on the tolerance of residual hydrocarbons in situ.


Ecosystem , Lakes , Petroleum Pollution , Petroleum , Polycyclic Aromatic Hydrocarbons , Water Pollutants, Chemical , Petroleum/metabolism , Lakes/microbiology , Polycyclic Aromatic Hydrocarbons/metabolism , Canada , Water Pollutants, Chemical/metabolism , Biodegradation, Environmental , Geologic Sediments/microbiology , Microbiota/drug effects , Bacteria/genetics , Bacteria/drug effects , Bacteria/metabolism , Bacteria/classification , Fresh Water/microbiology
10.
FEMS Microbiol Ecol ; 100(5)2024 Apr 10.
Article En | MEDLINE | ID: mdl-38650064

With the increase in crude oil transport throughout Canada, the potential for spills into freshwater ecosystems has increased and additional research is needed in these sensitive environments. Large enclosures erected in a lake were used as mesocosms for this controlled experimental dilbit (diluted bitumen) spill under ambient environmental conditions. The microbial response to dilbit, the efficacy of standard remediation protocols on different shoreline types commonly found in Canadian freshwater lakes, including a testing of a shoreline washing agent were all evaluated. We found that the native microbial community did not undergo any significant shifts in composition after exposure to dilbit or the ensuing remediation treatments. Regardless of the treatment, sample type (soil, sediment, or water), or type of associated shoreline, the community remained relatively consistent over a 3-month monitoring period. Following this, metagenomic analysis of polycyclic aromatic and alkane hydrocarbon degradation mechanisms also showed that while many key genes identified in PAH and alkane biodegradation were present, their abundance did not change significantly over the course of the experiment. These results showed that the native microbial community present in a pristine freshwater lake has the prerequisite mechanisms for hydrocarbon degradation in place, and combined with standard remediation practices in use in Canada, has the genetic potential and resilience to potentially undertake bioremediation.


Biodegradation, Environmental , Hydrocarbons , Lakes , Petroleum Pollution , Lakes/microbiology , Canada , Hydrocarbons/metabolism , Microbiota , Water Pollutants, Chemical/metabolism , Bacteria/genetics , Bacteria/metabolism , Bacteria/classification , Polycyclic Aromatic Hydrocarbons/metabolism , Geologic Sediments/microbiology , Fresh Water/microbiology , Metagenomics
11.
Chemosphere ; 353: 141635, 2024 Apr.
Article En | MEDLINE | ID: mdl-38447897

The performance of bacterial strains in executing degradative functions under the coexistence of heavy metals/heavy metal-like elements and organic contaminants is understudied. In this study, we isolated a fluorene-degrading bacterium, highly arsenic-resistant, designated as strain 2021, from contaminated soil at the abandoned site of an old coking plant. It was identified as a member of the genus Rhodococcus sp. strain 2021 exhibited efficient fluorene-degrading ability under optimal conditions of 400 mg/L fluorene, 30 °C, pH 7.0, and 250 mg/L trivalent arsenic. It was noted that the addition of arsenic could promote the growth of strain 2021 and improve the degradation of fluorene - a phenomenon that has not been described yet. The results further indicated that strain 2021 can oxidize As3+ to As5+; here, approximately 13.1% of As3+ was converted to As5+ after aerobic cultivation for 8 days at 30 °C. The addition of arsenic could greatly up-regulate the expression of arsR/A/B/C/D and pcaG/H gene clusters involved in arsenic resistance and aromatic hydrocarbon degradation; it also aided in maintaining the continuously high expression of cstA that codes for carbon starvation protein and prmA/B that codes for monooxygenase. These results suggest that strain 2021 holds great potential for the bioremediation of environments contaminated by a combination of arsenic and polycyclic aromatic hydrocarbons. This study provides new insights into the interactions among microbes, as well as inorganic and organic pollutants.


