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1.
Water Sci Technol ; 89(10): 2716-2731, 2024 May.
Article En | MEDLINE | ID: mdl-38822610

The anaerobic biodegradation of polycyclic aromatic hydrocarbons (PAHs) is challenging due to its toxic effect on the microbes. Microbial electrolysis cells (MECs), with their excellent characteristics of anodic and cathodic biofilms, can be a viable way to enhance the biodegradation of PAHs. This work assessed different cathode materials (carbon brush and nickel foam) combined with bioaugmentation on typical PAHs-naphthalene biodegradation and analyzed the inhibition amendment mechanism of microbial biofilms in MECs. Compared with the control, the degradation efficiency of naphthalene with the nickel foam cathode supplied with bioaugmentation dosage realized a maximum removal rate of 94.5 ± 3.2%. The highest daily recovered methane yield (227 ± 2 mL/gCOD) was also found in the nickel foam cathode supplied with bioaugmentation. Moreover, the microbial analysis demonstrated the significant switch of predominant PAH-degrading microorganisms from Pseudomonas in control to norank_f_Prolixibacteraceae in MECs. Furthermore, hydrogentrophic methanogenesis prevailed in MEC reactors, which is responsible for methane production. This study proved that MEC combined with bioaugmentation could effectively alleviate the inhibition of PAH, with the nickel foam cathode obtaining the fastest recovery rate in terms of methane yield.


Biodegradation, Environmental , Electrolysis , Polycyclic Aromatic Hydrocarbons , Wastewater , Water Pollutants, Chemical , Polycyclic Aromatic Hydrocarbons/metabolism , Polycyclic Aromatic Hydrocarbons/chemistry , Wastewater/chemistry , Water Pollutants, Chemical/metabolism , Water Pollutants, Chemical/chemistry , Waste Disposal, Fluid/methods , Bioreactors , Bacteria/metabolism , Electrodes , Biofilms
2.
Chemosphere ; 358: 142171, 2024 Jun.
Article En | MEDLINE | ID: mdl-38714247

Marine oil spills directly cause polycyclic aromatic hydrocarbons (PAHs) pollution and affect marine organisms due to their toxic property. Chemical and bio-based dispersants composed of surfactants and solvents are considered effective oil spill-treating agents. Dispersants enhance oil biodegradation in the marine environment by rapidly increasing their solubility in the water column. However, the effect of dispersants, especially surfactants, on PAHs degradation by enzymes produced by microorganisms has not been studied at the molecular level. The role of the cytochrome P450 (CYP) enzyme in converting contaminants into reactive metabolites during the biodegradation process has been evidenced, but the activity in the presence of surfactants is still ambiguous. Thus, this study focused on the evaluation of the impact of chemical and bio-surfactants (i.e., Tween 80 (TWE) and Surfactin (SUC)) on the biodegradation of naphthalene (NAP), chrysene (CHR), and pyrene (PYR), the representative components of PAHs, with CYP enzyme from microalgae Parachlorella kessleri using molecular docking and molecular dynamics (MD) simulation. The molecular docking analysis revealed that PAHs bound to residues at the CYP active site through hydrophobic interactions for biodegradation. The MD simulation showed that the surfactant addition changed the enzyme conformation in the CYP-PAH complexes to provide more interactions between the enzyme and PAHs. This led to an increase in the enzyme's capability to degrade PAHs. Binding free energy (ΔG||Bind) calculations confirmed that surfactant treatment could enhance PAHs degradation by the enzyme. The SUC gave a better result on NAP and PYR biodegradation based on ΔG||Bind, while TWE facilitated the biodegradation of CHR. The research outputs could greatly facilitate evaluating the behaviors of oil spill-treating agents and oil spill response operations in the marine environment.


