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1.
J Environ Manage ; 326(Pt B): 116775, 2023 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-36402015

RESUMO

Nanoscale zero-valent iron is considered to be a promising nanostructure for environmental remediation, while increasing the electron selectivity of nanoscale zerovalent iron (nZVI) during target contaminant removal is still a challenge (electron selectivity, defined as the percentage of electrons transferred to the target contaminants over the number of electrons donated by nZVI). In this study, the strategy for increasing the reactivity and electron selectivity of nZVI via sophorolipid (SL-nZVI) modification was proposed. The results showed that the removal efficiency and electron selectivity of SL-nZVI toward Cr(VI) was 99.99% and 56.30%, which was higher than that of nZVI (61.16%, 25.91%). Meanwhile, the particles were well characterized and the mechanism for enhanced reactivity and electron selectivity was investigated. Specially, both the morphology and BET specific surface area characterization suggested that stability against aggregation was higher in SL-nZVI nanoparticles than in nZVI. Besides, X-ray photoelectron spectroscopy (XPS), Tafel polarization curves, and Electrochemical impedance spectroscopy also indicated that the introduction of sophorolipid successfully prevent the nanoparticles from oxidation and benefit the electron transferring. In addition, a water contact angle test revealed that SL-nZVI nanoparticles were less hydrophilic (contact angle = 34.8°) than nZVI (contact angle = 23.9°). Therefore, in terms of reactivity, sophorolipid modification inhibited the aggregation of the nanoparticles and enhanced the electrical conductivity. For electron selectivity, the introduction of sophorolipid not only benefited Cr(VI) adsorption and the electron transfer from Fe0 to the surface-adsorbed Cr(VI) that followed but also reduced the possibility of side reactions between Fe0 and H2O. This study demonstrates that the introduction of sophorolipid is an effective strategy for developing a highly efficient nZVI-based nanocomposite system and highlights the potential role of sophorolipid in improving the electron selectivity of nZVI.


Assuntos
Ferro , Poluentes Químicos da Água , Ferro/química , Elétrons , Poluentes Químicos da Água/química , Cromo/química , Adsorção
2.
J Environ Manage ; 340: 118004, 2023 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-37119628

RESUMO

The problem of co-contaminated soil at e-waste dismantling sites is serious and constitutes a critical threat to human health and the ecological environment. Zero-valent iron (ZVI) has been proven to be effective in the stabilization of heavy metals and the removal of halogenated organic compounds (HOCs) from soils. However, for the remediation of co-contamination of heavy metals with HOCs, ZVI has disadvantages such as high remediation cost and inability to take into account both pollutants, which limits its large-scale application. In this paper, boric acid and commercial zero-valent iron (cZVI) were used as raw materials to prepare boric acid-modified zero-valent iron (B-ZVIbm) through a high-energy ball milling strategy. B-ZVIbm coupled with persulfate (PS) to achieve simultaneous remediation of co-contaminated soil. The synergistic treatment of PS and B-ZVIbm resulted in the removal efficiency of 81.3% for decabromodiphenyl ether (BDE209) and the stabilization efficiencies of 96.5%, 99.8%, and 28.8% for Cu, Pb, and Cd respectively in the co-contaminated soil. A series of physical and chemical characterization methods showed that the oxide coat on the surface of B-ZVIbm could be replaced by borides during ball milling. The boride coat facilitated the exposure of the Fe0 core, promoted the corrosion of ZVI and the orderly release of Fe2+. The analysis of the morphological transformation of heavy metals in soils revealed that most of the heavy metals in the exchangeable, carbonate-bound state were transformed into the residue state, which was the key mechanism for the remediation of heavy metal-contaminated soils with B-ZVIbm. The analysis of BDE209 degradation products showed that BDE209 was degraded to lower brominated products and further mineralized by ZVI reduction and free radical oxidation. In general, B-ZVIbm coupled with PS is a good recipe for synergistic remediation of co-contaminated soils with heavy metals and HOCs.


