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Degradation of chloramphenicol by Ti/PbO2–La anodes and alteration in bacterial community and antibiotics resistance genes
2022
Dong, Hao | Fu, Yanli | Wang, Pengqi | Jiang, Wenqiang | Gao, Guangfei | Zhang, Xuan
Antibiotics accumulation in the environment has given rise to multi-drug resistant 'superbugs' and antibiotics resistence genes (ARGs). Chloramphenicol (CAP), a kind of widely used antibiotics, was chosen as the model compound to investigate its degradation during electrochemical treatment process. The prepared Ti/PbO₂–La electrodes had a denser surface and a more complete PbO₂ crystal structure than Ti/PbO₂ electrode. The doping of La increased the onset potential and the overpotential, increased the current value of the oxidation peak and the reduction peak, reduced the impedance, and increased the lifetime. The reactions CAP degradation and TOC removal on Ti/PbO₂–La electrode was both primary kinetic reactions. CAP degradation rate increased with current density, and TOC obtained the highest removal at current density of 25 mA cm⁻². The electrolyte concentration had a small effect in the range of 0.050–0.150 mol L⁻¹. The effects under acidic and neutral conditions were better than under alkaline conditions. CAP was mainly directly oxidized at the electrode surface and indirect oxidation also took place via generated ·OH and SO₄·⁻. 15 intermediates and 2 degradation pathways have been postulated. The entry of CAP and CAP intermediates into the environment caused the alteration in bacterial community and ARGs, while complete degradation products had little effect on them. Redundancy analysis showed that intI1 was the dominant factor affecting ARGs, and Actinobacteria and Patescibacteria were the main factors affecting the abundances of ARGs in the microbial community.
اظهر المزيد [+] اقل [-]Treatment of microplastics in water by anodic oxidation: A case study for polystyrene
2021
Kiendrebeogo, Marthe | Karimi Estahbanati, M.R. | Khosravanipour Mostafazadeh, Ali | Drogui, Patrick | Tyagi, R.D.
Water pollution by microplastics (MPs) is a contemporary issue which has recently gained lots of attentions. Despite this, very limited studies were conducted on the degradation of MPs. In this paper, we reported the treatment of synthetic mono-dispersed suspension of MPs by using electrooxidation (EO) process. MPs synthetic solution was prepared with distilled water and a commercial polystyrene solution containing a surfactant. In addition to anode material, different operating parameters were investigated such as current intensity, anode surface, electrolyte type, electrolyte concentration, and reaction time. The obtained results revealed that the EO process can degrade 58 ± 21% of MPs in 1 h. Analysis of the operating parameters showed that the current intensity, anode material, electrolyte type, and electrolyte concentration substantially affected the MPs removal efficiency, whereas anode surface area had a negligible effect. In addition, dynamic light scattering analysis was performed to evaluate the size distribution of MPs during the degradation. The combination of dynamic light scattering, scanning electron microscopy, total organic carbon, and Fourier-transform infrared spectroscopy results suggested that the MPs did not break into smaller particles and they degrade directly into gaseous products. This work demonstrated that EO is a promising process for degradation of MPs in water without production of any wastes or by-products.
اظهر المزيد [+] اقل [-]Electrochemical removal of levofloxacin using conductive graphene/polyurethane particle electrodes in a three-dimensional reactor
2020
Guo, Cuicui | Liu, Haiyang | Wang, Chengzhi | Zhao, Jianchen | Zhao, Wenjun | Lu, Nan | Qu, Jiao | Yuan, Xing | Zhang, Ya-nan
The conductive polyurethane/polypyrrole/graphene (CPU/PPy/Gr) particle electrode was prepared by an in-situ oxidative polymerization method and used as particle electrodes to degrade levofloxacin (LEV) in a three-dimensional electrode reactor. The prepared CPU/PPy/Gr electrode was characterized systematically and the effects of initial pH, initial LEV concentration, aeration volume, voltage, and electrolyte concentration on the degradation efficiency were investigated. Results showed that more than 90% LEV was degraded and the energy consumption was 20.12 kWh/g LEV under conditions of pH 7, 6 V voltage, 2.0 L/min aeration volume, 20 mg/L initial LEV concentration, and 7 mM concentration of electrolyte (Na₂SO₄). A possible electrochemical oxidation pathway of LEV by the CPU/PPy/Gr electrode was proposed. In addition, the biotoxicity of LEV and its oxidation products was calculated using ECOSAR (Ecological Structure Activity Relationships) program in EPISuite. Toxicity evaluation using luminescent bacteria showed that the toxicities of some intermediates were higher than the parent compound. But the toxicity of degradation processes for LEV was effective decreasing. A possible reactive mechanism in the three-dimensional reactor was also recommended. In brief, the prepared CPU/PPy/Gr particle electrode constitutes an insight into the promising practical application in the wastewater treatment.