Arsenic , Polycyclic Aromatic Hydrocarbons , Rhodococcus , Soil Pollutants , Arsenic/metabolism , Rhodococcus/genetics , Rhodococcus/metabolism , Polycyclic Aromatic Hydrocarbons/metabolism , Fluorenes/metabolism , Biodegradation, Environmental , Soil Pollutants/metabolism , Soil Microbiology
12.
J Hazard Mater ; 470: 134109, 2024 May 15.
Article En | MEDLINE | ID: mdl-38547751

Polycyclic aromatic hydrocarbons (PAHs) are prevalent environmental contaminants that are harmful to ecological and human health. Bioremediation is a promising technique for remediating PAHs in the environment, however bioremediation often results in the accumulation of toxic PAH metabolites. The objectives of this research were to demonstrate the cometabolic treatment of a mixture of PAHs by a pure bacterial culture, Rhodococcus rhodochrous ATCC 21198, and investigate PAH metabolites and toxicity. Additionally, the surfactant Tween ® 80 and cell immobilization techniques were used to enhance bioremediation. Total PAH removal ranged from 70-95% for fluorene, 44-89% for phenanthrene, 86-97% for anthracene, and 6.5-78% for pyrene. Maximum removal was achieved with immobilized cells in the presence of Tween ® 80. Investigation of PAH metabolites produced by 21198 revealed a complex mixture of hydroxylated compounds, quinones, and ring-fission products. Toxicity appeared to increase after bioremediation, manifesting as mortality and developmental effects in embryonic zebrafish. 21198's ability to rapidly transform PAHs of a variety of molecular structures and sizes suggests that 21198 can be a valuable microorganism for catalyzing PAH remediation. However, implementing further treatment processes to address toxic PAH metabolites should be pursued to help lower post-remediation toxicity in future studies.


Biodegradation, Environmental , Cells, Immobilized , Polycyclic Aromatic Hydrocarbons , Rhodococcus , Surface-Active Agents , Zebrafish , Rhodococcus/metabolism , Surface-Active Agents/toxicity , Surface-Active Agents/chemistry , Surface-Active Agents/metabolism , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/chemistry , Polycyclic Aromatic Hydrocarbons/metabolism , Animals , Cells, Immobilized/metabolism , Polysorbates/toxicity , Polysorbates/chemistry , Environmental Pollutants/toxicity , Environmental Pollutants/metabolism , Environmental Pollutants/chemistry , Phenanthrenes/toxicity , Phenanthrenes/metabolism , Phenanthrenes/chemistry , Embryo, Nonmammalian/drug effects
13.
J Hazard Mater ; 470: 134122, 2024 May 15.
Article En | MEDLINE | ID: mdl-38552397

Polycyclic aromatic hydrocarbons (PAHs) are a class of toxic organic pollutants commonly detected in the aqueous phase. Traditional biodegradation is inefficient and advanced oxidation technologies are expensive. In the current study, a novel strategy was developed using calcium peroxide (CP) and PAH-degrading bacteria (PDB) to effectively augment PAH degradation by 28.62-59.22%. The PDB consisted of the genera Acinetobacter, Stenotrophomonas, and Comamonas. Applying the response surface model (RSM), the most appropriate parameters were identified, and the predictive degradation rates of phenanthrene (Phe), pyrene (Pyr), and ΣPAHs were 98%, 76%, and 84%, respectively. The constructed mixed system could reduce 90% of Phe and more than 60% of ΣPAHs and will perform better at pH 5-7 and lower salinity. Because PAHs tend to bind to dissolved organic matter (DOM) with larger molecular weights, humic acid (HA) had a larger negative effect on the PAH-degradation efficiency of the CP-PDB mixed system than fulvic acid (FA). The proposed PAH-degradation pathways in the mixed system were based on the detection of intermediates at different times. The investigation constructed and optimized a novel environmental PAH-degradation strategy. The synergistic application of PDB and oxidation was extended for organic contaminant degradation in aqueous environments.


Biodegradation, Environmental , Peroxides , Polycyclic Aromatic Hydrocarbons , Water Pollutants, Chemical , Peroxides/chemistry , Peroxides/metabolism , Water Pollutants, Chemical/metabolism , Water Pollutants, Chemical/chemistry , Polycyclic Aromatic Hydrocarbons/metabolism , Polycyclic Aromatic Hydrocarbons/chemistry , Bacteria/metabolism , Hydrogen-Ion Concentration
14.
Environ Sci Pollut Res Int ; 31(17): 25659-25670, 2024 Apr.
Article En | MEDLINE | ID: mdl-38483714

