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1.
J Environ Sci (China) ; 147: 114-130, 2025 Jan.
Article in English | MEDLINE | ID: mdl-39003034

ABSTRACT

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.


Subject(s)
Hydrogen Peroxide , Iron , Waste Disposal, Fluid , Iron/chemistry , Hydrogen Peroxide/chemistry , Waste Disposal, Fluid/methods , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/analysis , Wastewater/chemistry , Oxidation-Reduction , Hydroxyl Radical/chemistry
2.
J Environ Sci (China) ; 147: 688-713, 2025 Jan.
Article in English | MEDLINE | ID: mdl-39003083

ABSTRACT

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.


Subject(s)
Acetaminophen , Reactive Oxygen Species , Acetaminophen/chemistry , Reactive Oxygen Species/metabolism , Water Pollutants, Chemical/chemistry , Oxidation-Reduction , Pharmaceutical Preparations/metabolism
3.
J Colloid Interface Sci ; 677(Pt A): 282-293, 2024 Jul 25.
Article in English | MEDLINE | ID: mdl-39094489

ABSTRACT

Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are attractive approaches for solving the global problem of water pollution, due to the generation of highly-active reactive oxygen species (ROS). Therefore, highly-efficient PMS activation is crucial for promoting the catalytic degradation of environmental pollutants. Here, bimetallic CoGeO2(OH)2 nanosheets with abundant surface hydroxyl groups (CGH) were synthesized via a simple hydrothermal route for PMS activation and degradation of various organic contaminants for the first time. The abundant surface hydroxyl groups (≡Co-OH/≡Ge-OH) could promptly initiate PMS to generate highly-active species: singlet oxygen (1O2), sulfate radicals (SO4·-) and hydroxyl radicals (HO•), while the asymmetric electron distribution among Co-O-Ge bonds derived from the higher electronegativity of Ge than Co further enhances the quick electron transfer to promote the redox cycle of Co2+/Co3+ and Ge2+/Ge4+, thereby achieving an outstanding catalytic capability. The optimal catalyst exhibits nearly 100 % catalytic degradation performance of dyes (Methylene blue, Rhodamine B, Methyl orange, Orange II, Methyl green) and antibiotics (Norfloxacin, Bisphenol A, Tetracycline) over a wide pH range of 3-11 and under different coexisting anion conditions (Cl-, HCO3-, NO3-, HA), suggesting the excellent adaptability for practical usage. This study could potentially lead to novel perspectives on the remediation of water areas such as groundwater and deep-water areas.

4.
Environ Res ; 261: 119719, 2024 Aug 03.
Article in English | MEDLINE | ID: mdl-39098711

ABSTRACT

The pervasive presence of per and polyfluoroalkyl substances (PFAS), commonly referred to as "forever chemicals," in water systems poses a significant threat to both the environment and public health. PFAS are persistent organic pollutants that are incredibly resistant to degradation and have a tendency to accumulate in the environment, resulting in long-term contamination issues. This comprehensive review delves into the primary impacts of PFAS on both the environment and human health while also delving into advanced techniques aimed at addressing these concerns. The focus is on exploring the efficacy, practicality, and sustainability of these methods. The review outlines several key methods, such as advanced oxidation processes, novel materials adsorption, bioremediation, membrane filtration, and in-situ chemical oxidation, and evaluates their effectiveness in addressing PFAS contamination. By conducting a comparative analysis of these techniques, the study aims to provide a thorough understanding of current PFAS remediation technologies, as well as offer insights into integrated approaches for managing these persistent pollutants effectively. While acknowledging the high efficiency of adsorption and membrane filtration in reducing persistent organic pollutants due to their relatively low cost, versatility, and wide applicability, the review suggests that the integration of these methods could result in an overall enhancement of removal performance. Additionally, the study emphasizes the need for researcher attention in key areas and underscores the necessity of collaboration between researchers, industry, and regulatory authorities to address this complex challenge.