Biodegradation, Environmental , Molecular Docking Simulation , Molecular Dynamics Simulation , Petroleum Pollution , Polycyclic Aromatic Hydrocarbons , Surface-Active Agents , Water Pollutants, Chemical , Polycyclic Aromatic Hydrocarbons/metabolism , Polycyclic Aromatic Hydrocarbons/chemistry , Surface-Active Agents/chemistry , Surface-Active Agents/metabolism , Water Pollutants, Chemical/metabolism , Water Pollutants, Chemical/chemistry , Cytochrome P-450 Enzyme System/metabolism , Chlorophyta/metabolism
3.
Int J Mol Sci ; 25(10)2024 May 17.
Article En | MEDLINE | ID: mdl-38791537

Many years of foundry practice and much more accurate analytical methods have shown that sands with organic binders, in addition to their many technological advantages, pose risks associated with the emission of many compounds, including harmful ones (e.g., formaldehyde, phenol, benzene, polycyclic aromatic hydrocarbons, and sulfur), arising during the pouring of liquid casting alloys into molds, their cooling, and knock-out. The aim of this research is to demonstrate the potential benefits of adopting inorganic binders in European iron foundries. This will improve the environmental and working conditions by introducing cleaner and more ecological production methods, while also ranking the tested binders studied in terms of their harmful content. The article pays special attention to the analysis of seven innovative inorganic binders and one organic binder, acting as a reference for emissions of gases from the BTEX (benzene, toluene, ethylbenzene, and xylenes) and PAHs (polycyclic aromatic hydrocarbons) groups and other compounds such as phenol, formaldehyde, and isocyanates (MDI and TDI) generated during the mold pouring process with liquid metals. The knowledge gained will, for the first time, enrich the database needed to update the Reference Document on The Best Available Techniques for the Smitheries and Foundries Industry (SF BREF).


Polycyclic Aromatic Hydrocarbons , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Inorganic Chemicals/chemistry , Metallurgy , Formaldehyde/chemistry
4.
J Hazard Mater ; 471: 134467, 2024 Jun 05.
Article En | MEDLINE | ID: mdl-38691930

The beneficial roles of hydrochar in carbon sequestration and soil improvement are widely accepted. Despite few available reports regarding polycyclic aromatic hydrocarbons (PAHs) generated during preparation, their potential negative impacts on ecosystems remain a concern. A heating treatment method was employed in this study for rapidly removing PAHs and reducing the toxicity of corn stover-based hydrochar (CHC). The result showed total PAHs content (∑PAH) decreased and then sharply increased within the temperature range from 150 °C to 400 °C. The ∑PAH and related toxicity in CHC decreased by more than 80% under 200 °C heating temperature, compared with those in the untreated sample, representing the lowest microbial toxicity. Benzo(a)pyrene produced a significant influence on the ecological toxicity of the hydrochar among the 16 types of PAHs. The impact of thermal treatment on the composition, content, and toxicity of PAHs was significantly influenced by the adsorption, migration, and desorption of PAHs within hydrochar pores, as well as the disintegration and aggregation of large molecular polymers. The combination of hydrochar with carbonized waste heat and exhaust gas collection could be a promising method to efficiently and affordably reduce hydrochar ecological toxicity.


Hot Temperature , Polycyclic Aromatic Hydrocarbons , Soil Pollutants , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/chemistry , Soil Pollutants/toxicity , Soil Pollutants/chemistry , Charcoal/chemistry , Zea mays , Soil/chemistry , Adsorption , Heating
5.
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
6.
Chemosphere ; 359: 142248, 2024 Jul.
Article En | MEDLINE | ID: mdl-38710412

