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Biodegradation of Polycyclic Aromatic Hydrocarbons in Mangrove Sediments Under Different Strategies: Natural Attenuation, Biostimulation, and Bioaugmentation with Rhodococcus erythropolis T902.1
2016
Semboung Lang, Firmin | Destain, Jacqueline | Delvigne, Frank | Druart, Philippe | Ongena, Marc | Thonart, Philippe
peer reviewed | Polycyclic aromatic hydrocarbons (PAHs) are pollutants that occur in mangrove sediments. Their removal by bacteria often depends on specific characteristics as the number of benzene rings they possess and their solubility. Their removal also depends on environmental factors, such as pH, temperature, oxygen, and the ability of the endogenous or exogenous microflora to metabolize hydrocarbons.With the aim of treating mangrove sediments polluted by hydrocarbons in a biological way, a biodegradation experiment was conducted using mangrove sediments artificially contaminated with a mixture of four PAHs. The study used Rhodococcus erythropolis as an exogenous bacterial strain in order to assess the biodegradation of the PAH mixture by natural attenuation, biostimulation, bioaugmentation, and a combination of biostimulation and bioaugmentation. The results showed that the last three treatments were more efficient than natural attenuation. The biostimulation/bioaugmentation combination proved to be the most effective PAH degradation treatment.
Show more [+] Less [-]Microwave-responsive SiC foam@zeolite core-shell structured catalyst for catalytic pyrolysis of plastics
2022
Chen, Zhaohui | Monzavi, Mohammad | Latifi, Mohammad | Samih, Said | Chaouki, J.
Catalytic pyrolysis is a promising chemical recycling technology to supplement mechanical recycling since plastics can be broken down into monomers or converted to the required fuels and chemicals. In this study, a microwave (MW) -responsive SiC foam@zeoltie core-shell structured catalyst was proposed for the catalytic pyrolysis of polyolefins. Under microwave irradiation, the SiC foam core works as both microwave adsorber and catalyst support, thus concentrating the generated heat energy on the ZSM-5 zeolite shell, where the catalytic reaction takes place. SiC foam with an open cellular structure can also improve the global transport of mass and heat during plastics pyrolysis. In this work, the effects of the SiO₂/Al₂O₃ ratio and alkaline treatment of ZSM-5 zeolite coated SiC foam under MW irradiation on the variations in product distribution from low-density polyethylene (LDPE) pyrolysis were investigated at 450 °C. The results indicated that the appropriate acidity and pore structure were crucial to upgrading gas and liquid products. Particularly, the creation of a mesoporous structure in ZSM-5 zeolite via alkaline treatment could improve the diffusion of large molecules and products, thus significantly increasing the selectivity of high-valued light olefins and aromatics while inhibiting the formation of unwanted alkanes, which are expected in the chemical industry. Concretely, the concentration of olefins in gas increased to 51.0 vol% for ZSM-5(50)-0.25AT, and 65.6 vol% for ZSM-5 (50)-0.50AT, compared with 45.2 vol% for the parent ZSM-5(50). The relative concentration of aromatics in liquid decreased from 96.6% for ZSM-5(50) to 75.9% for ZSM-5(50)-0.25AT, and 71.1% for ZSM-5(50)-0.50AT. Given the respective yield of gas and liquid, the total selectivity of C2–C4 olefins and aromatics for mesoporous ZSM-5 zeolites could reach 58.6–64.9% during LDPE pyrolysis, which were higher than that for the parent ZSM-5 zeolite.
