Bioleaching and Fenton technology are commonly used preconditioning techniques for sludge dewatering. This study compared the dewatering mechanisms of different conditioning technologies. The results showed that bound water, specific resistance to filtration (SRF), and capillary suction time decreased from 3.95 g/g, 6.16 × 1012 m/kg, and 130.6 s to 3.15 g/g, 2.81 × 1011 m/kg, and 33 s, respectively, under combined treatment condition. Moreover, the free radicals, including ·OH, O2-·and Fe (Ⅳ), further damaged the cell structure, thus increasing the concentration of DNA in the S-EPS layer. This intense degradation sludge particle size decreased by 15.6% and significantly increased zeta potential. Under the combined technology, the α-helix and β-sheet decreased by 42.2% and 56.5%, respectively, destabilizing the spatial structure of proteins and promoting the release of bound water. In addition, the combined technology decreased (Ala/Lys) ratio in the TB-EPS layer by 67.6%, indicating the weakening of protein water-holding capacity. Moreover, the conversion of oxygen-containing compounds to nonpolar hydrocarbons increased the hydrophobicity of the sludge under a combined treatment, thus enhancing dewatering performance.

Transition metals are promising catalysts for environmental remediation. However, their low reactivity, poor stability and weak reusability largely limit practical applications. Herein, we report that the electron-rich dissolved black carbon (DBC) incorporated into the nanoscale zero-valent copper (nZVCu) can boost intrinsic reactivity, structural stability and cyclic reusability for superior peroxymonosulfate (PMS) activation and pollutant degradation. A series of refractory pollutants can be effectively removed on the DBC/nZVCu, in comparison with the nZVCu reference. Hydroxyl radical (‧OH) is identified as the dominant reactive oxygen species by electron spin resonance (ESR) and chemical quenching tests, mediated by the metastable Cu(III) as the key reactive intermediate. The electron-rich DBC protects nanoscale Cu from oxidative corrosion to slow down the surface formation of inert CuO layer, rendered by the thermodynamically and dynamically capacitive regulation of corrosive electron transfer from metallic core. By this refining way, the conducive DBC improves the neighboring utilization of reactive electron during metal corrosion, oxidant activation, radical generation and pollutant degradation in Fenton-like catalysis. Our findings suggest that the ubiquitous DBC can be an efficient chelating agent to refine transition metals by serving as the surface deactivator and electron mediator, and take new insights into their environmental and agricultural geochemistry.

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.

For the efficient degradation of organic pollutants with the goal of reducing the water environment pollution, we employed an alkaline hydrothermal treatment on primeval g-C3N4 to synthesize a hydroxyl-grafted g-C3N4 (CN-0.5) material, from which we engineered a novel Fenton-like catalyst, known as Cu-CN-0.5. The introduction of numerous hydroxyl functional groups allowed the CN-0.5 substrate to stably fix active copper oxide particles through surface complexation, resulting in a low Cu leaching rate during a Cu-CN-0.5 Fenton-like process. A sequence of characterization techniques and theoretical calculations uncovered that interfacial complexation induced charge redistribution on the Cu-CN-0.5 surface. Specifically, some of the π electrons in the tris-s-triazine units were transferred to the copper oxide particles along the newly formed chemical bonds (C(π)-O-Cu), forming a π-deficient area on the tris-s-triazine plane near the complexation site. In a typical Cu-CN-0.5 Fenton-like process, a stable π-π interaction was established due to the favorable positive-negative match of electrostatic potential between the aromatic pollutants and π-deficient areas, leading to a significant improvement in Cu-CN-0.5\'s adsorption capacity for aromatic pollutants. Furthermore, pollutants also delivered electrons to the Cu-CN-0.5 Fenton-like system via a \"through-space\" approach, which suppressed the futile oxidation of H2O2 in reducing the high-valent Cu2+ and significantly improved the generation efficiency of •OH with high oxidative capacity. As expected, Cu-CN-0.5 not only exhibited an efficient Fenton degradation for several typical aromatic organic pollutants, but also demonstrated both a low metal leaching rate (0.12 mg/L) and a H2O2 utilization rate exceeding 80%. The distinctive Fenton degradation mechanism substantiated the potential of the as-prepared material for effective wastewater treatment applications.

