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1.
J Environ Sci (China) ; 147: 114-130, 2025 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-39003034

RESUMEN

Fenton and Fenton-like processes, which could produce highly reactive species to degrade organic contaminants, have been widely used in the field of wastewater treatment. Therein, the chemistry of Fenton process including the nature of active oxidants, the complicated reactions involved, and the behind reason for its strongly pH-dependent performance, is the basis for the application of Fenton and Fenton-like processes in wastewater treatment. Nevertheless, the conflicting views still exist about the mechanism of the Fenton process. For instance, reaching a unanimous consensus on the nature of active oxidants (hydroxyl radical or tetravalent iron) in this process remains challenging. This review comprehensively examined the mechanism of the Fenton process including the debate on the nature of active oxidants, reactions involved in the Fenton process, and the behind reason for the pH-dependent degradation of contaminants in the Fenton process. Then, we summarized several strategies that promote the Fe(II)/Fe(III) cycle, reduce the competitive consumption of active oxidants by side reactions, and replace the Fenton reagent, thus improving the performance of the Fenton process. Furthermore, advances for the future were proposed including the demand for the high-accuracy identification of active oxidants and taking advantages of the characteristic of target contaminants during the degradation of contaminants by the Fenton process.


Asunto(s)
Peróxido de Hidrógeno , Hierro , Eliminación de Residuos Líquidos , Hierro/química , Peróxido de Hidrógeno/química , Eliminación de Residuos Líquidos/métodos , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/análisis , Aguas Residuales/química , Oxidación-Reducción , Radical Hidroxilo/química
2.
J Environ Sci (China) ; 147: 688-713, 2025 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-39003083

RESUMEN

Innately designed to induce physiological changes, pharmaceuticals are foreknowingly hazardous to the ecosystem. Advanced oxidation processes (AOPs) are recognized as a set of contemporary and highly efficient methods being used as a contrivance for the removal of pharmaceutical residues. Since reactive oxygen species (ROS) are formed in these processes to interact and contribute directly toward the oxidation of target contaminant(s), a profound insight regarding the mechanisms of ROS leading to the degradation of pharmaceuticals is fundamentally significant. The conceptualization of some specific reaction mechanisms allows the design of an effective and safe degradation process that can empirically reduce the environmental impact of the micropollutants. This review mainly deliberates the mechanistic reaction pathways for ROS-mediated degradation of pharmaceuticals often leading to complete mineralization, with a focus on acetaminophen as a drug waste model.


Asunto(s)
Acetaminofén , Especies Reactivas de Oxígeno , Acetaminofén/química , Especies Reactivas de Oxígeno/metabolismo , Contaminantes Químicos del Agua/química , Oxidación-Reducción , Preparaciones Farmacéuticas/metabolismo
3.
J Hazard Mater ; 479: 135686, 2024 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-39236530

RESUMEN

In this study, we selected 13 phenolic compounds containing -COOH, -CHO, -OH, and -COCH3 functional groups as model compounds for dissolved organic matter (DOM), and explored the redox reactions during the co-degradation of phenolic compounds with aniline disinfection by-products (DBPs) at the molecular level. When phenolic compounds and aniline DBPs were degraded, phenoxy radicals and aniline radicals were the most important intermediates. Phenoxy radicals can degrade aniline DBPs via hydrogen atom abstraction (HAA) reactions, and the reaction rates were related to the reduction potentials of the compounds. Compounds containing electron-withdrawing groups were more likely to oxidize aniline DBPs. Aniline DBPs were more easily degraded by phenoxy radicals when they contained electron-donating groups, and the increase in the number of chlorine atoms inhibited the reaction rates of aniline DBPs degradation by phenoxy radicals. Although phenolic compounds can reduce aniline DBPs, there was no significant correlation between the reaction rates and the reduction potentials of the compounds. Considering the redox effects of phenolic compounds on aniline DBPs, co-degradation simulations showed that phenolics inhibited the degradation efficiency of aniline DBPs. This work provided new insights into the transformation mechanisms and degradation efficiencies of DOM and aniline DBPs when they were co-degraded.