Show more [+] Less [-]Primary organic gas emissions from gasoline vehicles in China: Factors, composition and trends
2021
Qi, Lijuan | Zhao, Junchao | Li, Qiwei | Su, Sheng | Lai, Yitu | Deng, Fanyuan | Man, Hanyang | Wang, Xiaotong | Shen, Xiu'e | Lin, Yongming | Ding, Yan | Liu, Huan
Continuous tightening emission standards (ESs) facilitate the reduction of organic gas emissions from gasoline vehicles. Correspondingly, it is essential to update the emissions and chemical speciation of total organic gases (TOGs), including volatile organic compounds (VOCs), intermediate volatility organic compounds (IVOCs), CH₄, and unidentified non-methane hydrocarbons (NMHCs) for assessing the formation of ozone and secondary organic aerosol (SOA). In this study, TOG and speciation emissions from 12 in-use light-duty gasoline vehicle (LDGV) exhausts, covering the ESs from China II to China V, were investigated on a chassis dynamometer under the Worldwide Harmonized Light-duty Test Cycle (WLTC) in China. The results showed that the most effectively controlled subgroup in TOG emissions from LDGVs was VOCs, followed by the unidentified NMHCs and IVOCs. The mass fraction of VOCs in TOGs also reduced from 61 ± 9% to 46 ± 18% while the IVOCs gently increased from 2 ± 0.4% to 8 ± 4% along with the more stringent ESs. For the VOC subsets, the removal efficiency of oxygenated VOCs (OVOCs) was lower than those of other VOC subsets in the ESs from China IV to V, suggesting the importance of OVOC emission controls for relatively new LDGVs. The IVOC emissions were mainly subject to the ESs, then driving cycles and fuel use. The formation potentials of ozone and SOA from LDGVs decreased separately 96% and 90% along with the restricted ESs from China II-III to China IV. The major contributor of SOA formation transformed from aromatics in the VOC subsets for China II-III vehicles to IVOCs for China IV/V vehicles, highlighting that IVOC emissions from LDGVs are also needed more attentions to control in future.
Show more [+] Less [-]Effluent decontamination by the ibuprofen-mineralizing strain, Sphingopyxis granuli RW412: Metabolic processes
2021
The high global consumption of ibuprofen and its limited elimination by wastewater treatment plants (WWTPs), has led to the contamination of aquatic systems by this common analgesic and its metabolites. The potentially negative environmental and public health effects of this emerging contaminant have raised concerns, driving the demand for treatment technologies. The implementation of bacteria which mineralize organic contaminants in biopurification systems used to decontaminate water or directly in processes in WWTPs, is a cheap and sustainable means for complete elimination before release into the environment. In this work, an ibuprofen-mineralizing bacterial strain isolated from sediments of the River Elbe was characterized and assayed to remediate different ibuprofen-polluted media. Strain RW412, which was identified as Sphingopyxis granuli, has a 4.48 Mb genome which includes plasmid sequences which harbor the ipf genes that encode the first steps of ibuprofen mineralization. Here, we confirm that these genes encode enzymes which initiate CoA ligation to ibuprofen, followed by aromatic ring activation by a dioxygenase and retroaldol cleavage to unequivocally produce 4-isobutylcatechol and propionyl-CoA which then undergo further degradation. In liquid mineral salts medium, the strain eliminated more than 2 mM ibuprofen within 74 h with a generation time of 16 h. Upon inoculation into biopurification systems, it eliminated repeated doses of ibuprofen within a few days. Furthermore, in these systems the presence of RW412 avoided the accumulation of ibuprofen metabolites. In ibuprofen-spiked effluent from a municipal WWTP, ibuprofen removal by this strain was 7 times faster than by the indigenous microbiota. These results suggest that this strain can persist and remain active under environmentally relevant conditions, and may be a useful innovation to eliminate this emerging contaminant from urban wastewater treatment systems.