PAHs is the group of emerging micro-pollutants present in most environmental matrices that has the tendency to bioaccumulate and cause carcinogenic effects to human health. The present research involved the quantification and treatment of leachate produced from secured landfill, to eliminate the PAHS. Electro-Fenton process, a class of advanced oxidation process, is adopted to degrade the PAHs using titanium electrodes as both anode and cathode. Artificial intelligence based statistical tool "Central Composite Design" a module of JMP -19 software was used to design the experiments and optimize the critical parameters involved in the research. It was observed that the value of P is significant (P < 0.05) for all the independent variables evidencing the significant correlation between experimental values and predicted values of the software. The value of R2 obtained was 0.96 and 0.97 for COD and PAHs respectively. The maximum removal efficiency of COD and PAH was found to be 84.24% and 90.78% respectively. The optimized conditions obtained from the central composite design were: pH = 5; Fe2+ = 0.1 g/L; H2O2 = 2 g/L; reaction time = 60 min; and electric intensity = 0.2 A. Additionally, optimized experimental conditions were used to study the removal efficiencies of individual 16 PAHs and are also reported. From the close proximity of experimental and predicted results of the software it can be proved that central composite design is efficient enough to be used as a statistical tool in design and analysis for treatment of landfill leachate.


Environmental Restoration and Remediation , Hydrogen Peroxide , Iron , Polycyclic Aromatic Hydrocarbons , Water Pollutants, Chemical , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Polycyclic Aromatic Hydrocarbons/analysis , Hydrogen Peroxide/chemistry , Environmental Restoration and Remediation/methods , Iron/chemistry , Oxidation-Reduction , Carcinogens/chemistry , Carcinogens/analysis , Waste Disposal Facilities , Electrodes , Hydrogen-Ion Concentration
7.
Int J Biol Macromol ; 270(Pt 1): 132294, 2024 Jun.
Article En | MEDLINE | ID: mdl-38735602

Polycyclic aromatic hydrocarbons (PAHs) are molecules with two or more fused aromatic rings that occur naturally in the environment due to incomplete combustion of organic substances. However, the increased demand for fossil fuels in recent years has increased anthropogenic activity, contributing to the environmental concentration of PAHs. The enzyme chlorocatechol 1,2-dioxygenase from Pseudomonas putida (Pp 1,2-CCD) is responsible for the breakdown of the aromatic ring of catechol, making it a potential player in bioremediation strategies. Pp 1,2-CCD can tolerate a broader range of substrates, including halogenated compounds, than other dioxygenases. Here, we report the construction of a chimera protein able to form biomolecular condensates with potential application in bioremediation. The chimera protein was built by conjugating Pp 1,2-CCD to low complex domains (LCDs) derived from the DEAD-box protein Dhh1. We showed that the chimera could undergo liquid-liquid phase separation (LLPS), forming a protein-rich liquid droplet under different conditions (variable protein and PEG8000 concentrations and pH values), in which the protein maintained its structure and main biophysical properties. The condensates were active against 4-chlorocatechol, showing that the chimera droplets preserved the enzymatic activity of the native protein. Therefore, it constitutes a prototype of a microreactor with potential use in bioremediation.


Biodegradation, Environmental , Dioxygenases , Polycyclic Aromatic Hydrocarbons , Dioxygenases/metabolism , Dioxygenases/chemistry , Polycyclic Aromatic Hydrocarbons/chemistry , Polycyclic Aromatic Hydrocarbons/metabolism , Pseudomonas putida/enzymology , Catechols/metabolism , Catechols/chemistry , Bacterial Proteins/chemistry , Bacterial Proteins/metabolism
8.
Chemosphere ; 359: 142348, 2024 Jul.
Article En | MEDLINE | ID: mdl-38759803

Efficient remediation of soil contaminated by polycyclic aromatic hydrocarbons (PAHs) is challenging. To determine whether soil ecoenzyme stoichiometry influences PAH degradation under biostimulation and bioaugmentation, this study initially characterized soil ecoenzyme stoichiometry via a PAH degradation experiment and subsequently designed a validation experiment to answer this question. The results showed that inoculation of PAH degradation consortia ZY-PHE plus vanillate efficiently degraded phenanthrene with a K value of 0.471 (depending on first-order kinetics), followed by treatment with ZY-PHE and control. Ecoenzyme stoichiometry data revealed that the EEAC:N, vector length and angle increased before day five and decreased during the degradation process. In contrast, EEAN:P decreased and then increased. These results indicated that the rapid PAH degradation period induced more C limitation and organic P mineralization. Correlation analysis indicated that the degradation rate K was negatively correlated with vector length, EEAC:P, and EEAN:P, suggesting that C limitation and relatively less efficient P mineralization could inhibit biodegradation. Therefore, incorporating liable carbon and acid phosphatase or soluble P promoted PAH degradation in soils with ZY-PHE. This study provides novel insights into the relationship between soil ecoenzyme stoichiometry and PAH degradation. It is suggested that soil ecoenzyme stoichiometry be evaluated before designing bioremeiation stragtegies for PAH contanminated soils.