اظهر المزيد [+] اقل [-]Alginate affects agglomeration state and uptake of 14C-labeled few-layer graphene by freshwater snails: Implications for the environmental fate of graphene in aquatic systems
2018
Su, Yu | Huang, Ji | Lu, Fenxiao | Tong, Xin | Niu, Junfeng | Mao, Liang
Understanding of the interaction of graphene with natural polysaccharides (e.g., alginate) is crucial to elucidate its environmental fate. We investigated the impact of alginate on the agglomeration and stability of ¹⁴C-labeled few-layer graphene (FLG) in varying concentrations of monovalent (NaCl) and divalent (CaCl₂) electrolytes. Enhanced agglomeration occurred at high CaCl₂ concentrations (≥5 mM) due to the alginate gel networks formation in the presence of Ca²⁺. FLG enmeshed within extended alginate gel networks was observed under transmission electron microscope and atomic force microscope. However, background Na⁺ competition for binding sites with Ca²⁺ at the alginate surfaces shielded the gelation of alginate. FLG was readily dispersed by alginate under environmentally relevant ionic strength conditions (i.e., <200 mM Na⁺ and <5 mM Ca²⁺). In comparison with the bare FLG, the slow sedimentation of the alginate-stabilized FLG (158 μg/L) caused continuous exposure of this nanomaterial to freshwater snails, which ingested 1.9 times more FLG through filter-feeding within 72 h. Moreover, surface modification of FLG by alginate significantly increased the whole-body and intestinal levels of FLG, but reduced the internalization of FLG to the intestinal epithelial cells. These findings indicate that alginate will act as a stabilizing agent controlling the transport of FLG in aqueous systems. This study also provides the first evidence that interaction of graphene with natural polysaccharides affected the uptake of FLG in the snails, which may alter the fate of FLG in aquatic environments.
اظهر المزيد [+] اقل [-]Aggregation kinetics of microplastics in aquatic environment: Complex roles of electrolytes, pH, and natural organic matter
2018
Li, Shuocong | Liu, Hong | Gao, Rui | Abdurahman, Abliz | Dai, Juan | Zeng, Feng
Microplastics are an emerging contaminants of concern in aquatic environments. The aggregation behaviors of microplastics governing their fate and ecological risks in aquatic environments is in need of evaluation. In this study, the aggregation behavior of polystyrene microspheres (micro-PS) in aquatic environments was systematically investigated over a range of monovalent and divalent electrolytes with and without natural organic matter (i.e., Suwannee River humic acid (HA)), at pH 6.0, respectively. The zeta potentials and hydrodynamic diameters of micro-PS were measured and the subsequent aggregation kinetics and attachment efficiencies (α) were calculated. The aggregation kinetics of micro-PS exhibited reaction- and diffusion-limited regimes in the presence of monovalent or divalent electrolytes with distinct critical coagulation concentration (CCC) values, followed the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. The CCC values of micro-PS were14.9, 13.7, 14.8, 2.95 and 3.20 mM for NaCl, NaNO3, KNO3, CaCl2 and BaCl2, respectively. As expected, divalent electrolytes (i.e., CaCl2 and BaCl2) had stronger influence on the aggregation behaviors of micro-PS as compared to monovalent electrolytes (i.e., NaCl, NaNO3 and KNO3). HA enhanced micro-PS stability and shifted the CCC values to higher electrolyte concentrations for all types of electrolytes. The CCC values of micro-PS were lower than reported carbonaceous nanoparticles CCC values. The CCC[Ca2+]/CCC [Na+] ratios in the absence and presence of HA at pH 6.0 were proportional to Z−2.34 and Z−2.30, respectively. These ratios were in accordance with the theoretical Schulze–Hardy rule, which considers that the CCC is proportional to z−6–z−2. These results indicate that the stability of micro-PS in the natural aquatic environment and the possibility of significant aqueous transport of micro-PS.