Show more [+] Less [-]A new classification approach to enhance future VOCs emission policies: Taking solvent-consuming industry as an example
2021
Zhang, Xinmin | Zhao, Wenjuan | Nie, Lei | Shao, Xia | Dang, Hongyan | Zhang, Weiqi | Wang, Di
Volatile organic compounds (VOCs) has consistently been linked to ozone (O₃) and secondary organic aerosol (SOA) formation, and ongoing emission policies are primarily focusing on total VOCs without addressing the association between regulation measures and secondary pollution characteristic. For enhancing VOCs emission policy, we investigated potential formation of O₃ and SOA based on analyses of node-specific VOCs concentration and species distribution in solvent-consuming industry. Although aromatics were found to contribute most to O₃ and SOA formation averagely (2.57 ± 2.14 g O₃/g VOCs, 1.91 ± 1.67 g SOA/g VOCs), however, large disparity concerning emission and secondary pollution profile were identified among different emission nodes which demonstrated that regulation policy should be formulated based on comprehensive pollution characteristic. Therefore, emission nodes were classified into four clusters through data normalization, formatting and classification process, including aromatics dominated (7 emission nodes), aromatics-alkene dominated (4 emission nodes), aromatics-alcohols dominated (4 emission nodes) and alcohols dominated (4 emission nodes). And different dominating VOCs species were further obtained in each cluster. Subsequently, focusing regulation measures of reducing O₃ and SOA for different emission source clusters were proposed to guide pollution prevention and enhance future VOCs emission policies.
Show more [+] Less [-]Ozone and SOA formation potential based on photochemical loss of VOCs during the Beijing summer
2021
Zhan, Junlei | Feng, Zeming | Liu, Pengfei | He, Xiaowei | He, Zhouming | Chen, Tianzeng | Wang, Yafei | He, Hong | Mu, Yujing | Liu, Yongchun
Volatile organic compounds (VOCs) are easily degraded by oxidants during atmospheric transport. Therefore, the contribution of VOCs to ozone (O₃) and secondary organic aerosol (SOA) formation at a receptor site is different from that in a source area. In this study, hourly concentrations of VOCs and other pollutants, such as O₃, NOx, HONO, CO, and PM₂.₅, were measured in the suburbs (Daxing district) of Beijing in August 2019. The photochemical initial concentrations (PICs), in which the photochemical losses of VOCs were accounted for, were calculated to evaluate the contribution of the VOCs to O₃ and SOA formation. The mean (±standard deviation) measured VOC concentrations and the PICs were 11.2 ± 5.7 and 14.6 ± 8.4 ppbv, respectively, which correspond to O₃ formation potentials (OFP) of 57.8 ± 26.3 and 103.9 ± 109.4 ppbv and SOA formation potentials (SOAP) of 8.4 ± 4.1 and 10.3 ± 7.4 μg m⁻³, respectively. Alkenes contributed 80.5% of the consumed VOCs, followed by aromatics (13.3%) and alkanes (6.2%). The contributions of the alkenes and aromatics to the OFPPICₛ were 56.8% and 30.3%, respectively; while their corresponding contributions to the SOAPPICₛ were 1.9% and 97.3%, respectively. The OFPPICₛ was linearly correlated with the observed O₃ concentrations (OFPPICₛ = 41.5 + 1.40 × cO₃, R² = 0.87). The O₃ formation was associated with a VOC-limited regime at the receptor site based on the measured VOCs and changed to a transition regime and a NOx sensitive regime based on the PIC. Our results suggest that more attention should be paid to biogenic VOCs when studying O₃ formation in summer in Beijing, while the control of anthropogenic aromatic compounds should be given priority in terms of SOA formation.