Biodegradation, Environmental , Polycyclic Aromatic Hydrocarbons , Soil Microbiology , Soil Pollutants , Soil , Polycyclic Aromatic Hydrocarbons/metabolism , Polycyclic Aromatic Hydrocarbons/chemistry , Soil Pollutants/metabolism , Soil/chemistry , Phenanthrenes/metabolism , Kinetics
9.
Environ Res ; 253: 119124, 2024 Jul 15.
Article En | MEDLINE | ID: mdl-38734294

Polyaromatic hydrocarbons (PAHs) are the most persistent compounds that get contaminated in the soil and water. Nearly 16 PAHs was considered to be a very toxic according US protection Agency. Though its concentration level is low in the environments but the effects due to it, is enormous. Advanced Oxidation Process (AOP) is an emergent methodology towards treating such pollutants with low and high molecular weight of complex substances. In this study, sulfate radical (SO4‾•) based AOP is emphasized for purging PAH from different sources. This review essentially concentrated on the mechanism of SO4‾• for the remediation of pollutants from different sources and the effects caused due to these pollutants in the environment was reduced by this mechanism is revealed in this review. It also talks about the SO4‾• precursors like Peroxymonosulfate (PMS) and Persulfate (PS) and their active participation in treating the different sources of toxic pollutants. Though PS and PMS is used for removing different contaminants, the degradation of PAH due to SO4‾• was presented particularly. The hydroxyl radical (•OH) mechanism-based methods are also emphasized in this review along with their limitations. In addition to that, different activation methods of PS and PMS were discussed which highlighted the performance of transition metals in activation. Also this review opened up about the degradation efficiency of contaminants, which was mostly higher than 90% where transition metals were used for activation. Especially, on usage of nanoparticles even 100% of degradation could be able to achieve was clearly showed in this literature study. This study mainly proposed the treatment of PAH present in the soil and water using SO4‾• with different activation methodologies. Particularly, it emphasized about the importance of treating the PAH to overcome the risk associated with the environment and humans due to its contamination.


Environmental Restoration and Remediation , Oxidation-Reduction , Polycyclic Aromatic Hydrocarbons , Sulfates , Sulfates/chemistry , Sulfates/analysis , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Environmental Restoration and Remediation/methods , Environmental Pollutants/chemistry , Environmental Pollutants/analysis
10.
Environ Res ; 255: 119118, 2024 Aug 15.
Article En | MEDLINE | ID: mdl-38763278

Polycyclic aromatic hydrocarbons (PAH) are persistent environmental pollutants, which occasionally appear as contaminants in consumer products. Upon dermal contact, transfer of PAH into the stratum corneum (s.c.) and migration through the skin may occur, resulting in this class of highly toxic compounds to become bioavailable. In this study, dermal penetration through human and porcine skin of 24 PAH, comprising broad molar mass (M: 152-302 g/mol) and octanol-water partition coefficient (logP: 3.9-7.3) ranges, was evaluated via Franz diffusion cell in vitro assays. More lipophilic and potentially more toxic PAH had decreased permeation rates through the rather lipophilic s.c. into the more hydrophilic viable (epi-)dermis. Furthermore, human skin was less permeable than pigskin, a commonly used surrogate in skin penetration studies. In particular, the s.c. of human skin retains a greater share of PAH, an effect that is more pronounced for smaller PAH. Additionally, we compared the skin permeation kinetics of different PAH in pigskin. While small PAH (M < 230 g/mol, logP < 6) permeate the skin quickly and are detected in the receptor fluid after 2 h, large PAH (M > 252 g/mol, logP ≥ 6) do not fully permeate the skin up to 48 h. This indicates that highly lipophilic PAH do not become bioavailable as readily as their smaller congeners when transferred to the skin surface. Our data suggest that pigskin could be used as a surrogate for worst case scenario estimates of dermal PAH permeation through human skin.