Give the emergence of drug resistance in bacteria resulting from antibiotic misuse, there is an urgent need for research and application of novel antibacterial approaches. In recent years, nanoparticles (NPs) have garnered significant attention due to their potential to disrupt bacteria cellular structure through loading drugs and special mechanisms, thus rendering them inactive. In this study, the surface of hollow polydopamine (HPDA) NPs was utilized for the growth of Prussian blue (PB), resulting in the formation of HPDA-PB NPs. Incorporation of Co element during the preparation process led to partial doping of PB with Co2+ions. The performance test results demonstrated that the HPDA-PB NPs exhibited superior photothermal conversion efficiency and peroxidase-like activity compared to PB NPs. HPDA-PB NPs have the ability to catalyze the formation of hydroxyl radicals from H2O2in a weakly acidic environment. Due to the tiny PB particles on the surface and the presence of Co2+doping, they have strong broad-spectrum antibacterial properties. Bothin vitroandin vivoevaluations confirm their efficacy against various bacterial strains, particularlyStaphylococcus aureus, and their potential to promote wound healing, making them a promising candidate for advanced wound care and antimicrobial applications.

Wolframite (FeWO4), a typical polyoxometalate, serves as an auspicious candidate for heterogeneous catalysts, courtesy of its high chemical stability and electronic properties. However, the electron-deficient surface-active Fe species in FeWO4 are insufficient to cleave H2O2 via Fe redox-mediated Fenton-like catalytic reaction. Herein, we doped Sulfur (S) atom into FeWO4 catalysts to refine the electronic structure of FeWO4 for H2O2 activation and sulfamethoxazole (SMX) degradation. Furthermore, spin-state reconstruction on S-doped FeWO4 was found to effectively refine the electronic structure of Fe in the d orbital, thereby enhancing H2O2 activation. S doping also accelerated electron transfer during the conversion of sulfur species, promoting the cycling of Fe(III) to Fe(II). Consequently, S-doped FeWO4 bolstered the Fenton-like reaction by nearly two orders of magnitude compared to FeWO4. Significantly, the developed S-doped FeWO4 exhibited a remarkable removal efficiency of approximately 100% for SMX within 40 min in real water samples. This underscores its extensive pH adaptability, robust catalytic stability, and leaching resistance. The matrix effects of water constituents on the performance of S-doped FeWO4 were also investigated, and the results showed that a certain amount of Cl-, SO42-, NO3-, HCO3- and PO43- exhibited negligible effects on the degradation of SMX. Theoretical calculations corroborate that the distinctive spin-state reconstruction of Fe center in S-doped FeWO4 is advantageous for H2O2 decomposition. This discovery offers novel mechanistic insight into the enhanced catalytic activity of S doping in Fenton-like reactions and paves the way for expanding the application of FeWO4 in wastewater treatment.

In recent years, as global industrialization has intensified, environmental pollution has become an increasingly serious problem. Improving water quality and achieving wastewater purification remain top priorities for environmental health initiatives. The Fenton process is favored by researchers due to its high efficiency and ease of operation. Central to the Fenton process is a catalyst used to activate hydrogen peroxide, rapidly degrading pollutants, improving water quality. Among various catalysts developed, copper-based catalysts have attracted considerable attention due to their affordability, high activity, and stable performance. Based on this, this paper reviews the development of copper-based Fenton systems over the past decade. It mainly involves the research and application of copper-based catalysts in different Fenton systems, including photo-Fenton, electro-Fenton, microwave-Fenton, and ultrasonic-Fenton. This review provides a fundamental reference for the subsequent studies of copper-based Fenton systems, contributing to the goal of transitioning these systems from laboratory research into practical environmental applications.