Assuntos
Metais Pesados , Poluentes Químicos da Água , Humanos , Ferro/química , Metais Pesados/análise , Ácidos Bóricos , Solo/química , Poluentes Químicos da Água/química
3.
Environ Res ; 214(Pt 4): 114189, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-36030911

RESUMO

Novel modified-TiO2/Zr-doped SiO2/g-C3N4 ternary composite is fabricated via an in-situ grow of porous Zr-SiO2 layer to TiO2/g-C3N4 heterojunction, which exhibits well adsorption-photocatalytic performance under simulated solar light irradiation. The nano-size mesoporous TiO2 are dispersed on the lamellar g-C3N4, and the Zr-SiO2 is in-situ fabricated onto the surface of g-C3N4 sheets. The adsorption occurs on the SiO2 layers, and doping Zr element to SiO2 enhances the adsorption of pollutants, while the photocatalytic reaction occurs on the valence band (VB) of TiO2 and conduction band (CB) of g-C3N4, which gives reactive oxygen species of ∙O2-, h+, and ∙OH for high efficient decomposition of antibiotics, i.e. berberine hydrochloride (98.11%), tetracycline (80.76%), and oxytetracycline (84.84%). The excellent adsorption capacity and Z-scheme photoinduced charge carrier migration behavior endowed the novel material with enhanced berberine hydrochloride (BH) removal in water, which approximately 2.5 and 3.8 folds than that of pure g-C3N4 and sole TiO2, respectively. Three degradation pathways are unraveled by LC-MS and theoretical calculations. Furthermore, the toxicity of intermediates was evaluated by the Toxicity Estimation Software Tool (T.E.S.T.), the result demonstrated a good application potential of M-TiO2/Zr-SiO2/g-C3N4 as an novel adsorptive photocatalyst.


Assuntos
Berberina , Dióxido de Silício , Adsorção , Antibacterianos , Catálise , Luz , Titânio
4.
J Environ Manage ; 301: 113894, 2022 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-34638045

RESUMO

A biotic iron (Fe0) treatment system combined with mixed microorganisms was applied to remediate cadmium (Cd)-contaminated groundwater under the intervention of sulfate. Due to hydrogenotrophic desulfuration effect, severe iron corrosion was observed in this microbe-collaborative Fe0 system according to surface morphology analysis as lots of secondary minerals (e.g. magnetite, green rust and lepidocrocite) were generated, which was essential for Cd(II) adsorption and immobilization. The sulfate-mediated biotic Fe0 system thereafter achieved a significantly enhanced Cd(II) removal efficiency of 86.1%, over 3.3 times than that in the abiotic Fe0 system. Increasing initial sulfate concentration could improve the removal of cadmium, which further proved that hydrogenotrophic desulfuration played a key role for enhanced Cd removal. According to the experimental results and current reports, the mechanism of Cd(II) removal was revealed into three pathways including adsorption to secondary iron minerals, co-precipitation with iron (hydr)oxides and formation of cadmium sulfide precipitation. Increasing Fe0 dosages showed positive correlation to Cd(II) removal and neutral pH was preferred to sulfate-mediated biotic Fe0 corrosion. These results indicated that sulfate-mediated biotic Fe0 corrosion could greatly relieve the limitation of Fe0 in Cd(II) immobilization, which could be a promising method to eliminate Cd(II) pollution from groundwater.