Polycyclic Aromatic Hydrocarbons , Skin Absorption , Skin , Polycyclic Aromatic Hydrocarbons/pharmacokinetics , Polycyclic Aromatic Hydrocarbons/metabolism , Polycyclic Aromatic Hydrocarbons/chemistry , Humans , Animals , Swine , Skin/metabolism , Permeability , In Vitro Techniques , Female , Adult
11.
Chemosphere ; 360: 142384, 2024 Jul.
Article En | MEDLINE | ID: mdl-38797205

Interactions between polycyclic aromatic hydrocarbons (PAHs) and titanium dioxide (TiO2) nanoparticles (NPs) can produce unforeseen photoproducts in the aqueous phase. Both PAHs and TiO2-NPs are well-studied and highly persistent environmental pollutants, but the consequences of PAH-TiO2-NP interactions are rarely explored. We investigated PAH photoproduct formation over time for benzo[a]pyrene (BaP), fluoranthene (FLT), and pyrene (PYR) in the presence of ultraviolet A (UVA) using a combination of analytical and computational methods including, identification of PAH photoproducts, assessment of expression profiles for gene indicators of PAH metabolism, and computational evaluation of the reaction mechanisms through which certain photoproducts might be formed. Chemical analyses identified diverse photoproducts, but all PAHs shared a primary photoproduct, 9,10-phenanthraquinone (9,10-PQ), regardless of TiO2-NP presence. The computed reaction mechanisms revealed the roles photodissociation and singlet oxygen chemistry likely play in PAH mediated photochemical processes that result in the congruent production of 9,10-PQ within this study. Our investigation of PAH photoproduct formation has provided substantial evidence of the many, diverse and congruent, photoproducts formed from physicochemically distinct PAHs and how TiO2-NPs influence bioavailability and time-related formation of PAH photoproducts.


Nanoparticles , Photochemical Processes , Polycyclic Aromatic Hydrocarbons , Titanium , Ultraviolet Rays , Titanium/chemistry , Polycyclic Aromatic Hydrocarbons/chemistry , Nanoparticles/chemistry , Fluorenes/chemistry , Pyrenes/chemistry , Benzo(a)pyrene/chemistry , Environmental Pollutants/chemistry , Biological Availability
12.
Chemosphere ; 360: 142454, 2024 Jul.
Article En | MEDLINE | ID: mdl-38810801

The aim of the present study was to find environmentally friendly solutions for the disposal of problematic and toxic textile sludge (TS) by producing textile sludge biochar (TSB) by pyrolysis and evaluating its chemical properties, polycyclic aromatic hydrocarbon (PAH) content, heavy metals (HMs) speciation, environmental risks, and effects on seed germination. Pyrolysis of TS at temperatures ranging from 300 to 700 °C significantly reduced (85-95%) or eliminated certain PAHs in the biochar, enriched heavy metal content within land use limits, and increased bioavailability of HMs in biochar produced at 300 °C and decreased leaching capacity of HMs in biochar produced at 700 °C. The speciation of HMs and their bioavailability during pyrolysis processes was strongly temperature dependent, with lower temperatures increasing the toxic and bioavailable forms of Zn and Ni, while higher temperatures converted the bioavailable Ni to a more stable form, while Cu, Cr, and Pb were transformed from stable to toxic and bioavailable forms. The ecological risk index (RI) values of TSB-300 and TSB-700 are below the threshold value of 150, indicating a low-risk level, and the risk level decreases at temperatures above 500 °C. Further, the extracts of TSB-300 and TSB-700 had the highest percentage of germinating seeds, while the extracts of TS and TSB-500 inhibited seed germination by 20-30% compared to the control. These results indicate that pyrolysis effectively reduces PAHs and binds leachable HMs in biochar, however, the specific pyrolysis temperature influences metal speciation, bioavailability, seed germination, and environmental risk.


