Nano-confined catalysis with Co nanoparticles-encapsulated carbon nanotubes for enhanced peroxymonosulfate oxidation in secondary effluent treatment: Water quality improvement and membrane fouling alleviation.

Despite widespread deployment and investigation of ultrafiltration (UF) for secondary effluent purification, the challenge of membrane fouling due to effluent organic matter (EfOM) remains formidable. This study introduced a novel pretreatment method utilizing Co nanoparticles-encapsulated carbon nanotubes activated peroxymonosulfate (Co@CNT/PMS) to degrade EfOM and mitigate membrane fouling. Characterization of Co@CNT revealed the efficient encapsulation of Co nanoparticles within nanotubes, which notably enhanced the catalytic degradation of bisphenol A and typical organics. The tube-encapsulated structure increased the concentration of reactive species within the confined nanoscopic space, thereby improving the probability of collisions with pollutants and promoting their degradation. The Co@CNT/PMS pretreatment led to substantial reductions in aromatic compounds, fluorescent components, and both high and middle molecular weight substances. These changes proved crucial in diminishing the fouling potential in subsequent UF processes, where reversible and irreversible fouling resistances decreased by 97.1 % and 72.8 %, respectively. The transition volume from pore blocking to cake filtration markedly increased, prolonging the formation of a dense fouling layer. Surface properties analysis indicated a significant reduction of pollutants on membrane surfaces after the Co@CNT/PMS pretreatment. This study underscored the efficacy of confinement-based advanced oxidization pretreatment in enhancing UF performance, presenting a viable resolution to membrane fouling.

Cobalt single-atom catalyst tailored ceramic membrane for selective removal of emerging organic contaminants.

Water reuse is an effective way to solve the issues of current wastewater increments and water resource scarcity. Ultrafiltration, a promising method for water reuse, has the characteristics of low energy consumption, easy operation, and high adaptability to coupling with other water treatment processes. However, emerging organic contaminants (EOCs) in municipal wastewater cannot be effectively intercepted by ultrafiltration, which poses significant challenges to the effluent quality and sustainability of ultrafiltration process. Here, we develop a cobalt single-atom catalyst-tailored ceramic membrane (Co1-NCNT-CM) in conjunction with an activated peroxymonosulfate (PMS) system, achieving excellent EOCs degradation and anti-fouling performance. An interfacial reaction mechanism effectively mitigates membrane fouling through a repulsive interaction with natural organic matter. The generation of singlet oxygen at the Co-N3-C active sites through a catalytic pathway (PMS→PMS∗→OH∗→O∗→OO∗→1O2) exhibits selective oxidation of phenols and sulfonamides, achieving >90% removal rates. Our findings elucidate a multi-layered functional architecture within the Co1-NCNT-CM/PMS system, responsible for its superior performance in organic decontamination and membrane maintenance during secondary effluent treatment. It highlights the power of integrating Co1-NCNT-CM/PMS systems in advanced wastewater treatment frameworks, specifically for targeted EOCs removal, heralding a new direction for sustainable water management.

Nanofiltration Membranes with Salt-Responsive Ion Valves for Enhanced Separation Performance in Brackish Water Treatment: A Battle against the Limitation of Salt Concentration.

Utilizing brackish water resources has imposed a high requirement on the design and construction of nanofiltration membranes. To overcome the limitation of high salt concentration on the nanofiltration separation performance resulting from the weakened Donnan effect, a nanofiltration membrane with the effect of salt-responsive ion valves was developed by incorporating zwitterionic nanospheres into the polyamide layer (PA-ZNs). The interaction between the nanospheres and membranes at high salinity was revealed through a combination analysis from the perspectives of water transport model, positron annihilation spectroscopy, and solute rejection, contributing to the formation of the valve effect. The PA-ZNs membrane presented a breakthrough in overcoming the limitation of increased salt concentrations on nanofiltration separation performance, achieving a high selectivity of 105 for mono/multivalent anions. To reveal the role of the ion valve effect in ion transport through the membrane, the membrane conductance was determined at different salt concentrations, confirming channel-controlled transport at low salinity and ion valve-controlled transport at high salinity. Moreover, the main membrane separation mechanisms were systematically studied. The concept of salt-responsive ion valves may contribute to expanding the application of nanofiltration in brackish water treatment.