Polycyclic aromatic hydrocarbons (PAHs) were typical environmental contaminants that accumulated continuously in sediment. Microbial degradation is the main way of PAH degradation in the natural environment. Therefore, expanding the available pool of microbial resources and investigating the molecular degrading mechanisms of PAHs are critical to the efficient control of PAH-polluted sites. Here, a strain (identified as Xanthobacteraceae bacterium) with the ability to degrade pyrene was screened from the rhizosphere sediment of Vallisneria natans. Response surface analysis showed that the strain could degrade pyrene at pH 5-7, NaCl addition 0-1.5%, and temperature 25-40 °C, and the maximum pyrene degradation (~ 95.4%) was obtained under the optimum conditions (pH 7.0, temperature 28.5 °C, and NaCl-free addition) after 72 h. Also, it was observed that the effect of temperature on the degradation ratio was the most significant. Furthermore, eighteen metabolites were identified by mass spectrometry, among which (2Z)-2-hydroxy-3-(4-oxo-4H-phenalen-3-yl) prop-2-enoic acid, 7-(carboxymethyl)-8-formyl-1-naphthyl acetic acid, phthalic acid, naphthalene-1,2-diol, and phenol were the main metabolites. And the degradation pathway of pyrene was proposed, suggesting that pyrene undergoes initial ortho-cleavage under the catalysis of metapyrocatechase to form (2Z)-2-hydroxy-3-(4-oxo-4H-phenalen-3-yl) prop-2-enoic acid. Subsequently, this intermediate was progressively oxidized and degraded to phthalic acid or phenol, which could enter the tricarboxylic acid cycle. Furthermore, the pyrene biodegradation by the strain followed the first-order kinetic model and the degradation rate changed from fast to slow, with the rate remaining mostly slow in the later stages. The slow biodegradation rate was probably caused by a significant amount of phenol accumulation in the initial stage of degradation, which resulted in a decrease in bacterial activity or death.


Alphaproteobacteria , Phthalic Acids , Polycyclic Aromatic Hydrocarbons , Rhizosphere , Pyrenes/chemistry , Polycyclic Aromatic Hydrocarbons/metabolism , Bacteria/metabolism , Biodegradation, Environmental , Alphaproteobacteria/metabolism , Phenols
15.
Sci Total Environ ; 926: 171813, 2024 May 20.
Article En | MEDLINE | ID: mdl-38513868

Oil spills are a global challenge, contaminating the environment with organics and metals known to elicit toxic effects. Ecosystems within Nigeria's Niger Delta have suffered from prolonged severe spills for many decades but the level of impact on the soil microbial community structure and the potential for contaminant bioremediation remains unclear. Here, we assessed the extent/impact of an oil spill in this area 6 months after the accident on both the soil microbial community/diversity and the distribution of polycyclic aromatic hydrocarbon ring-hydroxylating dioxygenase (PAH-RHDGNα) genes, responsible for encoding enzymes involved in the degradation of PAHs, across the impacted area. Analyses confirmed the presence of oil contamination, including metals such as Cr and Ni, across the whole impacted area and at depth. The contamination impacted on the microbial community composition, resulting in a lower diversity in all contaminated soils. Gamma-, Delta-, Alpha- proteobacteria and Acidobacteriia dominated 16S rRNA gene sequences across the contaminated area, while Ktedonobacteria dominated the non-contaminated soils. The PAH-RHDαGN genes were only detected in the contaminated area, highlighting a clear relationship with the oil contamination/hydrocarbon metabolism. Correlation analysis indicated significant positive relationships between the oil contaminants (organics, Cr and Ni), PAH-RHDαGN gene, and the presence of bacteria/archaea such as Anaerolinea, Spirochaetia Bacteroidia Thermoplasmata, Methanomicrobia, and Methanobacteria indicating that the oil contamination not only impacted the microbial community/diversity present, but that the microbes across the impacted area and at depth were potentially playing an important role in degrading the oil contamination present. These findings provide new insights on the level of oil contamination remaining 6 months after an oil spill, its impacts on indigenous soil microbial communities and their potential for in situ bioremediation within a Niger Delta's ecosystem. It highlights the strength of using a cross-disciplinary approach to assess the extent of oil pollution in a single study.


Alphaproteobacteria , Microbiota , Polycyclic Aromatic Hydrocarbons , Soil Pollutants , Soil , RNA, Ribosomal, 16S/genetics , Niger , Bacteria/metabolism , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/metabolism , Alphaproteobacteria/genetics , Soil Microbiology , Soil Pollutants/toxicity , Soil Pollutants/metabolism , Biodegradation, Environmental
16.
Chemosphere ; 354: 141705, 2024 Apr.
Article En | MEDLINE | ID: mdl-38494000