Show more [+] Less [-]Characterization of a Dibenzofuran-degrading strain of Pseudomonas aeruginosa, FA-HZ1
2019
Ali, Fawad | Hu, Haiyang | Wang, Weiwei | Zhou, Zikang | Shah, Syed Bilal | Xu, Ping | Tang, Hongzhi
Dibenzofuran (DBF) derivatives have caused serious environmental problems, especially those produced by paper pulp bleaching and incineration processes. Prominent for its resilient mutagenicity and toxicity, DBF poses a major challenge to human health. In the present study, a new strain of Pseudomonas aeruginosa, FA-HZ1, with high DBF-degrading activity was isolated and identified. The determined optimum conditions for cell growth of strain FA-HZ1 were a temperature of 30 °C, pH 5.0, rotation rate of 200 rpm and 0.1 mM DBF as a carbon source. The biochemical and physiological features as well as usage of different carbon sources by FA-HZ1 were studied. The new strain was positive for arginine double hydrolase, gelatinase and citric acid, while it was negative for urease and lysine decarboxylase. It could utilize citric acid as its sole carbon source, but was negative for indole and H2S production. Intermediates of DBF 1,2-dihydroxy-1,2-dihydrodibenzofuran, 1,2-dihydroxydibenzofuran, 2-hydroxy-4-(3′-oxo-3′H-benzofuran-2′-yliden)but-2-enoic acid, 2,3-dihydroxybenzofuran, 2-oxo-2-(2′-hydrophenyl)lactic acid, and 2-hydroxy-2-(2′-hydroxyphenyl)acetic acid were detected and identified through liquid chromatography-mass analyses. FA-HZ1 metabolizes DBF by both the angular and lateral dioxygenation pathways. The genomic study identified 158 genes that were involved in the catabolism of aromatic compounds. To identify the key genes responsible for DBF degradation, a proteomic study was performed. A total of 1459 proteins were identified in strain FA-HZ1, of which 100 were up-regulated and 104 were down-regulated. A novel enzyme “HZ6359 dioxygenase”, was amplified and expressed in pET-28a in E. coli BL21(DE3). The recombinant plasmid was successfully constructed, and was used for further experiments to verify its function. In addition, the strain FA-HZ1 can also degrade halogenated analogues such as 2, 8-dibromo dibenzofuran and 4-(4-bromophenyl) dibenzofuran. Undoubtedly, the isolation and characterization of new strain and the designed pathways is significant, as it could lead to the development of cost-effective and alternative remediation strategies. The degradation pathway of DBF by P. aeruginosa FA-HZ1 is a promising tool of biotechnological and environmental significance.
Show more [+] Less [-]Cytochrome P450 1A transcript is a suitable biomarker of both exposure and response to diluted bitumen in developing frog embryos
2019
Lara-Jacobo, Linda R. | Willard, Brianna | Wallace, Sarah J. | Langlois, Valerie S.
In order for Alberta's thick bitumen to be transported through pipelines, condensates are added creating a diluted bitumen (dilbit) mixture. Recent pipeline expansion projects have generated concern about potential dilbit spills on aquatic wildlife health. Studies have suggested that polycyclic aromatic compounds (PACs) are toxic to aquatic vertebrates and could potentially also interfere with their endocrine system. The research objectives of this study were to investigate the toxicity of dilbit to developing frog embryos and to identify the molecular mechanisms of action involved. Fertilized embryos of Western clawed frog (Silurana tropicalis) were exposed for 72 h to water accommodated fractions (WAF; 0.7–8.9 μg/L TPACs) and chemically-enhanced WAFs (CEWAF; 0.09–56.7 μg/L TPACs) of Access Western Blend (AWB) and Cold Lake Blend (CLB) dilbits. Both dilbit's CEWAFs significantly increased embryonic mortality and malformation incidence in the highest treatments tested, while WAF treatments led to no visible toxic effects. Increases of the cytochrome P450 1A (cyp1a) mRNA levels were observed for all WAF and CEWAF dilbit treatments suggesting that phase I detoxification is activated in the dilbit-exposed larvae. When exposed to PAC concentrations ranging from 0.09 to 8.9 μg/L, the frogs displayed no observable malformations, but expressed significant increases of cyp1a mRNA levels (2- to 25-fold; indicating a suitable biomarker of exposure); however, when concentrations were of 46.6 μg/L or higher, both malformed frog phenotype and induction of cyp1a mRNA level (>250-fold) were measured (indicating a suitable biomarker of response). The expression of several genes related to cellular detoxification and endocrine disruption were also measured, but were not significantly altered by the treatments. In sum, cyp1a mRNA level is a highly sensitive endpoint to measure subtle molecular changes induced by PAC exposure in the frog embryos and larvae, and data suggest that PAC concentration higher than 46 μg/L would be toxic to the developing S. tropicalis.