Assuntos
Cádmio , Água Subterrânea , Cádmio/análise , Corrosão , Ferro , Sulfatos
5.
J Environ Manage ; 299: 113595, 2021 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-34450304

RESUMO

Mechanochemistry has been proved to be an effective method to remediation of organic-contaminated sites. However, the high ball-to-powder mass ratio (CR) limits the large-scale application of mechanochemistry. In this study, co-milling additives were introduced to enhance the mechanochemical degradation of decabromodiphenyl ether (BDE209)-contaminated soil under the condition of low CR. Based on additive screening experiments, sodium borohydride was selected as the ideal additive to assist the mechanochemical degradation of BDE209, and the resulting removal efficiency was approximately 100% with 2 h of ball milling at a rotational speed of 550 rpm. The main degradation intermediates and degradation pathway of BDE209 were identified using gas chromatography-tandem mass spectrometry. It was proposed that the degradation of BDE209 by sodium borohydride-assisted mechanochemistry was a concurrent process of stepwise and multistage debromination. Meanwhile, the meta-bromine atom in BDE209 was more susceptible to debromination than those at the para and ortho positions. The evolution of the concentration of Br- was monitored by ion chromatography, which revealed that reduction and oxidation both occurred in the removal of BDE209. This paper provides a new perspective for reducing the CR in the mechanochemical remediation of BDE209-contaminated soil.


Assuntos
Éteres Difenil Halogenados , Poluentes do Solo , Poluição Ambiental , Oxirredução , Solo , Poluentes do Solo/análise
6.
J Environ Manage ; 257: 109951, 2020 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-31868635

RESUMO

A collaborative system of carboxymethyl cellulose stabilized nanosized zero-valent iron (CMC-nFe0) and microorganisms was set up to enhance the stabilization of Cr(VI) in soil. In comparison with an aqueous-bound Cr(VI) removal of 18.9% in the nFe0 system, a higher Cr(VI) removal of 68.9% was achieved in the nFe0 and microorganisms system after 14 d remediation because the microorganisms on the nFe0 surface promoted nFe0 corrosion and enhanced abiotic and biotic Cr(VI) stabilization by generating highly active minerals such as magnetite, lepidocrocite and green rust on the nFe0 surface. As a stabilizing agent for nFe0 and an organic substrate for microorganisms, CMC on the nFe0 surface not only enhanced the dispersion of nFe0, but also boosted the activity of microorganisms, resulting in a promotion of 0.9 and 0.5 times higher aqueous-bound Cr(VI) removal via the improvement of nFe0 and microorganisms respectively, thus a total 4 times higher aqueous-bound Cr(VI) removal of 95.3% was achieved in the CMC-nFe0 and microorganisms system as compared to the nFe0 system. After 14 d remediation, easily available species of Cr(VI) and Crtotal, such as water soluble (WS), exchangeable (EX) and bounded to carbonates (CB), were mainly transformed to less available Fe-Mn oxides-bounded (OX) and residual (RS) species because of the production of ferrochrome precipitates (CrxFe1-xOOH or CrxFe1-x(OH)3). Besides, the stabilization of Cr(VI) in the CMC-nFe0 and microorganisms system was pH-dependent and it increased with CMC-nFe0 dosage. Due to excellent Cr(VI) stabilization and Cr immobilization, coupled CMC-nFe0 and anaerobic microorganisms process is of great potential in remediating Cr(VI)-containing soil.


Assuntos
Solo , Poluentes Químicos da Água , Anaerobiose , Carboximetilcelulose Sódica , Cromo
7.
Water Sci Technol ; 81(7): 1452-1460, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32616697

RESUMO

In the process of preparing magnetic palygorskite from waste pickling liquor of the steel industry, the dosage of NaOH will affect the properties of the magnetic palygorskite. The experimental results showed that magnetic palygorskite can be effectively prepared when NaOH dosage is between 255 and 330 g/L. Vibration sample magnetometry proved that different NaOH dosages can affect the saturation magnetization of magnetic palygorskite. The catalytic performance of five catalysts synthesized with different NaOH dosages hardly changed after five cycles of Fenton-like catalytic degradation of tetracycline (TC). The magnetic palygorskite prepared by this method had good catalytic performance even when the catalyst preparation conditions were magnified ten times, which can provide a reference for large-scale preparation of magnetic palygorskite.