A passive-active combined strategy for ultrafiltration membrane fouling control in continuous oily wastewater purification.

Membrane-based technology has been confirmed as an effective way to treat emulsified oily wastewater, however, membrane fouling is still one of practical challenges in long-term operation. Herein, a novel passive-active combined strategy was proposed to control membrane fouling in continuous oily wastewater purification, where the δ-MnO2 decoration layer helped to reduce the total fouling ratio (passive strategy for fouling mitigation) and the catalytic cleaning effectively removed the irreversible oil fouling (active strategy for fouling removal). The functional membrane was prepared via in-situ modification, referred to as δ-MnO2@TA-PES. The morphology, crystalline phase, chemical structure and surface properties of the membranes were systematically characterized. Compared with PES, the δ-MnO2@TA-PES possessed superhydrophilicity, enhanced electronegativity and narrowed pore size. The δ-MnO2@TA-PES achieved high water permeation flux of 723.9 L·m - 2·h - 1·bar-1, excellent oil rejection with separation efficiency above 98.5% for various emulsions, and durable anti-oil-fouling performance with FRRb of 98.0%. Notably, the oil cake layer fouling on δ-MnO2@TA-PES was greatly alleviated owing to its enhanced surface properties. In addition, δ-MnO2@TA-PES showed high cleaning efficiency in the peroxymonosulfate (PMS) cleaning process, where the radical and nonradical pathways occurred simultaneously. And the active substances generated in the nonradical process (especially 1O2) were considered as the main contributor to the reduction of irreversible fouling. Overall, the novel strategy of fouling control ensured the efficient operation of ultrafiltration membranes for the continuous oily wastewater purification.

Synergistic effects of prokaryotes and oxidants in rapid sand filters treatment of groundwater versus surface water: Purification efficacy, stability and associated mechanisms.

Effective elimination of manganese (Mn) and ammonium (NH4+-N) from drinking water is still challenging. Utilizing oxidants to improve the simultaneous removals of Mn and NH4+-N from rapid sand filter (RSF) systems has been extensively studied. However, the prokaryotes containing in the water geochemical properties greatly affected the RSF performance. In this study, groundwater and micro-polluted surface water were used to compare with/without potassium permanganate (KMnO4) assistant on the contaminants removals and system stability. Results showed that KMnO4 reduced the start-up period of RSF for treating groundwater and surface water to 20 and 41 days, respectively, with excellent Mn removal rates (>97%). The relative abundance of efficient ammonia-oxidizing bacteria (Nitrospira) in RSF treated groundwater without KMnO4 was higher than that in RSFs treated micro-polluted surface water or with KMnO4, resulting in a higher NH4+-N removal rate of the former (∼57%). Notably, KMnO4 and prokaryotes synergistically contributed to the amorphous structure, mixed phases (buserite, MnO2 and birnessite) and mixed-valence Mn system of active manganese oxides (MnOx), whose abundant oxygen vacancies and highly reactive Mn(III) favored the autocatalytic oxidation of Mn, while NH4+-N removal relied more on bacteria actions. Additionally, prokaryotes enriched the bacterial community diversity, leading to a more stable RSF system when facing hydraulic loading shock. This paper provided new insight into the synergistic effect of KMnO4 and prokaryotes on Mn and NH4+-N eliminations in RSFs and was helpful for practical applications.

Nanofiltration Membranes with Octopus Arm-Sucker Surface Morphology: Filtration Performance and Mechanism Investigation.

Precisely tailoring the surface morphology characteristics of the active layers based on bionic inspirations can improve the performance of thin-film composite (TFC) membranes. The remarkable water adsorption and capture abilities of octopus tentacles inspired the construction of a novel TFC nanofiltration (NF) membrane with octopus arm-sucker morphology using carbon nanotubes (CNTs) and beta-cyclodextrin (ß-CD) during interfacial polymerization (IP). The surface morphology, chemical elements, water contact angle (WCA), interfacial free energy (ΔG), electronegativity, and pore size of the membranes were systematically investigated. The optimal membrane exhibited an enhanced water permeance of 22.6 L·m-2·h-1·bar-1, 180% better than that of the TFC-control membrane. In addition, the optimal membrane showed improved single salt rejections and monovalent/divalent ion selectivity and can break the trade-off effect. The antiscaling performance and stability of the membranes were further explored. The construction mechanism of the octopus arm-sucker structure was excavated, in which CNTs and ß-CD acted as arm skeletons and suckers, respectively. Furthermore, the customization of the membrane surface and performance was achieved through tuning the individual effects of the arm skeletons and suckers. This study highlights the noteworthy potential of the design and construction of the surface morphology of high-performance NF membranes for environmental application.