4.
Chemosphere ; 364: 143249, 2024 Sep 02.
Artículo en Inglés | MEDLINE | ID: mdl-39233296

RESUMEN

Conventional electro-Fenton (EF) process at acidic pH ∼3 is recognized as a highly effective strategy to degrade organic pollutants; however, homogeneous metal catalysts cannot be employed in more alkaline media. To overcome this limitation, pyrolytic derivatives from metal-organic frameworks (MOFs) have emerged as promising heterogeneous catalysts. Cu-based MOFs were prepared using trimesic acid as the organic ligand and different pyrolysis conditions, yielding a set of nano-Cu/C catalysts that were analyzed by conventional methods. Among them, XPS revealed the surface of the Cu/C-A2-Ar/H2 catalyst was slightly oxidized to Cu(I) and, combined with XRD and HRTEM data, it can be concluded that the catalyst presents a core-shell structure where metallic copper is embedded in a carbon layer. The antihistamine diphenhydramine (DPH), spiked into either synthetic Na2SO4 solutions or actual urban wastewater, was treated in an undivided electrolytic cell equipped with a DSA-Cl2 anode and a commercial air-diffusion cathode able to electrogenerate H2O2. Using Cu/C as suspended catalyst, DPH was completely degraded in both media at pH 6-8, outperforming the EF process with Fe2+ catalyst at pH 3 in terms of degradation rate and mineralization degree thanks to the absence of refractory Fe(III)-carboxylate complexes that typically decelerate the TOC abatement. From the by-products detected by GC/MS, a reaction sequence for DPH mineralization is proposed.

5.
Chemosphere ; 364: 143291, 2024 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-39243904

RESUMEN

Nature iron is considered one of the promising catalysts in advanced oxidation processes (AOPs) that are utilized for soil remediation from polycyclic aromatic hydrocarbons (PAHs). However, the existence of anions, cations, and organic matter in soils considered impurities that restricted the utilization of iron that was harnessed naturally in the soil matrix and reduced the catalytic performance. In this regard, tropical soil naturally containing iron and relatively poor with impurities was artificially contaminated with 100 mg/50 g benzo[α]pyrene (B[α]P) and remediated using a slurry phase reactor supported with persulfate (PS). The results indicated that tropical soil containing iron and relatively poor with impurities capable of activating the oxidants and formation of radicals which successfully degraded B[α]P. The optimum removal result was 86% and obtained under the following conditions airflow = 260 mL/min, temperature 55 °C, pH 7, and [PS]0 = 1.0 g/L, at the same experimental conditions soil organic matter (SOM) mineralization was 48%. After the remediation process, there was a significant reduction in iron and aluminum contents, which considered the drawbacks of this system. Experiments to scavenge reactive species highlighted O2•- and SO4•- as the main radicals that oxidized B[α]P. Additionally, monitoring of by-products post-remediation aimed to assess toxicity and elucidate degradation pathways. Mutagenicity tests yielded positive results for two B[α]P by-products. The toxicity tests considered were the lethal concentration of 50% (LC50 96 h) for fat-head minnows revealed that all B[α]P by-products were less toxic than the parent pollutant itself. This research marks a significant advancement in soil remediation by advancing the use of the AOP method, removing the requirement for additional catalysts in the AOP system for the removal of B[α]P from soil.

