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1.
Environ Sci Technol ; 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39190653

RESUMO

Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), as a promising technology for water decontamination, are constrained by low reaction kinetics due to limited reaction selectivity and mass transfer. Herein, we designed a nanoconfined FeCo2O4-embedded ceramic membrane (FeCo2O4-CM) under flow-through pattern for PMS activation. Confining PMS and FeCo2O4 within nanochannels (3.0-4.7 nm) enhanced adsorption interactions (-7.84 eV vs -2.20 eV), thus boosting mass transfer. Nanoconfinement effect regulated electron transfer pathways from PMS to FeCo2O4-CM by modulating the active site transformation to ≡Co(III) in nanoconfined FeCo2O4-CM, enabling selectively generating 1O2. The primary role of 1O2 in the nanoconfined system was confirmed by kinetic solvent isotope experiments and indicative anthracene endoperoxide (DPAO2). The system enabled 100% removal of atrazine (ATZ) within a hydraulic retention time of 2.124 ms, demonstrating a rate constant over 5 orders of magnitude higher than the nonconfined system (3.50 × 103 s-1 vs 0.42 min-1). It also exhibited strong resilience to pH variations (3.3-9.0) and coexisting substances, demonstrating excellent stability indicated by consistent 100% ATZ removal for 14 days. This study sheds light on regulating electron transfer pathways to selectively generate 1O2 through the nanoconfinement effect, boosting the practical application of PMS-based AOPs in environmental remediation and potentially applying them to various other AOPs.

2.
Environ Res ; 262(Pt 2): 119925, 2024 Sep 12.
Artigo em Inglês | MEDLINE | ID: mdl-39276840

RESUMO

To address the issues of ZVI's susceptibility to oxidation and aggregation, ball milling and Na2S·9H2O modification were employed on ZVI to enhance its efficiency in removing Cr(VI) from effluent. The characterization results expressed that S-mZVIbm had mesoporous and macroporous structures, enabling successful capture of Cr(VI). Moreover, S-mZVIbm had the highest adsorption capacity for Cr(VI) (350.04 mg/g) at pH = 2.00 and reached kinetic equilibrium within 420 min. Furthermore, the adsorption of Cr(VI) by S-mZVIbm conformed to the Avrami-fractional-order model, demonstrated that the adsorption process indicated a complex multi-adsorption process. Meanwhile, the adsorption also fit to Langmuir and Sips models, suggesting monolayer-level adsorption with heterogeneous sites located on S-mZVIbm. The S-mZVIbm could enhance Cr(VI) adsorption through various synergistic mechanisms, such as electrostatic interaction, chemical precipitation, surface complexation, and reduction. Overall, this research presented an innovative perspective for the modification of ZVI, and S-mZVIbm could be widely applied in the practical remediation of wastewater containing Cr(VI).

3.
Environ Res ; 212(Pt B): 113287, 2022 09.
Artigo em Inglês | MEDLINE | ID: mdl-35483407

RESUMO

Dielectric barrier discharge plasma (DBDP) is an emerging and promising advanced oxidation process (AOP) for wastewater treatment. After investigating the effect of input voltage, O3 (generated by dielectric barrier discharge), and peroxydisulfate (PDS) dosage, the DBDPO3/PDS system was established. With the assistance of PDS, the atrazine (ATZ) removal efficiency increased from 69.67% to 82.46% within 25 min. Synergistic effect calculation suggests that there were markedly synergies between DBDP, O3, and PDS. Under the effect of SO4-•, the total organic carbon (TOC) removal and dechlorination efficiency were significantly improved. In addition, the DBDPO3/PDS system maintained the ATZ removal efficiency at a high level over a wide range of initial pH values. According to quenching experiments and electron paramagnetic resonance (EPR) detection, the dominant radical for ATZ degradation in the DBDPO3/PDS system was HO•. A possible degradation pathway of ATZ was proposed based on density functional theory (DFT) analysis, quadrupole-time of flight-liquid chromatography/mass spectrometry (Q-TOF-LC/MS) results, and related literature. The acute toxicity to aquatic minnows and the developmental toxicity of intermediate products prediction confirmed that the DBDPO3/PDS system could effectively reduce ATZ toxicity. The electrical energy per order (EEO) was 7.10 kWh m-3 order-1 illustrating that the DBDPO3/PDS was a more energy-economic system than other energy-intensive processing technologies.