5.
Chemosphere ; 364: 142980, 2024 Aug 06.
Article in English | MEDLINE | ID: mdl-39097109

ABSTRACT

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.

6.
J Hazard Mater ; 478: 135396, 2024 Aug 08.
Article in English | MEDLINE | ID: mdl-39121736

ABSTRACT

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.

7.
Sci Total Environ ; 950: 175401, 2024 Aug 08.
Article in English | MEDLINE | ID: mdl-39127198

ABSTRACT

The inherent toxicity and persistence of emerging contaminants such as antibiotics and endocrine disruptors pose substantial threats to the environment. Advanced oxidation processes (AOPs) employed for oxidative degradation could yield toxic oxidation by-products (OBPs), including organic acids and aromatic hydrocarbons. Despite their typically low concentrations, OBPs require scrutiny owing to their potential health risks. Although effective assessment methodologies are available, a comprehensive review focusing on the ecological and environmental effects of these pollutants is lacking. This study offers a succinct overview of existing ecotoxicological exposure assessments for emerging organic pollutants. Further, it encapsulates principal dose-response assessment techniques and provides a comparative analysis of several methods. The straightforward assessment factor method evaluates risk based on exposure and species sensitivity and is suitable for preliminary assessments of single pollutants; Species Sensitivity Distribution (SSD) compares species sensitivities to OBPs, emphasizing the importance of species-specific toxicological responses; microcosm and mesocosm methods simulate and predict the effects of OBPs on aquatic life by considering environmental diversity and biological community structures and are ideal for assessing the toxicity of multiple OBPs; the ecological risk analysis model employs mathematical and probabilistic approaches to comprehensively and accurately assess exposures and effects, accounting for the complexities and uncertainties inherent in ecotoxicological evaluations. Different risk characterization techniques are outlined in this study, including the risk quotient (RQ), which is ideal for quantifying and comparing risks; probabilistic ecological risk assessment (PERA), suitable for managing significant uncertainty; and the Environmental Pollution Index (EPI), the preferred method for quantitative assessment of OBP pollution levels. The merits and limitations of each of these quantitative assessment tools are evaluated, providing a comprehensive view of their applications in risk analysis. In addition, pressing contemporary challenges are identified and trajectories and pivotal issues suggested for future research.

8.
Water Res ; 263: 122173, 2024 Jul 29.
Article in English | MEDLINE | ID: mdl-39111213

ABSTRACT

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.

9.
Molecules ; 29(15)2024 Jul 31.
Article in English | MEDLINE | ID: mdl-39125039

ABSTRACT

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.

10.
Molecules ; 29(15)2024 Aug 02.
Article in English | MEDLINE | ID: mdl-39125061

ABSTRACT

The widespread presence and use of Bisphenol A (BPA) in aquatic environments has caused significant ecological damage. Coal gangue (CG), a byproduct of coal mining, poses a major environmental concern due to its vast land occupation and potential for pollution. A magnetic recyclable geopolymer (MnFe2O4-CGP) using coal gangue geopolymer (CGP) as the carrier was successfully synthesized and was evaluated for its ability to Fenton-like degrade BPA. The characterization techniques revealed the successful incorporation of spherical MnFe2O4 onto the CGP surface and that CGP serves as an excellent platform for the immobilization and dispersion of MnFe2O4. The degradation rate reached 100% within 60 min at pH = 5, 15 mmol/L H2O2, 0.6 g/L catalyst, and 50 mg/L BPA, significantly higher than MnFe2O4 and CGP alone. It was indicated that the degradation rate of BPA in MnFe2O4-CGP composites was 0.1121 min-1, which was consistent with the first-order kinetic model. The saturation magnetization of MnFe2O4-CGP was measured to be 10.96 emu/g, enabling convenient recovery. MnFe2O4-CGP exhibited excellent stability, as the degradation rate of BPA remained above 95% even after five reaction cycles. This efficiency may be due to the MnFe2O4-CGP induced generation of reactive radicals. Quenching and EPR radical trapping experiments unequivocally confirmed that the reactive radical was hydroxyl radical (•OH). These results indicate that MnFe2O4-CGP has potential application prospects as a magnetic recyclable geopolymer composite in Fenton-like catalysis.