6.
Chemosphere ; 364: 142980, 2024 Aug 06.
Artículo en Inglés | MEDLINE | ID: mdl-39097109

RESUMEN

In the present study, we introduce a covalent organic triazine framework polymer (COTF-P) using 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) with triazine-based amine. The resulting dark red COTF-P illustrated potential behavior as a photocatalyst under visible light. Due to the inadequate solar energy capture and ultrafast charge recombination of the resulting COTF-P, the prepared COTF-P has been decorated with CQDs (N-CQD and N-S-CQD) to build a Z-scheme CQDs/COTF-P heterojunction photocatalyst and utilizes as photocatalyst for the breakdown of phenanthrene (PHE) exposed to visible light. The prepared COTF-P and CQDs/COTF-P were fully characterized, analyzing the textural (N2 isotherms), structural (XRD and FTIR), chemical (EDX and XPS), morphological (FESEM and TEM), optical (DRS-UV-Vis and photoluminescence), and electrochemical properties (EIS impedance, transient photocurrent, and flat band potential). The prepared N-S-CQD/COTF-P heterojunction displayed optimum activity for the photocatalytic oxidation of PHE from water, owing to an enhanced separation of the photogenerated charges and lower bandgap value, 2.1 vs. 1.9 eV. The N-S-CQD/COTF-P heterojunction showed acceptable stability in terms of activity and structural properties after 5 cycles of reuse. The mechanism of activation highlights the importance played by superoxide radicals and hydroxyl radicals. This project sheds light on the potential use of CQDs for the decoration of polymers, extending the absorbance in the visible region and boosting the migration of charge, which boosts the activity of the resulting material.

7.
PNAS Nexus ; 3(8): pgae330, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-39189022

RESUMEN

Acetylperoxyl radical (CH3C(O)OO•) is among highly reactive organic radicals which are known to play crucial roles in atmospheric chemistry, aqueous chemistry and, most recently, peracetic acid (PAA)-based advanced oxidation processes. However, fundamental knowledge for its reactivity is scarce and severely hampers the understanding of relevant environmental processes. Herein, three independent experimental approaches were exploited for revelation and quantification of the reaction rates of acetylperoxyl radical. First, we developed and verified laser flash photolysis of biacetyl, ultraviolet (UV) photolysis of biacetyl, and pulse radiolysis of acetaldehyde, each as a clean source of CH3C(O)OO•. Then, using competition kinetics and selection of suitable probe and competitor compounds, the rate constants between CH3C(O)OO• and compounds of diverse structures were determined. The three experimental approaches complemented in reaction time scale and ease of operation, and provided cross-validation of the rate constants. Moreover, the formation of CH3C(O)OO• was verified by spin-trapped electron paramagnetic resonance, and potential influence of other reactive species in the systems was assessed. Overall, CH3C(O)OO• displays distinctively high reactivity and selectivity, reacting especially favorably with naphthyl and diene compounds (k ∼ 107-108 M-1 s-1) but sluggishly with N- and S-containing groups. Significantly, we demonstrated that incorporating acetylperoxyl radical-oxidation reactions significantly improved the accuracy in modeling the degradation of environmental micropollutants by UV/PAA treatment. This study is among the most comprehensive investigation for peroxyl radical reactivity to date, and establishes a robust methodology for investigating organic radical chemistry. The determined rate constants strengthen kinetic databases and improve modeling accuracy for natural and engineered systems.

8.
Water Res ; 263: 122173, 2024 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-39111213

RESUMEN

Wastewater treatment plants face significant challenges in transitioning from energy-intensive systems to carbon-neutral, energy-saving systems, and a large amount of chemical energy in wastewater remains untapped. Iron is widely used in modern wastewater treatment. Research shows that leveraging the coupled redox relationship of iron and carbon can redirect this energy (in the form of carbon) towards resource utilization. Therefore, re-examining the application of iron in existing wastewater carbon processes is particularly important. In this review, we investigate the latest research progress on iron for wastewater carbon flow restructuring. During the iron-based chemically enhanced primary treatment (CEPT) process, organic carbon is captured into sludge and its bioavailability is enhanced through iron-based advanced oxidation processes (AOP) pretreatment, further being recovered or upgraded to value-added products in anaerobic biological processes. We discuss the roles and mechanisms of iron in CEPT, AOP, anaerobic biological processes, and biorefining in driving organic carbon conversion. The dosage of iron, as a critical parameter, significantly affects the recovery and utilization of sludge carbon resources, particularly by promoting effective electron transfer. We propose a pathway for beneficial conversion of wastewater organic carbon driven by iron and analyze the benefits of the main products in detail. Through this review, we hope to provide new insights into the application of iron chemicals and current wastewater treatment models.