Assuntos
Poluentes Químicos da Água/análise , Compostos de Magnésio , Fenômenos Magnéticos , Compostos de Silício , Hidróxido de Sódio
8.
Water Sci Technol ; 77(5-6): 1622-1631, 2018 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-29595164

RESUMO

In this study, the remediation experiments were performed outdoors in natural conditions. Carboxymethyl cellulose (CMC)-stabilized nanoscale zero-valent iron (CMC-nZVI), biochar (BC) and CMC-stabilized nanoscale zero-valent iron composited with biochar (CMC-nZVI/BC) were synthesized and investigated for their effect on the in situ remediation of hexavalent chromium [Cr(VI)] contaminated soil and the concentration of available iron was tested after the remediation, compared with the untreated soil. The results of toxicity characteristic leaching procedure (TCLP) test showed that CMC-nZVI and CMC-nZVI/BC used as remediation materials could obviously improve the remediation rate of Cr contaminated soil and when the ratio of CMC-nZVI to Fe0 was 2.5 g/Kg, the leachability of Cr(VI) and Crtotal can be reduced by 100% and 95.8% simultaneously. Moreover, sequential extraction procedure (SEP) showed that most exchangeable Cr converted to carbonate-bound and Fe-Mn oxides-bound, reducing the availability and leachability of Cr in the soil.


Assuntos
Cromo/química , Ferro/química , Nanopartículas Metálicas/química , Poluentes do Solo/química , Solo/química , Carboximetilcelulose Sódica , Carvão Vegetal , Poluição Ambiental , Recuperação e Remediação Ambiental , Óxidos
9.
Ecotoxicol Environ Saf ; 132: 224-30, 2016 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-27337496

RESUMO

In this study, a high efficiency and low cost biochar-supported nano-hydroxyapatite (nHAP@BC) material was used in the remediation of lead (Pb)-contaminated soil. The remediation effect of nHAP@BC on Pb-contaminated soil was evaluated through batch experiments. The stability, bioaccessibility of Pb in the soil and the change in soil characteristics are discussed. Furthermore, the effects of the amendments on the growth of cabbage mustard seedlings and the accumulation of Pb were studied. The results showed that the immobilization rates of Pb in the soil were 71.9% and 56.8%, respectively, after a 28 day remediation using 8% nHAP and nHAP@BC materials, and the unit immobilization amount of nHAP@BC was 5.6 times that of nHAP, indicating that nHAP@BC can greatly reduce the cost of remediation of Pb in soil. After the nHAP@BC remediation, the residual fraction Pb increased by 61.4%, which greatly reduced the bioaccessibility of Pb in the soil. Moreover, nHAP@BC could effectively reduce the accumulation of Pb in plants by 31.4%. Overall, nHAP@BC can effectively remediate Pb-contaminated soil and accelerate the recovery of soil fertility.


Assuntos
Carvão Vegetal/química , Durapatita/química , Recuperação e Remediação Ambiental/métodos , Chumbo/química , Nanopartículas/química , Poluentes do Solo/química , Carvão Vegetal/farmacocinética , Durapatita/farmacocinética , Chumbo/farmacocinética , Mostardeira/efeitos dos fármacos , Mostardeira/crescimento & desenvolvimento , Mostardeira/metabolismo , Poluentes do Solo/farmacocinética
10.
Ecotoxicology ; 25(6): 1202-10, 2016 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-27207497

RESUMO

This paper was aimed to study the impact of "ageing" (aged in non-saturated soil for 2 and 4 weeks prior to exposure) nanoscale zero-valent iron (nZVI) on the terrestrial plant. The effects of nZVI on Oryza Sativa germination, seedlings growth, chlorophyll biosynthesis, oxidative stress and the activities of antioxidant enzymes at low (250 mg/kg) and high (1000 mg/kg) concentrations were investigated in this study. The results showed that neither the freshly added nor the "ageing" nZVI to the soil had a significant effect on germination, regardless of concentration. At the low concentration, the freshly added nZVI had no visible toxic effects on the rice seedlings growth, but the rice seedlings exhibited obvious toxic symptoms at the high concentration. At the high concentration, toxicity effects of nZVI were reduced after aging with 2 and 4 weeks in soils compared to fresh nZVI, but the "ageing" nZVI continued to significantly inhibit the rice seedlings growth compared with the control, and the inhibition rates of 2 and 4-week-old nZVI were not significantly different. The mechanism of ageing decreased the phytotoxicity of nZVI was due to nZVI particles incomplete oxidation, and some of which had remained in the soil after 4 weeks aged.