Assuntos
Atrazina , Poluentes Químicos da Água , Purificação da Água , Atrazina/análise , Atrazina/toxicidade , Cromatografia Líquida , Oxirredução , Poluentes Químicos da Água/análise , Purificação da Água/métodos
4.
Phys Chem Chem Phys ; 20(27): 18601-18609, 2018 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-29953161

RESUMO

A series of Fe-doped ZnS (Fex-ZnS) photocatalysts were synthesized using a one-pot hydrothermal method. The physicochemical properties of the as-prepared Fex-ZnS microspheres were characterized by different microscopic and spectroscopic techniques. Fe doping did not obviously change the morphology and crystallinity of ZnS, but effectively broadened the light response range into the visible-light region. Degradation of p-nitrophenol (PNP) was used to evaluate the photocatalytic performance of the Fex-ZnS catalysts under visible light irradiation with the addition of H2O2 to facilitate photo-Fenton-like reactions. The highest PNP removal rate of 83.8% after 180 min of irradiation was achieved under the optimal conditions, including a doping ratio of 6%, a H2O2 concentration of 3 mmol L-1 and a catalyst dosage of 0.8 g L-1. The effects of aqueous/solid mass transfer and intraparticle mass transfer limitations on the PNP degradation reactions were analyzed, indicating that the variations of catalyst size caused by different Fe doping ratios did not affect the photocatalytic reactions in this study. The PNP removal mechanism of the Fex-ZnS photocatalyst with H2O2 addition under visible light irradiation was proposed.

5.
Photochem Photobiol Sci ; 15(8): 1046-53, 2016 08 04.
Artigo em Inglês | MEDLINE | ID: mdl-27436621

RESUMO

This work investigated the effects of organic acids and initial solution pH on the photodegradation of BPA in a photo-Fenton-like process using α-FeOOH as a catalyst. The results showed that the addition of different organic acids affected the formation of the ferric-carboxylate complexes and free radicals, which in turn varied the photodegradation efficacy. Compared with the other acids, oxalic acid (OA) was found to be the most effective in enhancing the photodegradation of BPA, which strongly depends on the OA concentration. Particularly, the addition of OA could significantly extend the working pH from an acidic to a neutral range for the photocatalytic process and thus the acidification pretreatment may not be needed. A high photocatalytic degradation of BPA occurred at pH 6.0, due to the formation of ferric-oxalate complexes and ˙OH radicals in the synergistic interactions of OA and α-FeOOH. This finding highlights that the oxalate-promoted photo-Fenton-like process using the α-FeOOH catalyst may be used for wastewater treatment without pH adjustment.

6.
Environ Sci Pollut Res Int ; 31(13): 20621-20636, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38381294

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) in soil are potentially harmful to human health. However, the use of photocatalysis technology to treat soil contaminated with PAHs remains challenging. Therefore, TiO2/α-FeOOH composite photocatalyst has been synthesized by hydrothermal method and sol-gel method and applied to photocatalytic degradation of fluoranthene in soil. The morphology, elements, crystal structure, optical properties, electrochemical characteristics, and photocatalytic activity of TiO2/α-FeOOH have been characterized. Results showed that TiO2 is tightly fixed on the surface of α-FeOOH, and TiO2/α-FeOOH had higher photocatalytic activity on photocatalytic degradation of fluoranthene in soil under simulated sunlight. The degradation efficiency of TiO2/α-FeOOH is 3.0 and 4.8 times higher than that of TiO2 and α-FeOOH, respectively. This is attributed to enhanced photocatalytic ability by enhancing the transfer capacity of electrons and holes and broadening the spectrum absorption range. The highest degradation efficiency was achieved when the pH of the soil is neutral, the ratio of water/soil is 10:1, and the dosage of catalyst is 50 mg/g. In addition, it was proved that •O2-, h+, and 1O2 are the main active substances in the photocatalysis of TiO2/α-FeOOH. The possible mechanism of a Z-type electron transfer structure was also proposed. The degradation products of fluoranthene were detected, and the degradation pathway was deduced.