Asunto(s)
Carbono , Hierro , Eliminación de Residuos Líquidos , Aguas Residuales , Hierro/química , Aguas Residuales/química , Eliminación de Residuos Líquidos/métodos , Oxidación-Reducción , Aguas del Alcantarillado/química
9.
Chemosphere ; 364: 143124, 2024 Aug 19.
Artículo en Inglés | MEDLINE | ID: mdl-39168383

RESUMEN

Persulfates activation by various nanomaterials has been intensively reported for advanced oxidation processes (AOPs), and substantial progress has been made in understanding the mechanism. However, most of the published articles only present the unnormalized catalytic properties, which generated confusion to compare different catalysts and identify the active sites. Herein, we presented electrochemical surface area (ECSA) as a practical normalized method and confirmed the primary active sites in N-doped graphene. By controlling the aggregation state of graphene sheets to adjust the activity of doped graphite-N species, the active sites for peroxydisulfate (PDS) activation were accurately estimated. In further experiments, specific surface area (SSA, by N2-physisorption and methylene blue adsorption) and ECSA were adopted to conclude the normalized oxidation rate constant and graphitic-N was confirmed as the primary site in nitrogen-doped graphene for the carbocatalyst/PDS system. The normalized results revealed that SSA derived from inert gas on materials could not reflect the true active sites at solid-liquid interface, while ECSA considering the operated solid-liquid situation can be used for accurate estimation of the active sites. Therefore, this study suggests that ECSA integrates the properties of both kinetics and thermodynamics, which can be adopted as a useful methodology for analyzing nano-sized environmental catalysts performance.

10.
J Colloid Interface Sci ; 677(Pt B): 952-966, 2024 Aug 18.
Artículo en Inglés | MEDLINE | ID: mdl-39178674

RESUMEN

Although nanozymes have shown significant potential in wastewater treatment, enhancing their degradation performance remains challenging. Herein, a novel catalytic behavior was revealed for defective nanozymes with catalase-mimicking characteristics that efficiently degraded tetracycline (TC) in wastewater. Hydroxyl groups adsorbed on defect sites facilitated the in-situ formation of vacancies during catalysis, thereby replenishing active sites. Additionally, electron transfer considerably enhanced the catalytic reaction. Consequently, numerous reactive oxygen species (ROS) were generated through these processes and subsequent radical reactions. The defective nanozymes, with their unique catalytic behavior, proved effective for the catalytic degradation of TC. Experimental results demonstrate that •OH, •O2-, 1O2 and e- were the primary contributors to the degradation process. In real wastewater samples, the normalized degradation rate constant for defective nanozymes reached 26.0 min-1 g-1 L, exceeding those of other catalysts. This study reveals the new catalytic behavior of defective nanozymes and provides an effective advanced oxidation process for the degradation of organic pollutants.

11.
Water Sci Technol ; 90(3): 824-843, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-39141037

RESUMEN

In recent years, studies on the degradation of emerging organic contaminants by sulfate radical (SO4-·) based advanced oxidation processes (SR-AOPs) have triggered increasing attention. Metal-loaded biochar (Me-BC) can effectively prevent the agglomeration and leaching of transition metals, and its good physicochemical properties and abundant active sites induce outstanding in activating persulfate (PS) for pollutant degradation, which is of great significance in the field of advanced oxidation. In this paper, we reviewed the preparation method and stability of Me-BC, the effect of metal loading on the physicochemical properties of biochar, the pathways of pollutant degradation by Me-BC-activated PS (including free radical pathways: SO4-·, hydroxyl radical (·OH), superoxide radicals (O2-·); non-free radical pathways: singlet oxygen (1O2), direct electron transfer), and discussed the activation of different active sites (including metal ions, persistent free radicals, oxygen-containing functional groups, defective structures, etc.) in the SR-AOPs system. Finally, the prospect was presented for the current research progress of Me-BC in SR-AOPs technology.