Assuntos
Ferro/toxicidade , Nanopartículas Metálicas/toxicidade , Oryza/efeitos dos fármacos , Poluentes do Solo/toxicidade , Recuperação e Remediação Ambiental , Germinação , Ferro/química , Nanopartículas Metálicas/química , Oxirredução , Plântula , Solo , Poluentes do Solo/química
11.
J Environ Manage ; 166: 478-83, 2016 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-26560640

RESUMO

Polybrominated diphenyl ethers (PBDEs) are a new class of environmental pollutants which easily accumulated in the soil, especially at e-waste sites. However, knowledge about their phytotoxicity after degradation is not well understood. Nano zero valent iron (nZVI) immobilized in mesoporous silica microspheres covered with FeOOH (SiO2@FeOOH@Fe) synthesized in this study was utilized to remove decabromodiphenyl ether (BDE209) from soil. Results revealed that the removal efficiency of BDE209 can be achieved 78% within 120 h using a dosage of 0.165 g g(-1) and a pH of 5.42. Furthermore, the removal efficiency enhanced with increasing soil moisture content and the decreasing of initial BDE209 concentration. Phytotoxicity assays (biomass and germination rate, shoots and roots elongation of Chinese cabbage) were carried out to provide a preliminary risk assessment of treated soil for the application of SiO2@FeOOH@Fe.


Assuntos
Recuperação e Remediação Ambiental/métodos , Éteres Difenil Halogenados , Ferro , Nanopartículas Metálicas , Poluentes do Solo , Testes de Toxicidade/métodos , Brassica/efeitos dos fármacos , Brassica/crescimento & desenvolvimento , Éteres Difenil Halogenados/toxicidade , Ferro/química , Nanopartículas Metálicas/química , Microesferas , Raízes de Plantas/efeitos dos fármacos , Raízes de Plantas/crescimento & desenvolvimento , Dióxido de Silício/química , Poluentes do Solo/toxicidade
12.
J Environ Manage ; 182: 247-251, 2016 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-27479241

RESUMO

In this study, a kind of biochar-supported nano-hydroxyapatite (nHAP@BC) material was used in in-situ remediation of lead-contaminated soil. Column experiments were performed to compare the mobility of nHAP@BC and Bare-nHAP. The immobilization, accumulation and toxic effects of Pb in the after-amended soil were assessed by the in vitro toxicity tests and pot experiments. The column experiments showed a significant improvement in the mobility of nHAP@BC. The immobilization rate of Pb in the soil was 74.8% after nHAP@BC remediation. Sequential extraction procedures revealed that the residual fraction of Pb increased by 66.6% after nHAP@BC remediation, which greatly reduced the bioavailability of Pb in the soil. In addition, pot experiments indicated that nHAP@BC could effectively reduce the upward translocation capacity of Pb in a soil-plant system. The concentration of Pb in the aerial part of the cabbage mustard was 0.1 mg/kg, which is lower than the tolerance limit (0.3 mg/kg). nHAP@BC can remediate Pb-contaminated soil effectively, which can restore soil quality for planting.