Assuntos
Compostos de Ferro , Minerais , Hidrocarbonetos Policíclicos Aromáticos , Solo , Humanos , Fluorenos , Luz Solar
7.
Bioresour Technol ; 407: 131075, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38996847

RESUMO

Phosphorus (P) plays a crucial role in plant growth, which can provide nutrients for plants. Nonetheless, excessive phosphate can cause eutrophication of water, deterioration of aquatic environment, and even harm for human health. Therefore, adopting feasible adsorption technology to remove phosphate from water is necessary. Biochar (BC) has received wide attention for its low cost and environment-friendly properties. However, undeveloped pore structure and limited surface groups of primary BC result in poor uptake performance. Consequently, this work introduced the synthesis of pristine BC, parameters influencing phosphate removal, and corresponding mechanisms. Moreover, multifarious metal-doped BCs were summarized with related design principles. Meanwhile, mechanisms of selective phosphate adsorption by metal-doped BC were investigated deeply, and the recovery of phosphate from water, and the utilization of phosphate-loaded adsorbents in soil were critically presented. Finally, challenges and prospects for widespread applications of selective phosphate adsorption were proposed in the future.


Assuntos
Carvão Vegetal , Fosfatos , Poluentes Químicos da Água , Purificação da Água , Carvão Vegetal/química , Fosfatos/química , Adsorção , Purificação da Água/métodos , Metais/química , Água/química , Reciclagem
8.
J Colloid Interface Sci ; 658: 286-300, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38109816

RESUMO

The self-sufficient heterogeneous photo-Fenton (SH-PF) system was constructed for doxycycline hydrochloride (DOH) degradation with hydroxyapatite (Hap) modified CuFeO2 (Hap/CuFeO2) composites through H2O2 in-situ production. The modification of Hap could improve the specific surface area, visible-light response, light conversion efficiency, photoelectron lifetime and oxygen vacancies (OVs) of CuFeO2, which was conducive to H2O2 production and DOH degradation in SH-PF system. Notably, Hap/CuFeO2 fabricated with 0.5 g Hap (Hap/CuFeO2-0.5) displayed more superior performance for DOH degradation compared to other synthesized catalysts. The Hap/CuFeO2-0.5 load and initial solution pH for DOH degradation in SH-PF system were optimized, and the Hap/CuFeO2-0.5 had good reusability and stability. The •OH was the main active species for DOH degradation, and the facilitation effect of •O2- and photoelectrons on DOH degradation was associated with the H2O2 production in the present work. In addition, the capture of photogenerated holes suppressed the recombination of photogenerated carriers, elevating the production of photoelectrons and thereby enhancing H2O2 production and DOH degradation. The degradation pathways for DOH were proposed and the comprehensive toxicities of DOH were relieved after degradation in SH-PF system.

9.
J Hazard Mater ; 459: 132199, 2023 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-37541123

RESUMO

Activated peroxymonosulfate (PMS) processes have emerged as an efficient advanced oxidation process to eliminate refractory organic pollutants in water. This study synthesized a novel spherical manganese oxide catalyst (0.4KBr-ß-MnO2) via a simple KBr-guided approach to activate PMS for degrading dimethyl phthalate (DMP). The 0.4KBr-ß-MnO2/PMS system enhanced DMP degradation under different water quality conditions, exhibiting an ultrahigh and stable catalytic activity, outperforming equivalent quantities of pristine ß-MnO2 by 8.5 times. Mn(V) was the dominant reactive species that was revealed by the generation of methyl phenyl sulfone from methyl phenyl sulfoxide oxidation. The selectivity of Mn(V) was demonstrated by the negligible inhibitory effects of Inorganic anions. Theoretical calculations confirmed that Mn (V) was more prone to attack the CO bond of the side chain of DMP. This study revealed the indispensable roles of high-valent manganese species in DMP degradation by the 0.4KBr-ß-MnO2/PMS system. The findings could provide insight into effective PMS activation by Mn-based catalysts to efficiently degrade pollutants in water via the high-valent manganese species.