Asunto(s)
Carbón Orgánico , Sulfatos , Contaminantes Químicos del Agua , Carbón Orgánico/química , Sulfatos/química , Contaminantes Químicos del Agua/química , Metales/química , Oxidación-Reducción
12.
Molecules ; 29(15)2024 Jul 31.
Artículo en Inglés | MEDLINE | ID: mdl-39125039

RESUMEN

To explore advanced oxidation catalysts, peroxymonosulfate (PMS) activation by Co-Ni-Mo/carbon nanotube (CNT) composite catalysts was investigated. A compound of NiCo2S4, MoS2, and CNTs was successfully prepared using a simple one-pot hydrothermal method. The results revealed that the activation of PMS by Co-Ni-Mo/CNT yielded an exceptional Rhodamine B decolorization efficiency of 99% within 20 min for the Rhodamine B solution. The degradation rate of Co-Ni-Mo/CNT was 4.5 times higher than that of Ni-Mo/CNT or Co-Mo/CNT, and 1.9 times as much than that of Co-Ni/CNT. Additionally, radical quenching experiments revealed that the principal active groups were 1O2, surface-bound SO4•-, and •OH radicals. Furthermore, the catalyst exhibited low metal ion leaching and favorable stability. Mechanism studies revealed that Mo4+ on the surface of MoS2 participated in the oxidation of PMS and the transformation of Co3+/Co2+ and Ni3+/Ni2+. The synergism between MoS2 and NiCo2S4 reduces the charge transfer resistance between the catalyst and solution interface, thus accelerating the reaction rate. Interconnected structures composed of metal sulfides and CNTs can also enhance the electron transfer process and afford sufficient active reaction sites. Our work provides a further understanding of the design of multi-metal sulfides for wastewater treatment.

13.
J Hazard Mater ; 478: 135396, 2024 Oct 05.
Artículo en Inglés | MEDLINE | ID: mdl-39121736

RESUMEN

Quaternary ammonium compounds (QACs) are widely detected in the aquatic environment due to their extensive use in a wide array of antibacterial products during the pandemic. In the current study, UV/monochloramine (UV/NH2Cl) was used to degrade three typical QACs, namely benzalkonium compounds (BACs), dialkyl dimethyl ammonium compounds (DADMACs), and alkyl trimethyl ammonium compounds (ATMACs). This process achieved high efficiency in removing BACs from water samples. The transformation products of QACs treated with UV/NH2Cl were identified and characterized using a high-resolution mass spectrometer, and transformation pathways were proposed. The formation of N-nitroso-N-methyl-N-alkylamines (NMAs) and N-nitrosodimethylamine (NDMA) were observed during QAC degradation. The molar formation yield of NDMA from C12-BAC was 0.04 %, while yields of NMAs reached 1.05 %. The ecotoxicity of NMAs derived from QACs was predicted using ECOSAR software. The increased toxicity could be attributed to the formation of NMAs with longer alkyl chains; these NMAs, exhibited a one order of magnitude increase in toxicity compared to their parent QACs. This study provides evidence that QACs are the specific and significant precursors of NMAs. Greater attention should be given to NMA formation and its potential threat to the ecosystem, including humans.


Asunto(s)
Cloraminas , Compuestos de Amonio Cuaternario , Rayos Ultravioleta , Contaminantes Químicos del Agua , Compuestos de Amonio Cuaternario/química , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/efectos de la radiación , Contaminantes Químicos del Agua/análisis , Cinética , Cloraminas/química , Dimetilnitrosamina/química , Nitrosaminas/química , Nitrosaminas/análisis
14.
Water Sci Technol ; 89(12): 3344-3356, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-39150428

RESUMEN

In this study, a potassium ferrate (K2FeO4)-modified biochar (Fe-BC) was prepared and characterized. Afterwards, Fe-BC was applied to activated periodate (PI) to degrade tetracycline (TC), an antibiotic widely used in animal farming. The degradation effects of different systems on TC were compared and the influencing factors were investigated. In addition, several reactive oxygen species (ROS) generated by the Fe-BC/PI system were identified, and TC degradation pathways were analyzed. Moreover, the reuse performance of Fe-BC was evaluated. The results exhibited that the Fe-BC/PI system could remove almost 100% of TC under optimal conditions of [BC] = 1.09 g/L, initial [PI] = 3.29 g/L, and initial [TC] = 20.3 mg/L. Cl-, HCO3-, NO3-, and humic acid inhibited TC degradation to varying degrees in the Fe-BC/PI system due to their quenching effects on ROS. TC was degraded into intermediates and even water and carbon dioxide by the synergistic effect of ROS generated and Fe on the BC surface. Fe-BC was reused four times, and the removal rate of TC was still maintained above 80%, indicating the stable nature of Fe-BC.