Assuntos
Carvão Vegetal/química , Durapatita/química , Chumbo/análise , Nanoestruturas/química , Poluentes do Solo/análise , Solo/química , Brassica/química , Poluição Ambiental/análise , Poluição Ambiental/prevenção & controle , Mostardeira/química
13.
Water Sci Technol ; 71(12): 1800-5, 2015.
Artigo em Inglês | MEDLINE | ID: mdl-26067499

RESUMO

Effective in situ remediation of groundwater requires the successful delivery of reactive iron particles through sand. However, the agglomeration of nano zero-valent iron (NZVI) particles limits the migration distance, which inhibits their usefulness. In the study described herein, NZVI supported by mesoporous silica microspheres covered with FeOOH (SiO2@FeOOH@Fe) was synthesized, and its mobility was demonstrated on the basis of transport in porous media. Degradation of decabromodiphenyl ether (BDE209) was more efficient by SiO2@FeOOH@Fe than by 'bare' NZVI. Breakthrough curves and mass recovery showed the mobility of SiO2@FeOOH@Fe in granular media was better than that of bare NZVI. It increased greatly in the presence of natural organic matter (NOM) and decreased when high Ca2+ and Mg2+ concentrations were encountered. Analysis of the transport data on the basis of filtration theory showed diffusion to be the main mechanism for particle removal in silicon sand. Increasing the NOM may decrease agglomeration of the grains of sand, which has a positive effect on the mobility of SiO2@FeOOH@Fe. Presumably, increasing the concentrations of Ca2+ and Mg2+ compresses the diffuse double layer of SiO2@FeOOH@Fe, resulting in a reduction of mobility.


Assuntos
Ferro/química , Nanopartículas Metálicas/química , Microesferas , Dióxido de Silício/química , Recuperação e Remediação Ambiental/métodos , Filtração/instrumentação , Filtração/métodos , Água Subterrânea
14.
Environ Sci Pollut Res Int ; 31(43): 55422-55436, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39230818

RESUMO

Phyllanthus emblica L. fruit extract (PFE) was introduced to improve ZVI/H2O2 technology, and the efficiency and mechanism of PFE promoting ZVI/H2O2 technology were explored. With the introduction of PFE, the Norfloxacin (NOR) removal rate and kobs of the process were improved by 41.17% and 5.08 times, respectively. In the ZVI/H2O2/PFE process, the degradation of NOR by the attack of ROS is the main pathway for decontamination and is dominated by the heterogeneous reaction on the catalyst surface. PFE contains 13.92 g/L titratable acid and has good complexing ability and antioxidant ability. The mechanism of PFE promoting ZVI/H2O2 technology was based on lowering the pH, complemented by chelation and antioxidant capacity. With the introduction of PFE, the utilization rate of the reagent was significantly increased (7.56 times for ZVI and 3.21 times for H2O2), the applicable pH range was widened (6-9) and the iron sludge was reduced (32.80%). Meanwhile, the concept of UPR is proposed for the first time. The result is the key role to the selection of green promoters in the ZVI/H2O2 process depends on the abundance of titratable acid, followed by a certain chelating ability and antioxidant capacity.


Assuntos
Antioxidantes , Quelantes , Frutas , Peróxido de Hidrogênio , Phyllanthus emblica , Extratos Vegetais , Phyllanthus emblica/química , Peróxido de Hidrogênio/química , Extratos Vegetais/química , Frutas/química , Quelantes/química
15.
Bioresour Technol ; 395: 130394, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38301940

RESUMO

Molecularly imprinted magnetic biochar (MBC@MIPs) was synthesized through molecular imprinting precipitation polymerization. This material demonstrated a selective adsorption capacity of oxytetracycline (OTC) from water samples. Upon characterization of MBC@MIPs, results revealed the formation of a memory cavity shell layer on the magnetic biochar's surface, exhibiting a distinctive recognition effect alongside commendable magnetic and thermal stability. Analysis of the adsorption kinetics indicated that the OTC adsorption process aligned well with the pseudo-second-order rate equation, with chemisorption acting as the predominant mechanism for antibiotic adsorption onto MBC@MIPs. The data could be well described by the Langmuir isotherm model. At 299 K, MBC@MIPs showed a maximum binding capacity of 67.89 mg·g-1, surpassing that of MBC (38.84 mg·g-1) by 1.77 times. MBC@MIPs exhibited the highest selectivity towards OTC, with an imprinting factor (IF) of 5.64. Even amidst interference from antibiotics, MBC@MIPs maintained a significant adsorption capacity for OTC (6.10 mg·g-1), with IF of 6.70.