اظهر المزيد [+] اقل [-]Interaction between Al2O3 and different sizes of GO in aqueous environment
2018
Liu, Xia | Xu, Xuetao | Sun, Ju | Duan, Shengxia | Sun, Yubing | Hayat, Tasawar | Li, Jiaxing
Although the aggregation of graphene oxide (GO) has been widely researched, the influence of the GO size on the homoaggregation behavior and its interaction with environmental media are still unexplored. In this work, critical coagulation concentration (CCC) values for GO with different sizes, from micro to nanosheet, were measured with NaCl and CaCl₂ electrolytes, and the results indicated that GO with the largest size presented the smallest CCC value. Aluminum oxide (Al₂O₃) was selected as a natural solid particle representative to mimic the interaction between GO and environmental media. Batch experiments were conducted in solution with different pH and ionic strength. Results indicated that the attachment capacity of large GO onto Al₂O₃ particles was greater than that of small GO. The experimental data were well fitted with Freundlich model. The electrostatic attraction and hydrogen-bonding interaction dominated the interaction process between GO and Al₂O₃. These findings are important for better understanding in the environmental fate and transport of GO.
اظهر المزيد [+] اقل [-]Transport and retention of biochar nanoparticles in a paddy soil under environmentally-relevant solution chemistry conditions
2017
Chen, Ming | Wang, Dengjun | Yang, Fan | Xu, Xiaoyun | Xu, Nan | Cao, Xinde
Land application of biochar has been increasingly recommended as a powerful strategy for carbon sequestration and soil remediation. However, the biochar particles, especially those in the nanoscale range, may migrate or carry the inherent contaminants along the soil profile, posing a potential risk to the groundwater. This study investigated the transport and retention of wood chip-derived biochar nanoparticles (NPs) in water-saturated columns packed with a paddy soil. The environmentally-relevant soil solution chemistry including ionic strength (0.10–50 mM), electrolyte type (NaCl and CaCl2), and natural organic matter (0–10 mg L−1 humic acid) were tested to elucidate their effects on the biochar NPs transport. Higher mobility of biochar NPs was observed in the soil at lower ionic strengths, with CaCl2 electrolyte being more effective than NaCl in decreasing biochar NPs transport. The retained biochar NPs in NaCl was re-entrained (∼57.7%) upon lowering transient pore-water ionic strength, indicating that biochar NPs were reversibly retained in the secondary minimum. In contrast, negligible re-entrainment of biochar NPs occurred in CaCl2 due to the primary minimum and/or particle aggregation. Humic acid increased the mobility of biochar NPs, likely due to enhanced electrosteric repulsive interactions. The transport behaviors of biochar NPs can be well interpreted by a two-site kinetic retention model that assumes reversible retention for one site, and irreversible retention for the other site. Our findings indicated that the transport of wood chip biochar NPs is significant in the paddy soil, highlighting the importance of understanding the mobility of biochar NPs in natural soils for accurately assessing their environmental impacts.