Asunto(s)
Carbón Orgánico , Hierro , Tetraciclina , Contaminantes Químicos del Agua , Tetraciclina/química , Hierro/química , Carbón Orgánico/química , Contaminantes Químicos del Agua/química , Especies Reactivas de Oxígeno/metabolismo , Purificación del Agua/métodos , Antibacterianos/química , Antibacterianos/farmacología , Compuestos de Potasio , Compuestos de Hierro
15.
Artículo en Inglés | MEDLINE | ID: mdl-39210224

RESUMEN

The application of hybrid advanced oxidation processes (AOPs) is an efficacious way to remediate emerging contaminants from wastewater. In the present research work, a hybrid electrochemical oxidation and ultraviolet light-based persulfate activation processes (EO-UV/PS) were used to efficiently degrade sodium dodecyl sulfate (SDS) surfactant from synthetic and municipal wastewater. By operating the EO-UV/PS at optimum operating conditions at pH of 7.0, NaCl of 0.02 M, current density of 6.4 mA/cm2, persulfate dose of 2.5 mM, and operating period of 180 min, about 94.5 ± 2.8% of SDS (20 mg/L) removal was achieved from synthetic wastewater. The abetment of SDS in both EO and UV/PS obeyed pseudo-first-order kinetics with a rate constant of 0.012 and 0.019 min-1, respectively. Moreover, the economic analysis revealed 0.23 $ m-3 order-1 as the operating cost for degrading SDS in EO-UV/PS. The degradation pathway experimentation suggested the generation of lauric acid by-product during SDS abatement. Besides, nearly 89.3 ± 2.9% of SDS and 58.7 ± 2.4% of total organic carbon reduction was also achieved from real municipal wastewater. Phytotoxicity test on Vigna radiata affirms the non-toxic nature of the EO-UV/PS effluent.

16.
Environ Monit Assess ; 196(9): 820, 2024 Aug 17.
Artículo en Inglés | MEDLINE | ID: mdl-39154115

RESUMEN

Drugs and related goods are widely used in order to promote public health and the quality of life. One of the most serious environmental challenges affecting public health is the ongoing presence of antibiotics in the effluents generated by pharmaceutical industries and hospitals. Antibiotics cannot be entirely removed from wastewater using the traditional wastewater treatment methods. Unmetabolized antibiotics generated by humans can be found in urban and livestock effluent. The antibiotic present in effluent contributes to issues with resistance to antibiotics and the creation of superbugs. Over the recent 2 years, the coronavirus disease 2019 pandemic has substantially boosted hospital waste volume. In this situation, a detailed literature review was conducted to highlight the harmful effects of untreated hospital waste and outline the best approaches to manage it. Approximately 50 to 70% of the emerging contaminants prevalent in the hospital wastewater can be removed using traditional treatment strategies. This paper emphasizes the numerous treatment approaches for effectively eliminating emerging contaminants and antibiotics from hospital wastewater and provides an overview of global hospital wastewater legislation and guidelines on hospital wastewater administration. Around 90% of ECs might be eliminated by biological or physical treatment techniques when used in conjunction with modern oxidation techniques. According to this research, hybrid methods are the best approach for removing antibiotics and ECs from hospital wastewater. The document outlines the many features of effective hospital waste management and might be helpful during and after the coronavirus disease 2019 outbreak, when waste creation on all hospitals throughout the globe has considerably increased.