Assuntos
Carvão Vegetal , Impressão Molecular , Oxitetraciclina , Polímeros/química , Antibacterianos , Adsorção , Fenômenos Magnéticos
16.
Sci Total Environ ; 914: 169820, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38199363

RESUMO

The conventional ZVI/H2O2 technology suffers from poor reagent utilization, excess iron sludge generation, and strong low pH dependence. Therefore, eucalyptus leaf extract (ELE) was introduced to improve ZVI/H2O2 technology, and the efficacy and mechanism of ELE promoting ZVI/H2O2 technology were deeply explored. The results showed that the norfloxacin (NOR) removal and kobs of the ZVI/H2O2/ELE process were enhanced by 35.64 % and 3.27 times, respectively, compared to the ZVI/H2O2 process. In the ZVI/H2O2 process, the production of three reactive oxygen species (ROS: 1O2,·O2-,·OH) was effectively promoted by ELE so that the reaction efficacy was significantly enhanced. Moreover, the attack and degradation of pollutants by ROS was the main way to remove pollutants. With the introduction of ELE, the reactive sites on the catalyst appearance were increased to some extent, and the Fe(III)/Fe(II) cycle was improved. The analysis showed that ELE is rich in titratable acids and the ZVI/H2O2 technology is promoted mainly by lowering the pH of the process. In addition, the chelation of ELE and the reduction in pH by the ELE synergistically enhanced the ZVI/H2O2 technology, which significantly improved the reagent utilization (4.70 times for ZVI and 3.03 times for H2O2), broadened the pH range of the technology (6-9) and was able to effectively reduce the iron sludge contamination (30.33 %) of the process. Therefore, the study offers an important value to study eucalyptus leaves in micron-scale ZVI-Fenton technology.


Assuntos
Poluentes Ambientais , Eucalyptus , Poluentes Químicos da Água , Norfloxacino , Poluentes Químicos da Água/química , Peróxido de Hidrogênio/química , Esgotos , Espécies Reativas de Oxigênio , Compostos Férricos , Ferro/química , Extratos Vegetais
17.
J Hazard Mater ; 480: 135851, 2024 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-39298950

RESUMO

Oxalic acid-modified ball-milled zero-valent iron (OA-ZVIbm) was employed to activate sodium chlorite (ClO2-) for the removal of norfloxacin (NOR). The complete removal of 20 mg/L NOR was achieved within 60 min by the OA-ZVIbm/ClO2- process. Compared with the ZVIbm/ClO2- process which was the ball-milled zero-valent iron (ZVIbm) activate sodium chlorite, the reaction activity of the OA-ZVIbm/ClO2- process was increased by 102.6 times. Through scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), electrochemical testing, and density functional theory (DFT) calculations, which has been confirmed that the introduction of oxalic acid can significantly increase the surface Fe(II) content of OA-ZVIbm, and accelerate the electron transfer rate of iron nuclei, thereby improve the efficiency of ClO2- activation for the removal of NOR. The role of various active species in NOR removal, which were •O2-, 1O2, Fe(IV), ClO2, and •OH, was elucidated through free radical quenching experiments, electron paramagnetic resonance (EPR) spectroscopy, and quantitative detection of active species. These active species all participated in the reaction, while •O2- played a dominant role in the reaction because it could transform into other active species, such as (•OH, 1O2). Inorganic anions and natural organic matter have no significant effect on the removal of NOR in the OA-ZVIbm/ClO2- process. The protonation of oxalic acid ensured its good pH applicability range (pH = 2-11), thus exhibiting excellent performance in NOR removal in real water bodies. This further demonstrates that OA-ZVIbm prepared by oxalic acid ball milling modification is an efficient ClO2- activator, offering promising prospects for antibiotic removal technology.