11.
Chemosphere ; : 143071, 2024 Aug 09.
Article in English | MEDLINE | ID: mdl-39128776

ABSTRACT

Two microwave (MW) responsive heterojunction nanocomposite catalysts, i.e., α-Bi2O3/CoFe2O4 (BO/CFO) and ZnO/CoFe2O4 (ZO/CFO), with weight% ratio of 70/30, 50/50, 30/70 were synthesized by sequential thermal decomposition and co-precipitation methods, and used for the degradation of tetracycline (TC) under MW irradiation. The formation of desired catalysts was confirmed through the characterization results of XRD, FT-IR, SEM, VSM, UV-DRS, XPS, BET, etc. Using batch MW experiments, the catalyst dose, pH, initial TC concentration, reaction temperature, and MW power were optimized for TC removal. Under the following reaction conditions: catalyst dose ∼1 g/L, initial TC concentration ∼1 mg/L, temperature ∼90ºC, MW ∼450 W, BO/CFO, and ZO/CFO showed ∼97.55% and 88.23% TC degradation, respectively, after 5 min. The difference in the catalytic response against TC degradation indicated the difference in reflective loss (RL) between these two catalysts. The presence of other competitive anions has affected the removal efficiency of TC due to the scavenging effect. The radical trapping study revealed the significant contribution of TC degradation by hydroxyl radicals in the case of ZO/CFO, whereas for BO/CFO, superoxide (●O2-) and hydroxyl radicals (●OH) both played influential roles. The Z-scheme heterojunction of BO/CFO allowed the formation of ●O2- but the same was inhibited in type-II heterojunction of ZO/CFO due to the valance band position. The dielectric loss, magnetic loss, interfacial polarization, and high electrical conductivity, 'hotspots' were produced over the catalyst surface alongside electron-hole separation at heterojunctions, which were responsible for the generation of reactive oxygen species. In addition, Co3+/Co2+ and Fe3+/Fe2+ redox cycles have promoted ●O2- and sulfate radical production during persulfate application. Among the two MW responsive catalysts, BO/CFO could be a potential material for rapidly destroying emerging organic pollutants from wastewater without applying other oxidative chemicals under MW irradiation.

12.
Water Sci Technol ; 89(12): 3309-3324, 2024 Jun.
Article in English | MEDLINE | ID: mdl-39150426

ABSTRACT

Polyacrylamide (PAM) in environmental water has become a major problem in water pollution management due to its high molecular mass, high viscosity and non-absorption by soil. CoFe2O4 with strong magnetic properties was prepared by solvent-thermal synthesis method and used as the catalyst for the removal on PAM in heterogeneous Electro-Fenton (EF) system. It showed that the removal efficiency of PAM by the heterogeneous EF system using CoFe2O4 catalyst was 92.01% at pH 3 after 120 min. Further studies indicated that ·OH was the most significant active species for the removal of PAM, and the contribution of ·O2- and SO4·- for the removal of PAM was less than 15%. The reusability test and XRD, XPS, FTIR analyses proved that the catalyst had good stability. After a repeated use for five times, the catalyst still had a high PAM removal rate and stable structure. The valence distribution and functional groups of the phase components of the catalyst did not change significantly before and after the reaction. The possible mechanism of catalyst activation of H2O2 was deduced by mechanism investigation. The CoFe2O4 is an efficient and promising catalyst for the removal of PAM wastewater.