Asunto(s)
Antibacterianos , COVID-19 , Hospitales , Aguas Residuales , Aguas Residuales/química , COVID-19/epidemiología , Antibacterianos/análisis , Humanos , Contaminantes Químicos del Agua/análisis , Eliminación de Residuos Líquidos/métodos , Pandemias , SARS-CoV-2 , Monitoreo del Ambiente/métodos
17.
Chemosphere ; 363: 142893, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39029705

RESUMEN

Advanced oxidation processes based on persulfate activation by biochar have been widely used to remove antibiotics and antibiotic resistance genes (ARGs) from wastewater. In this study, we used a common continuous fixed-bed reactor based on a biochar/persulfate system to treat wastewater. The average apparent ARG-removal efficiency was 82.38% in the biochar/persulfate reactor. The results of continuous reactor activity suggested the presence of ARG residues in the biochar (the abundance of ARG in the biochar increased 103-fold) and unstable removal of extracellular ARGs, raising concerns about a potential environmental burden. Kinetic experiments showed that the absolute abundance of intracellular ARGs (iARGs) rapidly decreased 98.3% within 30 min, but extracellular ARGs (eARGs) correspondingly increased 15-fold, suggesting that persulfate broke bacterial cells open and quickly released iARGs as eARGs. Moreover, the proportions of the three types of ARGs showed that ARG removal was attributed to about 70% degradation and 30% adsorption by the biochar/persulfate reactor. Further analysis revealed that biochar acts as a special shelter for ARGs. Release experiment of used biochar indicated that nearly half of absorbed ARGs could be released into new environment and causing potential risk. Overall, our findings provide a fundamental understanding of the fate of ARGs during treatment of antibiotic-contaminated wastewater and new insights into the multiple roles of biochar, which can potentially represent an additional burden on ecosystems and human health.


Asunto(s)
Antibacterianos , Carbón Orgánico , Farmacorresistencia Microbiana , Eliminación de Residuos Líquidos , Aguas Residuales , Carbón Orgánico/química , Aguas Residuales/química , Antibacterianos/química , Antibacterianos/farmacología , Eliminación de Residuos Líquidos/métodos , Farmacorresistencia Microbiana/genética , Contaminantes Químicos del Agua/química , Genes Bacterianos , Adsorción
18.
Environ Sci Pollut Res Int ; 31(35): 48164-48174, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-39017866

RESUMEN

Ribavirin (RBV), which is extensively used to treat viral diseases such as COVID-19, is considered one of the major emerging contaminants due to its long-term existence and health risk in the aqueous environmental system. However, research on effective removal of RBV still remains insufficient. In this study, we investigated the RBV degradation kinetics and mechanism in UV/chlorine/Fe(II) process. The degradation rate constant kobs-RBV of RBV was 2.52 × 10-4 s-1 in UV/chlorine/Fe(II) process, which increased by 1.6 times and 1.3 times than that in chlorine alone and UV/chlorine process, respectively. Notably, trace amount Fe(II) promoted RBV degradation in UV/chlorine system through Fe2+/Fe3+ cycles, enhancing the yield of reactive species such as HO· and certain species reactive chlorine radicals (RCS). The contributions of HO· and RCS toward RBV degradation were 53.91% and 16.11%, respectively. Specifically, Cl·, ClO·, and Cl2·- were responsible for 8.59%, 2.69%, and 4.83% of RBV removal. The RBV degradation pathway indicated that the reactive species preferentially attacked the amide moiety of RBV, which cleaved the ether bond and the hydroxyl group. The toxicity evaluation of RBV degradation products elucidated that UV/chlorine/Fe(II) process was beneficial for RBV detoxification.


Asunto(s)
Cloro , Hierro , Ribavirina , Rayos Ultravioleta , Contaminantes Químicos del Agua , Purificación del Agua , Purificación del Agua/métodos , Cloro/química , Contaminantes Químicos del Agua/química , Ribavirina/química , Hierro/química , Cinética
19.
Water Res ; 261: 122049, 2024 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-38976932