18.
Bioresour Technol ; 402: 130755, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38688394

RESUMO

Carbothermal reduction is a promising method for the industrial preparation of nano-zero-valent iron. Preparing it also involves very high pyrolysis temperatures, which leads to a significant amount of energy consumption. The temperature required for the preparation of nano-zero-valent iron by carbothermal reduction was reduced by 200 °C by the addition of sodium salt. Carbon-loaded nano zero-valent iron (Fe0/CB-Na) was prepared by carbothermal reduction through the addition of sodium salt. The results showed that Fe0/CB-Na@700 had the same activation performance as Fe0/CB@900 and the newly prepared nano-zero-valent iron. The addition of sodium salt promoted the transfer of oxygen from the iron oxide to the carbon structure during the roasting process so that the iron oxide was reduced to as much Fe0 as possible. Thus, sodium salts were optimized for the preparation of nano-zero-valent iron by carbothermal reduction through interfacial amorphization and oxygen transfer, thus reducing the preparation cost.


Assuntos
Antibacterianos , Ferro , Ferro/química , Antibacterianos/química , Sulfatos/química , Oxirredução , Temperatura , Sódio/química
19.
J Hazard Mater ; 465: 133309, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38185080

RESUMO

The utilization of nano zero-valent iron (nZVI) in polybrominated diphenyl ethers remediation has been studied extensively. However, challenges in balancing cost and reactivity have been encountered. A submicron zero-valent iron coated with FeC2O4·2 H2O layers (OX-smZVI) was synthesized via a mechanochemical method, aiming to resolve this contradiction. Characterization via SEM, TEM, and XPS confirmed the structure as FeC2O4·2 H2O coated iron lamellate with a surface area 24-fold higher than ball-milled zero-valent iron (smZVI). XRD highlighted an Fe/C eutectic in OX-smZVI, boosting its electron transfer capacity. Decabromodiphenyl ether degradation by OX-smZVI follows a two-stage process, with initial degradation by FeC2O4·2 H2O and a subsequent phase dominated by electron transfer. OX-smZVI exhibits a 4.52-34.40 times faster BDE209 removal rate than nZVI and scaled-up OX-smZVI displayed superior reactivity with preparation costs only 1/680 of nZVI. Given its enhanced reactivity and cost-efficiency, OX-smZVI emerges as a promising replacement for nZVI.

20.
Sci Total Environ ; 916: 170312, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38278274

RESUMO

In this study, lanthanum-doped magnetic biochar (LaMBC) was synthesized from bagasse by co-doping iron salt and lanthanum salt, and it was characterized for its application in the activation of persulfate (PS) in the degradation of Florfenicol (FLO). The results indicated that the LaMBC/PS system consistently achieved a degradation efficiency of over 99.5 %, with a reaction rate constant 4.71 times as that of MBC. The mechanism of FLO degradation suggested that O2•- and •OH played dominant roles, contributing 40.92 % and 36.96 %, respectively, during FLO degradation. Through physicochemical characterization and quenching experiments, it can be concluded that the key reasons for the enhancement of MBC activation performance are as follows: (1) Lanthanum doping in magnetized biochar increased the Fe(II) content in MBC. (2) Lanthanum doping significantly improved the adsorption capacity of LaMBC, increased the concentration of pollutants on the catalyst surface and effectively enhancing the reaction rate. (3) Lanthanum doping effectively increased the surface Fe(II) content during the reaction process in LaMBC, promoted the generation of active oxygen species in PS. This study delves into synthesizing and applying LaMBC for PS activation and FLO removal. The emphasis is on comprehensively characterizing and experimenting to elucidate the mechanism, proposing an innovative approach for efficiently degrading antibiotic wastewater.


Assuntos
Lantânio , Tianfenicol/análogos & derivados , Poluentes Químicos da Água , Carvão Vegetal/química , Fenômenos Magnéticos , Compostos Ferrosos , Poluentes Químicos da Água/análise
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