اظهر المزيد [+] اقل [-]Preparation of immobilized coating Fenton-like catalyst for high efficient degradation of phenol
2017
Wang, Jiankang | Yao, Zhongping | Wang, Yajing | Xia, Qixing | Chu, Huiya | Jiang, Zhaohua
In this study, solid acid amorphous Fe3O4/SiO2 ceramic coating decorated with sulfur on Q235 carbon steel as Fenton-like catalyst for phenol degradation was successfully prepared by plasma electrolytic oxidation (PEO) in silicate electrolyte containing Na2S2O8 as sulfur source. The surface morphology and phase composition were characterized by SEM, EDS, XRD and XPS analyses. NH3-TPD was used to evaluate surface acidity of PEO coating. The results indicated that sulfur decorated amorphous Fe3O4/SiO2 ceramic coatings with porous structure and higher acid strength had the similar pore size and the surface became more and more uneven with the increase of Na2S2O8 in the silicate electrolyte. The Fenton-like catalytic activity of sulfur decorated PEO coatings was also evaluated. In contrast to negligible catalytic activity of sulfur undecorated PEO coating, catalytic activity of sulfur decorated PEO coating was excellent and PEO coating prepared with 3.0 g Na2S2O8 had the highest catalytic activity which could degrade 99% of phenol within 8 min under circumneutral pH. The outstanding performance of sulfur decorated PEO coating was attributed to strong acidic microenvironment and more Fe²⁺ on the surface. The strong acid sites played a key factor in determining catalytic activity of catalyst. In conclusion, rapid phenol removal under circumneutral pH and easier separation endowed it potential application in wastewater treatment. In addition, this strategy of preparing immobilized solid acid coating could provide guidance for designing Fenton-like catalyst with excellent catalytic activity and easier separation.
اظهر المزيد [+] اقل [-]Deposition and release kinetics of nano-TiO2 in saturated porous media: Effects of solution ionic strength and surfactants
2013
Godinez, Itzel G. | Darnault, Christophe J.G. | Khodadoust, Amid P. | Bogdan, Dorin
The aggregation, transport and deposition kinetics (i.e. attachment and release) of TiO2 nanoparticles (nano-TiO2) were investigated as a function of ionic strength and the presence of anionic (sodium dodecylbenzene sulfonate, SDBS) and non-ionic (Triton X-100) surfactants in 100% critical micelle concentration (CMC). The electrolyte concentration of the suspensions dictated the kinetic stability of nano-TiO2 thus influencing the transport and retention of the nanoaggregates in the saturated porous medium. With increasing ionic strength, the interaction between approaching nano-TiO2 and nano-TiO2 already deposited onto collectors surfaces seemed to be more favorable than the interaction between approaching nano-TiO2 and bare collectors surfaces. The abrupt and gradual reduction in electrolyte concentration during the flushing cycles of the column experiments induced the release of previously deposited nano-TiO2 suggesting attachment of nano-TiO2 through secondary energy minimum.
اظهر المزيد [+] اقل [-]Coupled with EDDS and approaching anode technique enhanced electrokinetic remediation removal heavy metal from sludge
2021
Tang, Jian | Qiu, Zhongping | Tang, Hengjun | Wang, Haiyue | Sima, Weiping | Liang, Chao | LIao, Yi | Li, Zhihua | Wan, Shan | Dong, Jianwei
In this work, the novel technology was used to remove heavy metal from sludge. The coupled with biodegradable ethylenediamine disuccinic acid (EDDS) and approaching anode electrokinetic (AA-EK) technique was used to enhance heavy metal removing from sludge. Electric current, sludge and electrolyte characteristics, heavy metal removal efficiency and residual content distribution, and heavy metal fractions percentage of variation were evaluated during the electrokinetic remediation process. Results demonstrated that the coupled with EDDS and AA-EK technique obtain a predominant heavy metal removal efficiency, and promote electric current increasing during the enhanced electrokinetic remediation process. The catholyte electrical conductivity was higher than the anolyte, and electrical conductivity of near the cathode sludge achieved a higher value than anode sludge during the coupled with EDDS and AA-EK remediation process. AA-EK technique can produce a great number of H⁺, which caused the sludge acidification and pH decrease. Cu, Zn, Cr, Pb, Ni and Mn obtain the highest extraction efficiency after the coupled with EDDS and AA-EK remediation, which were 52.2 ± 2.57%, 56.8 ± 3.62%, 60.4 ± 3.62%, 47.2 ± 2.35%, 53.0 ± 3.48%, 54.2 ± 3.43%, respectively. Also, heavy metal fractions analysis demonstrated that the oxidizable fraction percentage decreased slowly after the coupled with EDDS and AA-EK remediation.
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