Charcoal , Metals, Heavy , Polycyclic Aromatic Hydrocarbons , Pyrolysis , Sewage , Temperature , Metals, Heavy/analysis , Metals, Heavy/chemistry , Charcoal/chemistry , Sewage/chemistry , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Textiles , Germination/drug effects , Industrial Waste
13.
J Environ Manage ; 359: 120984, 2024 May.
Article En | MEDLINE | ID: mdl-38678905

The chronic lack of effective disposal of pollutants has resulted in the detection of a wide variety of EPs in the environment, with concentrations high enough to affect ecological health. Laccase, as a versatile oxidase capable of catalyzing a wide range of substrates and without producing toxic by-products, is a potential candidate for the biodegradation of pollutants. Immobilization can provide favorable protection for free laccase, improve the stability of laccase in complex environments, and greatly enhance the reusability of laccase, which is significant in reducing the cost of industrial applications. This study introduces the properties of laccase and subsequently elaborate on the different support materials for laccase immobilization. The research advances in the degradation of EDs, PPCPs, and PAHs by immobilized laccase are then reviewed. This review provides a comprehensive understanding of laccase immobilization, as well as the advantages of various support materials, facilitating the development of more economical and efficient immobilization systems that can be put into practice to achieve the green degradation of EPs.


Biodegradation, Environmental , Enzymes, Immobilized , Laccase , Laccase/metabolism , Enzymes, Immobilized/metabolism , Enzymes, Immobilized/chemistry , Environmental Pollutants/metabolism , Polycyclic Aromatic Hydrocarbons/chemistry , Polycyclic Aromatic Hydrocarbons/metabolism
14.
Waste Manag ; 182: 21-31, 2024 Jun 15.
Article En | MEDLINE | ID: mdl-38631177

This research investigates the formation mechanism of soot and particulate matter during the pyrolysis and gasification of waste derived from Municipal Solid Waste (MSW) in a laboratory scale drop tube furnace. Compared with CO2 gasification atmosphere, more ultrafine particles (PM0.2, aerodynamic diameter less than 0.2 µm) were generated in N2 atmosphere at 1200℃, which were mainly composed of polycyclic aromatic hydrocarbons (PAHs), graphitic carbonaceous soot and volatile alkali salts. High reaction temperatures promote the formation of hydrocarbon gaseous products and their conversion to PAHs, which ultimately leads to the formation of soot particles. The soot particles generated by waste derived from MSW pyrolysis and gasification both have high specific surface area and well-developed pore structure. Compared with pyrolysis, the soot generated by gasification of waste derived from MSW had smaller size and higher proportion of inorganic components. The higher pyrolysis temperature led to the collapse of the mesoporous structure of submicron particles, resulting in a decrease in total pore volume and an increase in specific surface area. Innovatively, this research provides an explanation for the effect of reaction temperature/ CO2 on the formation pathways and physicochemical properties of soot and fine particulate matter.


Hot Temperature , Particulate Matter , Pyrolysis , Solid Waste , Soot , Particulate Matter/analysis , Particulate Matter/chemistry , Solid Waste/analysis , Soot/analysis , Soot/chemistry , Refuse Disposal/methods , Incineration/methods , Carbon Dioxide/analysis , Carbon Dioxide/chemistry , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Particle Size
15.
J Chromatogr A ; 1722: 464889, 2024 May 10.
Article En | MEDLINE | ID: mdl-38598894