Benzo[a]pyrene (BaP), as the typical representative of polycyclic aromatic hydrocarbons (PAHs), is a serious hazard to human health and natural environments. Though the study of microbial degradation of PAHs has persisted for decades, the degradation pathway of BaP is still unclear. Previously, Pontibacillus chungwhensis HN14 was isolated from high salinity environment exhibiting a high BaP degradation ability. Here, based on the intermediates identified, BaP was found to be transformed to 4,5-epoxide-BaP, BaP-trans-4,5-dihydrodiol, 1,2-dihydroxy-phenanthrene, 2-carboxy-1-naphthol, and 4,5-dimethoxybenzo[a]pyrene by the strain HN14. Furthermore, functional genes involved in degradation of BaP were identified using genome and transcriptome data. Heterogeneous co-expression of monooxygenase CYP102(HN14) and epoxide hydrolase EH(HN14) suggested that CYP102(HN14) could transform BaP to 4,5-epoxide-BaP, which was further transformed to BaP-trans-4,5-dihydrodiol by EH(HN14). Moreover, gene cyp102(HN14) knockout was performed using CRISPR/Cas9 gene-editing system which confirmed that CYP102(HN14) play a key role in the initial conversion of BaP. Finally, a novel BaP degradation pathway was constructed in bacteria, which showed BaP could be converted into chrysene, phenanthrene, naphthalene pathways for the first time. These findings enhanced our understanding of microbial degradation process for BaP and suggested the potential of using P. chungwhensis HN14 for bioremediation in PAH-contaminated environments.


Bacillaceae , Naphthalenes , Phenanthrenes , Polycyclic Aromatic Hydrocarbons , Humans , Benzo(a)pyrene/metabolism , Biodegradation, Environmental , Polycyclic Aromatic Hydrocarbons/metabolism , Epoxy Compounds
17.
Sci Total Environ ; 924: 171449, 2024 May 10.
Article En | MEDLINE | ID: mdl-38460699

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous organic compounds in the environment. They are produced by many anthropogenic sources of different origins and are known for their toxicity, carcinogenicity, and mutagenicity. Sixteen PAHs have been identified as Priority Pollutants by the US EPA, which are often associated with particulate matter, facilitating their dispersion through air and water. When human skin is exposed to PAHs, it might occur simultaneously with solar radiation, potentially leading to phototoxic effects. Phototoxic mechanisms involve the generation of singlet oxygen and reactive oxygen species, DNA damage under specific light wavelengths, and the formation of charge transfer complexes. Despite predictions of phototoxic properties for some PAHs, there remains a paucity of experimental data. This study examined the photoreactive and phototoxic properties of the 16 PAHs enlisted in the Priority Pollutants list. Examined PAHs efficiently photogenerated singlet oxygen and superoxide anion in simple solutions. Furthermore, singlet oxygen phosphorescence was detected in PAH-loaded HaCaT cells. Phototoxicity against human keratinocytes was evaluated using various assays. At 5 nM concentration, examined PAHs significantly reduced viability and mitochondrial membrane potential of HaCaT cells following the exposure to solar simulated light. Analyzed compounds induced a substantial peroxidation of cellular proteins after light treatment. The results revealed that a majority of the examined PAHs exhibited substantial reactive oxygen species photoproduction under UVA and violet-blue light, with their phototoxicity corresponding to their photoreactive properties. These findings improve our comprehension of the interactions between PAHs and human skin cells under environmental conditions, particularly when exposed to solar radiation.


Environmental Pollutants , Polycyclic Aromatic Hydrocarbons , Humans , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/metabolism , Ultraviolet Rays , Reactive Oxygen Species/metabolism , Singlet Oxygen/pharmacology , Keratinocytes/metabolism , Keratinocytes/radiation effects , Environmental Pollutants/toxicity
18.
Environ Pollut ; 347: 123710, 2024 Apr 15.
Article En | MEDLINE | ID: mdl-38458518