10.
J Hazard Mater ; 451: 130901, 2023 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-36881985

RESUMO

The sulfate radical-based advanced oxidation processes (SR-AOPs) offer huge potential for the removal of organic pollutants. In this study, Co(II)-intercalated δ-MnO2 (Co-δ-MnO2) catalyst was successfully prepared by a simple cation exchange reaction. The obtained Co-δ-MnO2 exhibited high catalytic performance for the removal of dimethyl phthalate (DMP) under the activation of peroxymonosulfate (PMS), with the degradation efficiency reaching 100% within 6 h. Experiments and theoretical calculations revealed that interlayer Co(II) provided unique active sites in Co-δ-MnO2. In addition, radical and non-radical pathways were confirmed to play a role in Co-δ-MnO2/PMS system. •OH, SO4• ̶, and 1O2 were identified to be the dominating reactive species in Co-δ-MnO2/PMS system. This study provided new insights into the design of catalysts and laid a foundation for developing modifiable layered heterogeneous catalysts.

11.
Water Res ; 235: 119843, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-36934540

RESUMO

Peroxymonosulfate (PMS) activation is a promising technology for water purification, but the removal performance of multiple pollutant matrices and the mechanism for reactive species transformation in the heterogeneous catalytic system remain ambiguous. Herein, a novel CuFe2O4/diatomite was fabricated for PMS activation to achieve efficient removal of typical pesticides. Uniform distribution of CuFe2O4 on diatomite efficiently alleviated the agglomeration of CuFe2O4 and increased specific surface area (57.20 m2 g-1, 3.8-fold larger than CuFe2O4). CuFe2O4/5% diatomite (5-CFD)/PMS system showed nearly 100% removal efficiency for mixed pesticide solution within 10 min (0.10 g L-1 5-CFD and 0.40 g L-1 PMS) and excellent anti-interference performance towards various coexisting substances (≥90% removal efficiency). The electrochemical measurements confirmed that the lower charge transfer resistance of 5-CFD significantly enhanced the electron-transfer capacity between 5-CFD and PMS, accelerating the reactions among Fe(III)/Fe(II), Cu(II)/Cu(I), and PMS, further generating •OH (261.3 µM), 1O2 (138.8 µM), SO4•- (11.8 µM), and O2•-. The O in reactive oxygen species didn't originate from dissolved oxygen (DO) but PMS, independent of the low solubility of DO and slow diffusion rate of O2 in water. Furthermore, the production of 1O2 went through the process: PMS â†’ O2•- â†’ 1O2, and SO4•- could rapidly convert into •OH. The degradation pathways and the evolution of intermediates were proposed by HPLC-QTOF-MS/MS and DFT calculations. QSAR analysis illustrated that the toxicity became lower with the reaction process. This study provides novel insights into the mechanism for pesticide degradation and active species transformation and the anti-interference capability of systems.


Assuntos
Compostos Férricos , Poluentes Químicos da Água , Espectrometria de Massas em Tandem , Poluentes Químicos da Água/química , Peróxidos/química
12.
J Hazard Mater ; 451: 131154, 2023 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-36889068

RESUMO

A novel Bi2WO6-g-C3N4/polyvinylidene fluoride (PVDF) composite ultrafiltration (UF) membrane (BWO-CN/PVDF) was prepared by microwave hydrothermal and immersion precipitation phase transformation method. The BWO-CN/PVDF-0.10 exhibited an outstanding photocatalytic removal rate of atrazine (ATZ) (97.65 %) under the simulated sunlight and enhanced permeate flux (1356.09 L·m-2·h-1). The multiple optical and electrochemical detection confirmed that combining ultrathin g-C3N4 and Bi2WO6 can increase carrier separation rate and prolong its lifetime. The quenching test revealed that h+ and 1O2 were the prominent reactive species. Additionally, after a 10-cycle photocatalytic process, the BWO-CN/PVDF membrane presented remarkable reusability and durability. And it showed excellent anti-fouling performance by filtering BSA, HA, SA, and Songhua River under simulated solar irradiation. The molecular dynamic (MD) simulation showed that the combination of g-C3N4 and Bi2WO6 can enhance the interaction between BWO-CN and PVDF. This work opens up a new idea for designing and constructing a highly efficient photocatalytic membrane for water treatment.