Show more [+] Less [-]Correlations and adsorption mechanisms of aromatic compounds on biochars produced from various biomass at 700 °C
2018
Yang, Kun | Jiang, Yuan | Yang, Jingjing | Lin, Daohui
Knowledge of adsorption behavior of organic contaminants on high heat temperature treated biochars is essential for application of biochars as adsorbents in wastewater treatment and soil remediation. In this study, isotherms of 25 aromatic compounds adsorption on biochars pyrolyzed at 700 °C from biomass including wood chips, rice straw, bamboo chips, cellulose, lignin and chitin were investigated to establish correlations between adsorption behavior and physicochemical properties of biochars. Isotherms were well fitted by Polanyi theory-based Dubinin-Ashtakhov (DA) model with three parameters, i.e., adsorption capacity (Q⁰) and adsorption affinity (E and b). Besides the negative correlation of Q⁰ with molecular maximum cross-sectional areas (σ) of organic compounds, positive correlations of Q⁰ with total pore volume (Vₜₒₜₐₗ) and average diameter of micropore (D) of biochars were observed, indicating that adsorption by biochars is captured by the pore-filling mechanism with molecular sieving effect in biochar pores. Linear solvation energy relationships (LSERs) of adsorption affinity (E) with solvatochromic parameters of organic compounds (i. e., αₘ and π∗) were established, suggesting that hydrophobic effect, π-π interaction and hydrogen-bonding interaction are the main forces responsible for adsorption. The regression coefficient (π₁) and intercept (C) of obtained LSERs are correlated with biochar H/C and Rₘᵢcᵣₒ, respectively, implying that biochars with higher aromaticity and more micropores have stronger π-π bonding potential and hydrophobic effect potential with aromatic molecule, respectively. However, hydrogen-bonding potential of biochars for organic molecules is not changed significantly with properties of biochars. A negative correlation of b with biochar H/C is also obtained. These correlations could be used to predict the adsorption behavior of organic compounds on high heat temperature treated biochars from various biomass for the application of biochars as sorbents and for the estimating of environmental risks of organic compounds in the present of biochars.
Show more [+] Less [-]Rapidly probing the interaction between sulfamethazine antibiotics and fulvic acids
2018
Xu, Juan | Hu, Yan-Yun | Li, Xiu-Yan | Chen, Jie-Jie | Sheng, Guo-Ping
Antibiotics residuals in the environments receive wide concerns due to the high risk of generating antibiotic resistance. Natural organic matters (NOM) existed in the environments are considered to have the capacity of binding with organic contaminants, consequently influencing their speciation and transformation in the natural environments. To assess the migration of antibiotics in the environments, it is crucial to understand the binding mechanisms between NOM and antibiotics, which is still unclear due to the limit of available research methods. In this study, the interaction between fulvic acids (FA), one of the main components of NOM, and sulfamethazine (SMZ) was characterized by nuclear magnetic resonance (NMR) combined with surface plasmon resonance (SPR) and isothermal titration calorimetry (ITC) technology. The parameters related to kinetics and thermodynamics of the interaction were determined, and the possible mechanisms driving the interaction were also proposed. In addition, density functional theory (DFT) was used to predict the binding mode between FA and SMZ to reveal the interaction mechanism. Results indicate that FA can effectively bound with SMZ to form a stable complex with a binding constant at the level of 10³ L/mol. The kinetic parameters including association and dissociation constants were 29.4 L/mol/s and 6.64 × 10⁻³ 1/s, respectively. Hydrophobic interaction might play significant roles in the binding interaction with ancillary contribution of π-π conjunction arising from the aromatic rings stacking of FA and SMZ.
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