The pervasive presence of pathogenic bacteria in water environment poses a serious threat to public health. Here, a photocatalytic cascade was developed to reveal great water disinfection. Firstly, N-doped carbon nanosheets (N-CNSs) about 30-50 nm in size were synthesized by a hydrothermal strategy. It revealed wide-spectrum photocatalysis for H2O2 generation via a typical two-step single-electron process. A Fenton agent (Fe ion) was loaded, N-CNSs-Fe can in-situ convert photocatalytic H2O2 into ·OH with high oxidation potential. Moreover, its Fenton active is three times greater than pure Fe2+ owing to electron enrichment from N-CNSs to Fe for Fe3+/Fe2+ cycle. Further investigation displayed that Fe loading also could decrease bad gap and promote charge separation to boost photocatalysis. In addition, N-CNSs-Fe possesses positive surface potential to exhibit strong interaction with negative bacteria, facilitating the capture. Therefore, the nanocomposite can effectively inactivate E. coli with a lethality rate of 99.7 % under stimulated sunlight irradiation. In addition, it also was employed to treat a complex lake water sample, revealing great antibacterial (95.1 %) and dye-decolored (92.3 %) efficiency at the same time. With novel biocompatibility and antibacterial ability, N-CNSs-Fe possessed great potential for water disinfection.

The present study provided an innovative insight into the formation mechanism of persistent free radicals (PFRs) during the pyrolysis of Fenton-conditioned sludge. Fenton conditioners simultaneously improve the dewatering performance of sewage sludge and catalyze the pyrolysis of sewage sludge for the formation of PFRs. In this process, PFRs with a total number of spins of 9.533×1019 spins/g DS could be generated by pyrolysis of Fenton-conditioned sludge at 400°C. The direct thermal decomposition of natural organic matter (NOM) fractions contributed to the formation of carbon-centered radicals, while the Maillard reaction produced phenols precursors. Additionally, the reaction between aromatic proteins and iron played a crucial role in the formation of phenoxyl or semiquinone-type radicals. Kinetics analysis using discrete distributed activation energy model (DAEM) demonstrated that the average activation energy for pyrolysis was reduced from 178.28 kJ/mol for raw sludge to 164.53 KJ/mol for Fenton conditioned sludge. The reaction factor (fi) indicated that the primary reaction in Fenton-conditioned sludge comprised of 27 parallel first-order reactions, resulting from pyrolysis cleavage of the NOM fractions, the Maillard reaction, and iron catalysis. These findings are significant for understanding the formation process of PFRs from NOM in Fenton-conditioned sludge and provide valuable insight for controlling PFRs formation in practical applications.

Effective and economical processes for the advanced treatment of coking wastewater were urgently needed to reduce the persistent organic pollutants of external drainage. In the present work, we investigated the degradation of organic pollutants in coking wastewater through IHC/FO (imping stream hydrodynamic cavitation (IHC) coupled with the Fenton oxidation (FO) process) and IHC alone for their feasibility in the advanced treatment of coking wastewater. To select the optimum parameters, attention was paid to the effects of main operation conditions including inlet fluid pressure, medium temperature, initial pH, reaction time, and initial Fe(II) and initial H2O2 concentrations. The results showed that the effects of conditions that need energy to be maintained (such as initial pH and inlet pressure) on the organic pollutant removal efficiency through IHC/FO were less pronounced than those through IHC alone. Moreover, the application of IHC/FO could remove more organic pollutants from coking wastewater than IHC even at an energy-efficient condition. For example, the highest COD removal efficiency of 12.5% was achieved in the IHC treatment at 0.4 MPa, pH 3, and 60 min for the reaction time. In the case of IHC/FO, the maximum COD removal of 33.2% was obtained at pH 7, 0.1 MPa, 12 mmol/L H2O2, and 3 mmol/L Fe2+ after reacting for 15 min. The ultraviolet and visible spectrophotometry (UV-Vis) absorption spectra and gas chromatography and mass spectrometry (GC-MS) analysis further revealed that the kinds and amounts of pollutants (especially those that had benzenes) remaining in water treated through IHC/FO were much fewer and smaller than in water treated through IHC alone. The better performances of IHC/FO than IHC alone were likely related to the more hydroxyl radicals produced through IHC/FO. Taken together, our findings indicate that IHC/FO has great application potential in the advanced treatment of coking wastewater.