13.
Environ Sci Pollut Res Int ; 30(27): 70260-70276, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37147542

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) in soil have potential harm on human health. However, remediation of PAH-contaminated soils through photocatalytic technology remains a challenge. Therefore, the photocatalyst g-C3N4/α-Fe2O3 was synthesized and applied to photocatalytic degradation of fluoranthene in soil. The physicochemical properties of g-C3N4/α-Fe2O3 and various degradation parameters, such as catalyst dosage, the ratio of water/soil, and initial pH, were investigated in detail. In soil slurry reaction system (water/soil=10:1, w/w), the optimal degradation efficiency on fluoranthene was 88.7% after simulated sunlight irradiation for 12 h (contaminated soil=2 g, initial fluoranthene concentration=36 mg/kg, catalyst dosage=5%, and pH=6.8), and the photocatalytic degradation followed pseudo-first-order kinetics. The degradation efficiency of g-C3N4/α-Fe2O3 was higher compared with P25. Degradation mechanism analysis showed that •O2- and h+ are the main active species in photocatalytic degradation process of fluoranthene by g-C3N4/α-Fe2O3. Coupling g-C3N4 and α-Fe2O3 enhances the interfacial charge transport capacity via Z-scheme charge transfer route and inhibits the recombination of photogenerated electrons and holes of g-C3N4 and α-Fe2O3, then significantly improves the production of active species and photocatalytic activity. Results showed that photocatalytic treatment of soil by g-C3N4/α-Fe2O3 is an effective strategy for remediation of soils contaminated by PAHs.


Assuntos
Luz Solar , Humanos , Catálise
14.
Environ Pollut ; 306: 119457, 2022 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-35561795

RESUMO

Herein, magnetic porous pinecone-derived hydrochar (MPHCMW) co-activated by KHCO3 and K2FeO4 through one-step microwave-assisted pyrolysis was innovatively synthesized for hexavalent chromium (Cr(VI)) and anthracene (ANT) removal from water. The analyses of characterization consequences and co-activation mechanisms not merely proved the high specific surface area (703.97 m2/g) and remarkable microporous structures of MPHCMW caused by the synergistic chemical activation of KHCO3 and K2FeO4, but also testified successful loading of Fe0 and Fe3O4 on MPHCMW by the process of carbothermal reduction between K2FeO4 and carbon matrix of hydrochar. The resultant MPHCMW possessed pH-dependence for Cr(VI), while adsorption for ANT was hardly impacted by the pH of solution. Moreover, the adsorption processes of MPHCMW could attain equilibrium within 60 min for Cr(VI) and 30 min for ANT with multiple kinetics, and the corresponding adsorption capacity for Cr(VI) and ANT was 128.15 and 60.70 mg/g, respectively. Additionally, the adsorption percentages of MPBCMW for Cr(VI)/ANT was maintained at 87.87/82.64% after three times of adsorption-desorption cycles. Furthermore, pore filling, complexation, electrostatic interaction, reduction and ion exchange were testified to enhance the removal of Cr(VI), while the ANT removal was achieved via π-π stacking, complexation, pore filling and hydrogen bonding force.


Assuntos
Poluentes Químicos da Água , Água , Adsorção , Antracenos/análise , Cromo/química , Concentração de Íons de Hidrogênio , Cinética , Fenômenos Magnéticos , Porosidade , Poluentes Químicos da Água/análise
15.
J Hazard Mater ; 432: 128758, 2022 06 15.
Artigo em Inglês | MEDLINE | ID: mdl-35395706

RESUMO

Coexistence of heavy metals and endocrine disrupting compounds in polluted water with competitive adsorption behavior necessitates design of tailored adsorbents. In this work, ß-cyclodextrin modified magnetic rice husk-derived cellulose (ß-CD@MRHC) which can provide independent functional sites for effectively binding the above two types of contaminants was synthesized and used for Pb(II) and BPA elimination in both unit and multivariate systems. Characterizations results confirmed successful ß-CD grafting and Fe3O4 loading, and the ß-CD@MRHC had excellent magnetic property for its effectively recovery from water, which was not affected by the adsorption of pollutants. The ß-CD@MRHC possessed superior adsorption performance with maximal Pb(II)/BPA uptake of 266.2 or 412.8 mg/g, severally, and the adsorption equilibrium was fleetly reached in 30 and 7.5 min. Moreover, the ß-CD@MRHC could accomplish synergetic Pb(II) and BPA elimination through averting their competitive behaviors owing to diverse capture mechanisms for Pb(II) (ion exchange, complexation and electrostatic attraction) and BPA (hydrogen bonding and host-guest inclusion). Furthermore, after three cycles of step-wise desorption, the binding of Pb(II) as well as BPA byß-CD@MRHC dropped slightly in dualistic condition. In summary, ß-CD@MRHC was a promising tailored adsorbent to practical application for simultaneously removing heavy metals and organic matters from wastewater with high-performance magnetic recovery.