There is a lack of knowledge on the biodegradation mechanisms of benzene and benzo [a]pyrene (BaP), representative compounds of polycyclic aromatic hydrocarbons (PAHs), and benzene, toluene, ethylbenzene, and xylene (BTEX), under individually and mixed contaminated soils. Therefore, a set of microcosm experiments were conducted to explore the influence of benzene and BaP on biodegradation under individual and mixed contaminated condition, and their subsequent influence on native microbial consortium. The results revealed that the total mass loss of benzene was 56.0% under benzene and BaP mixed contamination, which was less than that of individual benzene contamination (78.3%). On the other hand, the mass loss of BaP was slightly boosted to 17.6% under the condition of benzene mixed contamination with BaP from that of individual BaP contamination (14.4%). The significant differences between the microbial and biocide treatments for both benzene and BaP removal demonstrated that microbial degradation played a crucial role in the mass loss for both contaminants. In addition, the microbial analyses revealed that the contamination of benzene played a major role in the fluctuations of microbial compositions under co-contaminated conditions. Rhodococcus, Nocardioides, Gailla, and norank_c_Gitt-GS-136 performed a major role in benzene biodegradation under individual and mixed contaminated conditions while Rhodococcus, Noviherbaspirillum, and Phenylobacterium were highly involved in BaP biodegradation. Moreover, binary benzene and BaP contamination highly reduced the Rhodococcus abundance, indicating the toxic influence of co-contamination on the functional key genus. Enzymatic activities revealed that catalase, lipase, and dehydrogenase activities proliferated while polyphenol oxidase was reduced with contamination compared to the control treatment. These results provided the fundamental information to facilitate the development of more efficient bioremediation strategies, which can be tailored to specific remediation of different contamination scenarios.


Polycyclic Aromatic Hydrocarbons , Soil Pollutants , Biodegradation, Environmental , Benzene/metabolism , Benzo(a)pyrene/metabolism , Toluene/metabolism , Polycyclic Aromatic Hydrocarbons/metabolism , Soil , Soil Pollutants/metabolism , Soil Microbiology
19.
Chem Biol Interact ; 393: 110950, 2024 Apr 25.
Article En | MEDLINE | ID: mdl-38479715

It is well known that anthracene is a persistent organic pollutant. Among the four natural polycyclic aromatic hydrocarbons (PAHs) degrading strains, Comamonas testosterone (CT1) was selected as the strain with the highest degradation efficiency. In the present study, prokaryotic transcriptome analysis of CT1 revealed an increase in a gene that encodes tryptophane-2,3-dioxygenase (T23D) in the anthracene and erythromycin groups compared to CK. Compared to the wild-type CT1 strain, anthracene degradation by the CtT23D knockout mutant (CT-M1) was significantly reduced. Compared to Escherichia coli (DH5α), CtT23D transformed DH5α (EC-M1) had a higher degradation efficiency for anthracene. The recombinant protein rT23D oxidized tryptophan at pH 7.0 and 37 °C with an enzyme activity of 2.42 ± 0.06 µmol min-1·mg-1 protein. In addition, gas chromatography-mass (GC-MS) analysis of anthracene degradation by EC-M1 and the purified rT23D revealed that 2-methyl-1-benzofuran-3-carbaldehyde is an anthracene metabolite, suggesting that it is a new pathway.


Comamonas testosteroni , Dioxygenases , Polycyclic Aromatic Hydrocarbons , Comamonas testosteroni/genetics , Dioxygenases/metabolism , Tryptophan , Anthracenes , Polycyclic Aromatic Hydrocarbons/metabolism
20.
Chemosphere ; 356: 141795, 2024 May.
Article En | MEDLINE | ID: mdl-38548078

Nitrated polycyclic aromatic hydrocarbons (nitro-PAHs) are persistent pollutants that have been introduced into the environment as a result of human activities. They are produced when PAHs undergo oxidation and are highly resistant to degradation, resulting in prolonged exposure and significant health risks for wildlife and humans. Nitro-PAHs' potential to induce cancer and mutations has raised concerns about their harmful effects. Furthermore, their ability to accumulate in the food chain seriously threatens the ecosystem and human health. Moreover, nitro-PAHs can disrupt the normal functioning of the endocrine system, leading to reproductive and developmental problems in humans and other organisms. Reducing nitro-PAHs in the environment through source management, physical removal, and chemical treatment is essential to mitigate the associated environmental and human health risks. Recent studies have focused on improving nitro-PAHs' phytoremediation by incorporating microorganisms and biostimulants. Microbes can break down nitro-PAHs into less harmful substances, while biostimulants can enhance plant growth and metabolic activity. By combining these elements, the effectiveness of phytoremediation for nitro-PAHs can be increased. This study aimed to investigate the impact of introducing microbial and biostimulant agents on the phytoremediation process for nitro-PAHs and identify potential solutions for addressing the environmental risks associated with these pollutants.


Biodegradation, Environmental , Environmental Restoration and Remediation , Polycyclic Aromatic Hydrocarbons , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/metabolism , Environmental Restoration and Remediation/methods , Humans , Ecosystem , Nitro Compounds/toxicity
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