RESUMEN

The secondary effluent of fermentation pharmaceutical wastewater exhibits high chromaticity, elevated salinity, and abundant refractory effluent organic matter (EfOM), presenting significant treatment challenges and environmental threats. Herein, Cu2(OH)3NO3/γ-Al2O3 was fabricated through ultrasound-assisted impregnation and calcination to catalyze the Fenton-like oxidation for degrading organic pollutants in this secondary effluent. Under neutral conditions, with 400.00 mg/L H2O2, 8 g/L catalyst, and at 30 ℃, the EfOM and CODCr removal efficiencies can reach 96.90 % and 51.56 %, respectively. The Cu2(OH)3NO3/γ-Al2O3 catalyst possesses ideal reusability, maintaining CODCr, chromaticity, and EfOM removal efficiencies at 44.44 %-64.59 %, 85.45 %-93.45 %, and 61.00 %-95.00 % over 220 h in a continuous-flow catalytic oxidation system operated at room temperatures (15-25 ℃). Electron paramagnetic resonance results and density functional theory calculations indicate that •OOH may be the predominant reactive oxygen species, facilitated by the easier elongation of the OH bond in H2O2 compared to the OO bond. The adjusted electronic structure endows Cu2(OH)3NO3/γ-Al2O3 composite sites with superior catalytic selectivity for H2O2 activation compared to Cu2(OH)3NO3 single crystal sites, with γ-Al2O3 additionally facilitating H2O2 activation through electron donation. This research highlights the efficacy of Cu2(OH)3NO3/γ-Al2O3 in the advanced treatment of complex industrial wastewater, elucidating its catalytic mechanisms and potential applications.


Asunto(s)
Peróxido de Hidrógeno , Oxidación-Reducción , Eliminación de Residuos Líquidos , Aguas Residuales , Contaminantes Químicos del Agua , Aguas Residuales/química , Catálisis , Peróxido de Hidrógeno/química , Eliminación de Residuos Líquidos/métodos , Contaminantes Químicos del Agua/química , Óxido de Aluminio/química , Cobre/química , Fermentación
20.
Chemosphere ; 362: 142736, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38950752

RESUMEN

Developing high-performance and durable catalysts presents a significant challenge for oxidizing toxic inorganic and pharmaceutical compounds in wastewater. Recently, there has been a surge in the development of new heterogeneous catalysts for degrading pharmaceutical compounds, driven by advancements in electrocatalysts and photoelectrocatalysts. In this study, a plasmonic Ag nanoparticles decorated CoFe2O4@TiO2 heteronanostructures have been successfully designed to fabricate a high-performing photoelectrode for the oxidation of pharmaceutical compounds. The developed Ag-CoFe2O4@TiO2 possessed a higher electrochemical stability and effectively harvested the UV to visible and NIR radiation in sunlight which generates the enormous photochemical reactive species that involved in the oxidation of ibuprofen in wastewater. Under direct sunlight irradiation, Ag-CoFe2O4@TiO2 achieved complete oxidation of ibuprofen in wastewater at 0.8 V vs RHE. This indicates that metallic Ag nanoparticles are involved in the charge separation and transport of charge carriers from the photoactive sites of CoFe2O4@TiO2, promoting the generation of abundant hydroxy, oxy, and superoxide radicals that actively break the bonds of ibuprofen. Additionally, oxidation agents such as urea and H2O2 were utilized to enhance the formation of superoxide ions and hydroxyl radicals, which rapidly participate in the oxidation of ibuprofen. Significantly, testing for recyclability confirmed the stability of the Ag-CoFe2O4@TiO2 photoanode, ensuring its suitability for prolonged use in photoelectrochemical advanced oxidation processes. Integrating Ag-CoFe2O4@TiO2 photoanodes into water purification systems could enhance economic feasibility, reduce energy consumption, and improve efficiency.


Asunto(s)
Antibacterianos , Oxidación-Reducción , Plata , Titanio , Aguas Residuales , Contaminantes Químicos del Agua , Titanio/química , Aguas Residuales/química , Plata/química , Catálisis , Contaminantes Químicos del Agua/química , Antibacterianos/química , Nanopartículas del Metal/química , Cobalto/química , Procesos Fotoquímicos , Ibuprofeno/química , Peróxido de Hidrógeno/química , Eliminación de Residuos Líquidos/métodos , Técnicas Electroquímicas/métodos , Compuestos Férricos/química
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