Assuntos
Metais Pesados , Poluentes Químicos da Água , beta-Ciclodextrinas , Adsorção , Compostos Benzidrílicos , Celulose/química , Cinética , Chumbo , Fenômenos Magnéticos , Fenóis , Água , Poluentes Químicos da Água/química , beta-Ciclodextrinas/química
16.
J Hazard Mater ; 423(Pt A): 127043, 2022 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-34479084

RESUMO

Bioremediation by phosphate-solubilizing bacteria (PSB) has attracted extensive attentions due to its economical and eco-friendly properties for lead (Pb) passivation in soil. Herein, bone char (BC) supported biochemical composite (CFB1-P) carrying advantages of BC, PSB, iron sulfide (FeS) and carboxymethyl cellulose (CMC) was designed and applied to Pb passivation. The composite at a mass ratio of BC:CMC:FeS = 1:1:1 possessed high passivation efficiency (65.47%), and has been demonstrated to offer appropriate habitat environment for PSB to defend against Pb(II) toxicity, thus enhancing the phosphate-solubilizing amount of PSB to 140.72 mg/L for passivating Pb(II). Batch experiments showed that the CFB1-P possessed excellent adsorption properties with maximal monolayer Pb(II) uptake of 452.99 mg/g during an extensive pH range of 2.0-6.0. Furthermore, by applying CFB1-P dosage of 3% into Pb-contaminated soil, the labile Pb fractions were reduced from 29.05% to 6.47% after simulated remediation of 10 days, and converted into steady fractions. The CFB1-P was demonstrated to achieve high Pb(II) passivation through combined functions of chemical precipitation, complexation, electrostatic attraction and biomineralization, accompanied by the formation of more stable crystal structures, for instance, Pb5(PO4)3OH, Pb3(PO4)2 and PbS. These results suggested CFB1-P as a potential alternative for efficient remediation of Pb-contaminated soil.


Assuntos
Poluentes do Solo , Solo , Bactérias , Carboximetilcelulose Sódica , Chumbo , Fosfatos/análise , Poluentes do Solo/análise
17.
J Hazard Mater ; 414: 125602, 2021 07 15.
Artigo em Inglês | MEDLINE | ID: mdl-34030426

RESUMO

The dielectric barrier discharge plasma (DBDP) process has received extensive attention for the removal of organic contaminants from water. A novel microwave-assisted hydrothermal method was used to easily and rapidly synthesize MnFe2O4 catalysts. Based on the DBDP process, MnFe2O4 can enhance 4-fluorophenol (4-FP) abatement from 44.15% to 58.78% through the catalysis within 18 min. Then, the adjunction of O3 generated by discharge can further boost 4-FP degradation to 94.94%. After the whole optimization process is complete, the associated pseudo-first-order reaction kinetic constant and energy efficiency were enhanced from 0.0327 to 0.1536 min-1 and 2067.13 mg kW h-1 to 4444.75 mg kW h-1, respectively. With the help of the condition, blank and radical capture experiments, the catalytic performance caused by MnFe2O4 and O3 was attributed to the joint action of Fenton-like reactions, photocatalysis (ultraviolet, UV), photoassisted Fenton reactions and O3 catalysis. The overall downward trend of the possible intermediate toxicities indicated that the DBDP/MnFe2O4/O3 process can effectively remove and mineralize 4-FP without the generation of more toxic intermediates. In addition, during the 5 cycles, MnFe2O4 can maintain excellent recovery, efficiency and durability. In summary, the coupling of discharge plasma and MnFe2O4 sheds new light on catalysis for wastewater treatment.