Subject(s)
Acrylic Resins , Cobalt , Ferric Compounds , Hydrogen Peroxide , Iron , Acrylic Resins/chemistry , Cobalt/chemistry , Catalysis , Hydrogen Peroxide/chemistry , Iron/chemistry , Ferric Compounds/chemistry , Water Pollutants, Chemical/chemistry , Water Purification/methods , Waste Disposal, Fluid/methods
13.
Water Sci Technol ; 89(12): 3344-3356, 2024 Jun.
Article in English | MEDLINE | ID: mdl-39150428

ABSTRACT

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.


Subject(s)
Charcoal , Iron , Tetracycline , Water Pollutants, Chemical , Tetracycline/chemistry , Iron/chemistry , Charcoal/chemistry , Water Pollutants, Chemical/chemistry , Reactive Oxygen Species/metabolism , Water Purification/methods , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/pharmacology , Potassium Compounds , Iron Compounds
14.
J Med Biochem ; 43(4): 424-435, 2024 Jun 15.
Article in English | MEDLINE | ID: mdl-39139165

ABSTRACT

Background: The pathophysiological mechanisms crucial in the development of nephrotic syndrome (NS) in the pediatric population are still not fully understood. This study aimed to investigate the relationship between hypertension, oxidative stress, and inflammation in pediatric patients during the acute phase of the disease. Methods: The study included 33 children, aged 2 to 9 years, with nephrotic syndrome. Blood samples were collected during the acute phase and remission. Parameters of oxidative status were determined, including total oxidative status (TOS), advanced oxidation protein products (AOPP), prooxidant-antioxidant balance (PAB), sulfhydryl groups (-SH), paraoxonase 1 (PON1), and total antioxidant status (TAS) in serum, measured spectrophotometrically. Inflam - matory parameters such as pentraxin 3 (PTX3), leptin, program med cell death ligand 1 (PD-L1), and E-cadherin were determined using enzyme-linked immunosorbent assay (ELISA). Results: Patients with nephrotic syndrome and hypertension had significantly higher levels of advanced oxidation protein products and total antioxidant status (p=0.029 and p=0.003, respectively). During the acute phase of the disease, lower activity of sulfhydryl groups and paraoxonase 1 was observed compared to remission (p<0.001, for both). Pentraxin 3 levels were higher, while leptin levels were lower during the acute phase (p<0.001, for both). Pentraxin 3 correlated with advanced oxidation protein products and total antioxidant status during the acute phase but not in remission (rs=0.42, p=0.027 and rs=0.43, p=0.025, respectively). A negative correlation between Advanced oxidation protein products and leptin was observed during the acute phase, which disappeared in remission (rs=-0.42, p=0.028). Conclusions: Results of this study show that hypertension influences oxidative stress markers, and decreased antioxidant capacity may contribute to nephrotic syndrome development. Pentraxin 3 appears as a potential disease activity marker, indicating a dynamic connection between inflammation and oxidative stress. Leptin may also play a role in oxidative stress in nephrotic syndrome.

15.
Sci Total Environ ; : 175472, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-39142414

ABSTRACT

Acetaminophen (APAP) is a well-known type of over-the-counter painkiller and is frequently found in surface waterbodies, causing hepatotoxicity and skin irritation. Due to its persistence and chronic effects on the environment, innovative solutions must be provided to decompose APAP effectively. Successfully, innovative catalysts of tungsten-modified iron oxides (TF) were developed via a combustion method and thoroughly characterized using SEM, TEM, XRD, XPS, a porosimetry analysis, Mössbauer spectroscopy, VSM magnetometry, and EPR. With the synthesis method, tungsten was successfully incorporated into iron oxides to form ferrites and other magnetic iron oxides with a high porosity of 19.7 % and a large surface area of 29.5 m2/g. Also, their catalytic activities for APAP degradation by activating peroxymonosulfate (PMS) were evaluated under various conditions. Under optimal conditions, TF 2.0 showed the highest APAP degradation of 95 % removal with a catalyst loading of 2.0 g/L, initial APAP concentration of 5 mg/L, PMS 6.5 mM, and pH 2.15 at room temperature. No inhibition by solution pHs, alkalinity, and humic acid was observed for APAP degradation. The catalysts also showed chemical and mechanical stability, achieving 100 % degradation of 1 mg/L APAP during reusability tests with three consecutive experiments. These results show that TFs can effectively degrade persistent contaminants of emerging concern in water, offering an impactful contribution to wastewater treatment to protect human health and the ecosystem.