In this paper, three imidazole- and C18- bifunctional silica stationary phases (Sil-Im-C18) were prepared by adjusting introduction interval of octadecyltrichlorosilane (ODS) and 3-imidazol-1-ylpropyl(trimethoxy)silane (TMPImS), which can be used for reversed-phase liquid chromatography (RPLC) and ion exchange chromatography (IEC) with adjustable performance. The successful preparation of Sil-Im-C18 were confirmed by the characterizations of elemental analysis, infrared spectroscopy (FTIR) and contact angle (CA). Chromatographic performance of Sil-Im-C18 were evaluated by the separation of Tanaka test mixture, alkylbenzenes, linear PAHs and a set of analytes with different properties (uracil, phenol, 1,2-dinitrobenzene and naphthalene), and compared with commonly used C18 column. It was found that the chromatographic performance of Sil-Im-C18 changed significantly with the difference in bonding amount of imidazole and C18. Sil-Im-C18 demonstrated the excellent separation performance towards polycyclic aromatic hydrocarbons (PAHs), phenylesters, phenylamines, phenols and inorganic anions, and notably, nucleobases and nucleosides can be separated using pure water as mobile phases. The van Deemter plot showed that the column efficiency of Sil-Im-C18-3 was 64,933 plate·m-1 for naphthalene, indicated that Sil-Im-C18 was reasonably chromatographic columns. The RSD values of retention time were 0.22 %-0.61 % for 10 needles alkylbenzenes injected continuously at 50 °C to investigate thermal stability and repeatability, all the fluctuations of k of naphthalene were less than 2.3 % for Sil-Im-C18-1 during flushing 24 h with the mobile phase at different pH values (pH = 3 and 8), the retention time of alkylbenzenes were almost same for Sil-Im-C18-1 at different time, the RSD values of retention time of alkylbenzenes were 0.45 %-2.28 % for two batches Sil-Im-C18-1, revealing the excellent repeatability, thermal stability, durability and reproducibility of Sil-Im-C18, and implying a commercial prospect.


Chromatography, Reverse-Phase , Imidazoles , Polycyclic Aromatic Hydrocarbons , Silicon Dioxide , Imidazoles/chemistry , Silicon Dioxide/chemistry , Chromatography, Reverse-Phase/methods , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/isolation & purification , Polycyclic Aromatic Hydrocarbons/chemistry , Silanes/chemistry , Chromatography, Ion Exchange/methods
16.
Chemosphere ; 356: 141794, 2024 May.
Article En | MEDLINE | ID: mdl-38579945

With new oil and gas lease sales in high-latitude regions, there exists a need to better understand the chemical fate of spilled oil and its effects on biological life. To address this need, laboratory simulations of crude oil spills under sub-Arctic conditions were conducted using artificial seawater and exposure to solar irradiation to create Hydrocarbon Oxidation Products (HOPs). HOPs characterization and their biological effects were assessed using ultra high-performance liquid chromatography (UHPLC) with high resolution mass Orbitrap spectrometry and the aryl hydrocarbon receptor (AhR) chemically activated luciferase gene expression (CALUX) assay. Non-target UHPLC-Orbitrap mass spectrometry analysis identified 251 HOPs that were in greater abundance in light-exposed samples than dark controls. Oxidized polycyclic aromatic hydrocarbons were also detected, including phenanthrene quinone, anthraquinone, hydroxyanthraquinone, and 9-fluoreneone. The composition of HOPs were consistent with photo-products of alkylated two to four ring PAHs, primarily compounds between 1 and 3 aromatic rings and 1-3 oxygens. The HOP mixture formed during photochemical weathering of Cook Inlet crude oil induced greater AhR activity than parent petroleum products solubilized in dark controls, indicating that HOPs, as a complex mixture, may contribute to petroleum toxicity more than the parent petroleum compounds. These non-targeted approaches provide the most comprehensive analysis of hydrocarbon oxidation products to date, highlighting the diversity of the complex mixture resulting from the photooxidation of crude oil and the limitations of targeted analyses for adequately monitoring HOPs in the environment. Taken together, these data identify a critical "blind spot" in environmental monitoring and spill clean-up strategies as there is a diverse pool of HOPs that may negatively impact human and ecosystem health.