18.
J Hazard Mater ; 403: 123607, 2021 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-32791481

RESUMO

For green synthesis of nZVI with low aggregation and high antioxidation, green tea extracts were explored as reductant during the synthesis with modification by hydrophilic porous activated carbon (HPAC) and sulfidation technology. Characterization results identified the effective preparation of porous activated carbon (PAC) with microporous and mesoporous characteristics, and the successful loading of S-nZVI nanoparticles on S-nZVI@HPAC. Moreover, HPAC was identified to have a higher degree of hydrophilicity surface compared to PAC, while the S-nZVI with an atomic ratio of S/Fe (0.16) further improved the hydrophilic performance of S-nZVI@HPAC. Batch adsorption revealed that the S-nZVI@HPAC possessed a pH-dependent adsorption performance with a fast kinetic equilibrium within 120 min and an outstanding Pb(II) binding of 295.30 mg/g at pH = 5.0 and 50 °C. Thermodynamic results exhibited positive ΔH° and ΔS°, clearly indicative of the endothermic property of Pb(II) uptake onto S-nZVI@HPAC with an increase in randomness, while the negative ΔG° uncovered a favorable and spontaneous process. Furthermore, the S-nZVI@HPAC was believed to enhance the Pb(II) uptake via the synergistic effects of electrostatic attraction, chemical precipitation, complexation and reduction. The results of this work highlighted the hydrophilic porous activated carbon supported sulfide nZVI for efficient remediation of Pb(II) contaminated water.

19.
J Hazard Mater ; 403: 124011, 2021 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-33265040

RESUMO

Ag2O/ZnO/rGO heterojunction photocatalysts were synthesized via a rapid microwave hydrothermal method for photocatalytic degradation of bisphenol A (BPA) under simulated solar light. Ag doping efficiently decreased the bandgap of ZnO, and loading on rGO inhibited the recombination of photoinduced electron-hole pairs. The highest BPA removal rate (80%) was achieved with an Ag doping ratio of 5% and a GO loading ratio of 3 wt%. The enhanced photocatalytic performance was attributed to the narrower bandgap and the improved separation efficiency of electron-hole pairs. Moreover, the recycling experiments proved that Ag2O/ZnO/rGO possessed excellent photostability. Hole (h+) and •OH played crucial roles in the photocatalytic system. The degradation pathway of BPA including hydroxylation and the cleavage of covalent bonds was proposed. The toxicity assessment of intermediates elucidated that most of intermediates were less toxic than BPA. The as-prepared Ag2O/ZnO/rGO exhibited outstanding photostability and pH adaptability, having great potential to be applied to the degradation of emerging organic pollutants in wastewater.

20.
Chemosphere ; 240: 124977, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31726600

RESUMO

In this study, Fe3O4 and microwave (MW) were combined to activate persulfate (PS) for the removal of organic matter, resulting in the enhanced degradation of p-nitrophenol (PNP) in solution. During the preparation of Fe3O4, the effect of sodium acetate was examined, and the results showed that the concentration of sodium acetate had little effect on the catalytic activity of the Fe3O4/PS/MW system but did have an effect on the Fe3O4 yield. In addition, with regards to the representative environmental factors, the degradation experiment showed that humic acid and the co-existing anions of chloride, sulfate, nitrate, and phosphate had little effects on p-nitrophenol removal; however, carbonate had a negative effect. In addition, the Fe3O4/PS/MW system performed well in the initial pH range of 3.0-9.0. According to the quenching experiment and electron paramagnetic resonance (EPR) detection, sulfate radicals and a minority of hydroxyl radicals play dominant roles in the degradation process. In addition, the role of Fe3O4 was confirmed to take part in the degradation process by X-ray photoelectron spectroscopy (XPS) analysis. Because of the good performance observed in the water matrices of tap water and the Songhua River, these results demonstrate the potential application of the Fe3O4/PS/MW system for wastewater treatment.


Assuntos
Compostos Férricos/química , Micro-Ondas , Nitrofenóis/química , Poluentes Químicos da Água/química , Catálise , Compostos Férricos/isolamento & purificação , Compostos Férricos/efeitos da radiação , Substâncias Húmicas/análise , Radical Hidroxila/química , Sulfatos/química , Água/química , Poluentes Químicos da Água/análise
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