16.
Environ Res ; : 119780, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-39142460

ABSTRACT

Antimicrobial resistance (AMR) poses a global health threat to aquatic environments and its propagation is a hot topic. Therefore, deactivating antibiotic-resistant bacteria (ARB) and removing antibiotic resistance genes (ARGs) from water is crucial for controlling AMR transmission. Peracetic acid (PAA), which is known for its potent oxidizing properties and limited by-product formation, is emerging as a favorable disinfectant for water treatment. In this study, we aimed to assess the efficacy of pre-exposure to PAA followed by UV treatment (PAA-UV/PAA) compared with the simultaneous application of UV and PAA (UV/PAA). The focus was on deactivating vancomycin-resistant Enterococcus faecalis (VREfs), a typical ARB in water. Pre-exposure to PAA significantly enhanced the efficacy of subsequent UV/PAA treatment. At a UV fluence of 7.2 mJ cm-2, the PAA-UV/PAA method achieved a 6.21 log reduction in VREfs, surpassing the 1.29 log reduction observed with UV/PAA. Moreover, compared to UV/PAA, PAA-UV/PAA showed increased efficacy with longer pre-exposure times and higher PAA concentrations, maintaining superior performance across a broad pH range and in the presence of humic acid. Flow cytometry analysis indicated minimal cellular membrane damage using both methods. However, the assessments of superoxide dismutase (SOD) activity and adenosine triphosphate content revealed that PAA-UV/PAA induced greater oxidative stress under similar UV irradiation conditions, leading to slower bacterial regrowth. Specifically, SOD activity in PAA-UV/PAA surged to 3.06 times its baseline, exceeding the 1.73-fold increase under UV/PAA conditions. Additionally, pre-exposure to PAA amplified ARGs degradation and reduced resistance gene leakage, effectively mitigating the spread of AMR. Pre-exposure to 200 µM PAA for 10 and 20 min enhanced vanB gene removal efficiency by 0.14 log and 1.29 log, respectively. Our study provides a feasible approach for optimizing UV/PAA disinfection for efficient removal of ARB and ARGs.

17.
Water Sci Technol ; 90(3): 824-843, 2024 Aug.
Article in English | MEDLINE | ID: mdl-39141037

ABSTRACT

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.


Subject(s)
Charcoal , Sulfates , Water Pollutants, Chemical , Charcoal/chemistry , Sulfates/chemistry , Water Pollutants, Chemical/chemistry , Metals/chemistry , Oxidation-Reduction
18.
Water Sci Technol ; 90(3): 1047-1069, 2024 Aug.
Article in English | MEDLINE | ID: mdl-39141051

ABSTRACT

Single-atom catalysts (SACs) exhibit outstanding catalytic activity due to their highly dispersed metal centers. Activating persulfates (PS) with SACs can generate various reactive oxygen species (ROS) to efficiently degrade emerging organic contaminants (EOCs) in aqueous environments, offering unique advantages such as high reaction rates and excellent stability. This technique has been extensively researched and holds enormous potential applications. In this paper, we comprehensively elaborated on the synthesis methods of SACs and their limitations, and factors influencing the catalytic performance of SACs, including metal center characteristics, coordination environment, and types of substrates. We also analyzed practical considerations for application. Subsequently, we discussed the mechanism of SACs activating PS for EOCs degradation, encompassing adsorption processes, radical pathways, and non-radical pathways. Finally, we provide prospects and outline our vision for future research, aiming to guide advancements in applying this technique.