Oxidation-Reduction , Petroleum Pollution , Petroleum , Polycyclic Aromatic Hydrocarbons , Petroleum/analysis , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Petroleum Pollution/analysis , Chromatography, High Pressure Liquid , Receptors, Aryl Hydrocarbon/metabolism , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/chemistry , Seawater/chemistry
17.
Environ Pollut ; 349: 123933, 2024 May 15.
Article En | MEDLINE | ID: mdl-38583795

The effects of two benthonic species, Perinereis aibuhitensis and Matuta planipes Fabricius, on the release of polycyclic aromatic hydrocarbons (PAHs) from sediments were investigated using a sediment-seawater microcosm. A Level IV fugacity model was used to simulate the behavior and fate of PAHs in the environment. This study revealed that both benthos significantly influenced the release of PAHs, and Matuta planipes Fabricius had a stronger disturbance effect than another. The final concentrations of Matuta planipes Fabricius group, Perinereis aibuhitensis group and the control group in the seawater phase reached 10.8, 9.94 and 7.90 µg/L, respectively. There were certain differences in the behaviour of the two benthonic species. Matuta planipes Fabricius caused more sediment resuspension, while Perinereis aibuhitensis increased the total organic carbon (TOC) content in the environment. The vertical concentration distribution of sediment indicated that vertical mixing was slightly stronger in the Matuta planipes Fabricius group than that in the Perinereis aibuhitensis group. The fugacity model effectively simulated the release behavior of PAHs, providing insight into PAH transport and distribution. The results demonstrated that bioturbation could promote the release of PAHs from seawater. The amount of PAHs released was significantly correlated with the biological habits of the benthos.


Geologic Sediments , Polycyclic Aromatic Hydrocarbons , Seawater , Water Pollutants, Chemical , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Geologic Sediments/chemistry , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/chemistry , Seawater/chemistry , Environmental Monitoring , Animals
18.
J Chem Inf Model ; 64(8): 3192-3204, 2024 Apr 22.
Article En | MEDLINE | ID: mdl-38500402

This work presents new experimental viscosity and density data for aromatic and polyaromatic compounds in binary and ternary pyrene, 1-methylnaphthalene, and dodecane mixtures. The lack of experimental viscosity data for these mixtures requires the development of a new database, which is vital for understanding the behavior of mixtures in more complex systems, such as asphaltenes and fuels. The mixtures proposed in this work have been measured over a temperature range of (293.15 to 343.15) K at atmospheric pressure. Several mixture compositions have been studied at these conditions: 1.0, 2.5, 5.0, 7.5, 10.0, 12.5, and 15.0% pyrene mass fraction. The concentration of pyrene correlates with an increase in the viscosity and density values. At the lowest temperature in binary mixtures, the corresponding values reach 4.4217 mPa·s for viscosity and 1.0447 × 103 kg·m-3 for density, respectively. In ternary mixtures, the introduction of dodecane leads to the lowest maximum values of 3.5555 mPa·s for viscosity and 1.0112 × 103 kg·m-3 for density at the same temperature. The experimental data have been employed for the specific modification of viscosity models. These modifications could facilitate the prediction of the viscosity of mixtures that are more complex than those presented in this work. Various viscosity models have been employed, such as Linear, Ratcliff and Khan, modified UNIFAC-Visco, and Krieger-Dougherty. The settings in the models used reliably reproduce the experiment reliably. However, the Ratcliff model agrees excellently with the experiment, having a low standard deviation (2.0%) compared to other models. Furthermore, a model based on the equation of state of Guo is proposed to predict the viscosity values by modifying the specific parameters and adjusting them to the mixtures proposed in this work. The results from this study are compared to previous work, where pyrene, toluene, and heptane mixtures were analyzed. In this case, we find that the decrease of aggregation grade in the present systems is predicted by the model fixed in this work.


Alkanes , Naphthalenes , Pyrenes , Temperature , Pyrenes/chemistry , Viscosity , Naphthalenes/chemistry , Alkanes/chemistry , Models, Chemical , Polycyclic Aromatic Hydrocarbons/chemistry
19.
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
20.
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
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