Toward Enhancing Desalination and Heavy Metal Removal of TFC Nanofiltration Membranes: A Cost-Effective Interface Temperature-Regulated Interfacial Polymerization.

Polyamide (PA) chemistry-based nanofiltration (NF) membranes have an important role in the field of seawater desalination and wastewater reclamation. Achieving an ultrathin and defect-free active layer via precisely controlled interfacial polymerization (IP) is an effective routine to improve the separation efficiencies of NF membranes. Herein, the morphologies and chemical structures of the thin-film composite (TFC) NF membranes were accurately regulated by tailoring the interfacial reaction temperature during the IP process. This strategy was achieved by controlling the temperature (-15, 5, 20, 35, and 50°) of the oil-phase solutions. The structural compositions, morphological variations, and separation features of the fabricated NF membranes were studied in detail. In addition, the formation mechanisms of the NF membranes featuring different PAs were also proposed and discussed. The temperature-assisted IP (TAIP) method greatly changed the compositions of the resultant PA membranes. A very smooth and thin PA film was obtained for the NF membranes fabricated at a low interfacial temperature; thus, a high 19.2 L m-2 h-1 bar-1 of water permeance and 97.7% of Na2SO4 rejection were observed. With regard to the NF membranes obtained at a high interfacial temperature, a lower water permeance and higher salt rejection with fewer membrane defects were achieved. Impressively, the high interfacial temperature-assisted NF membranes exhibited uniform coffee-ring-like surface morphologies. The special surface-featured NF membrane showed superior separation for selected heavy metals. Rejections of 93.9%, 97.9%, and 87.7% for Cu2+, Mn2+, and Cd2+ were observed with the optimized membrane. Three cycles of fouling tests indicated that NF membranes fabricated at low temperatures exhibited excellent antifouling behavior, whereas a high interface temperature contributed to the formation of NF membranes with high fouling tendency. This study provides an economical, facile, and universal TAIP strategy for tailoring the performances of TFC PA membranes for environmental water treatment.

High-performance nanofiltration membranes with a sandwiched layer and a surface layer for desalination and environmental pollutant removal.

To overcome the permeability-selectivity limitation and improve the performance of desalination membranes, novel methods and design strategies are needed to prepare new types of thin film composite (TFC) nanofiltration (NF) membranes. In this work, a modified TFC membrane with a sandwiched layer and a surface layer was fabricated through a facile additional two-step approach. The microfiltration (MF) substrate and TFC surface were modified by a cellulose nanocrystal (CNC) sandwiched layer and a polydopamine (PDA) layer, respectively. Scanning electron microscopy (SEM) analysis indicated that the support modified by CNCs presented a more homogeneous surface than the control TFC. Cross-sectional SEM images showed that the underneath MF support, CNC interlayer, polyamide layer and PDA deposition layer were perfectly integrated. The surface charge was determined by an electrophoretic analyzer and revealed that the CNC interlayer increased the membrane electronegativity, while the PDA layer presented the opposite effect. Compared to the control TFC membrane, the solute permeability and rejection of the resultant CNC-TFC-PDA membrane were simultaneously increased, indicating a breakthrough in the trade-off limitation. The modified membranes exhibited a high removal rate for Congo red, Rose Bengal, sodium lignosulfonate and alkaline lignin, suggesting their excellent rejection performance for textile dyes and lignin derivatives. Fouling tests indicated that both the interlayer and surface layer exhibited positive effects on fouling alleviation. The effects of each functional layer were explored, and the main factors for performance improvement, including the modified hydrophilicity, surface charge, pore size and surface roughness, were discussed.