Subject(s)
Sulfates , Water Pollutants, Chemical , Catalysis , Water Pollutants, Chemical/chemistry , Sulfates/chemistry , Water Purification/methods
19.
Environ Sci Technol ; 58(26): 11843-11854, 2024 Jul 02.
Article in English | MEDLINE | ID: mdl-38952299

ABSTRACT

Advanced oxidation processes (AOPs) are the most efficient water cleaning technologies, but their applications face critical challenges in terms of mass/electron transfer limitations and catalyst loss/deactivation. Bipolar electrochemistry (BPE) is a wireless technique that is promising for energy and environmental applications. However, the synergy between AOPs and BPE has not been explored. In this study, by combining BPE with AOPs, we develop a general approach of using carbon nanotubes (CNTs) as electric-field-induced bipolar electrodes to control electron transfer for efficient water purification. This approach can be used for permanganate and peroxide activation, with superior performances in the degradation of refractory organic pollutants and excellent durability in recycling and scale-up experiments. Theoretical calculations, in situ measurements, and physical experiments showed that an electric field could substantially reduce the energy barrier of electron transfer over CNTs and induce them to produce bipolar electrodes via electrochemical polarization or to form monopolar electrodes through a single particle collision effect with feeding electrodes. This approach can continuously provide activated electrons from one pole of bipolar electrodes and simultaneously achieve "self-cleaning" of catalysts through CNT-mediated direct oxidation from another pole of bipolar electrodes. This study provides a fundamental scientific understanding of BPE, expands its scope in the environmental field, and offers a general methodology for water purification.


Subject(s)
Electrodes , Nanotubes, Carbon , Oxidation-Reduction , Water Purification , Nanotubes, Carbon/chemistry , Water Purification/methods , Catalysis
20.
J Environ Manage ; 365: 121638, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38959766

ABSTRACT

In the sludge dewatering process, a formidable challenge arises due to the robust interactions between extracellular polymeric substances (EPS) and bound water. This study introduces a novel, synergistic conditioning method that combines iron (Fe2+)/peroxymonosulfate (PMS) and polyacrylamide (PAM) to significantly enhance sludge dewatering efficiency. The application of the Fe2+/PMS-PAM conditioning method led to a substantial reduction in specific filtration resistance (SFR) by 82.75% and capillary suction time (CST) by 80.44%, marking a considerable improvement in dewatering performance. Comprehensive analyses revealed that pre-oxidation with Fe2+/PMS in the Fe2+/PMS-PAM process effectively degraded EPS, facilitating the release of bound water. Subsequently, PAM enhanced the flocculation of fine sludge particles resulting from the advanced oxidation processes (AOPs). Furthermore, analysis based on the Extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory demonstrated shifts in interaction energies, highlighting the breakdown of energy barriers within the sludge and a transition in surface characteristics from hydrophilic (3.79 mJ m-2) to hydrophobic (-61.86 mJ m-2). This shift promoted the spontaneous aggregation of sludge particles. The innovative use of the Flory-Huggins theory provided insights into the sludge filtration mechanism from a chemical potential perspective, linking these changes to SFR. The introduction of Fe2+/PMS-PAM conditioning disrupted the uniformity of the EPS-formed gel layer, significantly reducing the chemical potential difference between the permeate and the water in the gel layer, leading to a lower SFR and enhanced dewatering performance. This thermodynamic approach significantly enhances our understanding of sludge dewatering and conditioning. These findings represent a paradigm shift, offering innovative strategies for sludge treatment and expanding our comprehension of dewatering and conditioning techniques.


Subject(s)
Acrylic Resins , Iron , Sewage , Waste Disposal, Fluid , Sewage/chemistry , Iron/chemistry , Acrylic Resins/chemistry , Waste Disposal, Fluid/methods , Flocculation , Peroxides/chemistry , Oxidation-Reduction , Filtration
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