Conventional covalent organic framework (COF)-modified membranes are often plagued by limited visible-light photocatalytic activity and poor self-cleaning performance. To tackle this, a novel bismuth oxybromide (BiOBr)/TpPa-1-PVDF membrane was fabricated via phase inversion. The optimal membrane (M-1.5) achieved a pure water flux of 101.75 Lm(-2)h(-1)bar(-1), which is 2.6 times higher than that of the pristine PVDF membrane, while maintaining high rejection rates (> similar to 90 %) for both Congo Red (CR) and Eriochrome Black T. More importantly, it demonstrated exceptional self-cleaning capability, achieving nearly complete degradation of adsorbed CR within 120 min under visible light irradiation. ESR analysis pinpointed the generation of OH and O-2(-) radicals as the key mechanism behind this efficient photocatalytic degradation. The membrane's practicality is further underscored by its outstanding recyclability over 8 cycles (20 h) and stable performance during a prolonged 60-hour filtration test (with light exposure every 10 h), confirming its long-term durability. This work provides a scalable strategy for developing multifunctional membranes that integrate high separation efficiency with robust visible-light-driven self-cleaning, demonstrating significant potential for sustainable wastewater treatment.

Herein, for the first time, MOF-on-MOF-derived CuO/Co3O4 composites with core-shell structure is prepared. The internal electric field formed at the heterojunction interface can accelerate charge transfer and offer more active sites, so enhancing the performance of CuO/Co3O4 composites in formaldehyde degradation via peroxymonosulfate (PMS) activation. It is surprised to find that the adjustment of core and shell position in CuO/Co3O4 composites has an important impact on the mechanism of PMS activation. Under the mediation of internal electric field, free electron will gather around Co3O4 component of CuO/Co3O4 composites. When Co3O4 is served as the shell of CuO/Co3O4 composite (marked as CuO/Co3O4-1), CuO/Co3O4 composite will become electron donor and provide electron to activate PMS for producing SO4 center dot- and OH center dot, which can oxidize formaldehyde into CO2 and H2O. Interestingly, CuO/Co3O4 composite will become electron acceptor when CuO is employed as the shell (denoted as CuO/Co3O4-2), so PMS can be easily oxidized into SO5 center dot- and then decomposed into 1O2. Due to the feature of 1O2 being moderate oxidation ability, formaldehyde can be selectively converted by 1O2 into formic acid with high economic value. Additionally, theoretical calculation based on density functional theory further proves these results. This work clarifies the effects of core and shell exchanges in CuO/ Co3O4 composite on catalytic activity, sharing some new insights for selective degradation of formaldehyde.

The treatment of complex wastewater containing coexisting immiscible oils and soluble organic pollutants remains a critical challenge for conventional remediation technologies. Existing strategies often lack the integrated multifunctionality required for simultaneous separation and degradation, leading to operational inefficiencies and secondary pollution. Drawing inspiration from the fluid transport architecture of wood xylem, a vertically aligned lamellar microstructure with vessel-like channels was constructed from waste silk fibroin (SF), achieving ultrafast capillary-driven uptake with saturation within 5 s. Glycerol in this system plays a triple role, as a plasticizer, molecular crowding agent, and interfacial compatibilizer, transforming fragile pore walls into a robust interconnected network. Subsequent hierarchical coating with polydimethylsiloxane (PDMS) and TiO2 nanoparticles endows stable superhydrophobicity (water contact angle of 144.1 degrees) and efficient photocatalytic activity. Under simulated solar light, the composite sponge achieved a 79% degradation of Rhodamine B within 3.5 h, which was further enhanced to 98% via a synergistic photocatalytic-Fenton reaction with H2O2. The optimized material retains 92% of its initial adsorption capacity after five cycles. By integrating rapid pollutant enrichment with photocatalytic degradation, this waste-derived, sustainable platform offers a promising strategy for advanced, integrated wastewater remediation.

Toxic and carcinogenic organic pollutants in wastewater severely threaten public health and environmental sustainability. Advanced oxidation processes (AOPs) can degrade such pollutants by generating highly reactive species, but their efficiency and durability depend heavily on the reaction pathways and mechanisms. Non-radical pathways offer notable advantages for complex wastewater due to their strong resistance to interference from impurities and coexisting ions. Herein, we demonstrate that the entropy can drive a transition in the peroxymonosulfate (PMS) activation mechanism from a free-radical- to a non-radical-dominated pathway. This is exemplified by the Co55Fe15Cu10Mn10Ni10 high-entropy alloy (HEA), which achieves over 98% degradation of rhodamine B within 15 minutes using a low PMS dosage of 0.15 g L-1, significantly outperforming monometallic and binary alloy catalysts. The non-radical mechanism combined with the high structural stability of HEA catalysts also grants exceptional resistance to coexisting ions and reliable performance in real water samples with multiple impurities. These findings highlight the promise of HEA catalysts in addressing key challenges in wastewater treatment, including pollutant diversity, impurity resilience, and system durability.

Electrocatalytic nitrogen reduction reaction (e‑NRR) is a green and environmentally friendly process that uses renewable electricity to convert nitrogen into ammonia under ambient conditions. Theoretical prediction of novel catalysts for the e‑NRR remains difficult. Single-atom alloys (SAAs) offer a viable solution, as they have well-defined theoretical models and can be readily obtained. We systematically investigate a series of transition‑metal (TM)‑doped Ag‑based single‑atom alloys (TM1-Ag(111)) as model e‑NRR catalysts using first‑principles calculations, where TM1 denotes a single TM atom. Our results indicate that Re1‑ and Os1‑Ag(111) show superior e-NRR activity, with limiting potentials as low as -0.29 and -0.49V, respectively. These catalysts also powerfully inhibit the hydrogen evolution reaction, leading to high e‑NRR selectivity. Moreover, we employ an intrinsic descriptor that directly predicts the limiting potential, eliminating the need for first-principles calculations, and confirm its scalability on Cu‑ and Au‑based SAAs. Our findings deliver a scalable design principle, providing atomic‑level guidance to accelerate the development of efficient and sustainable e‑NRR catalysts.

Thallium (Tl) is a highly toxic trace element that poses considerable risks to ecosystems and human health even at very low concentrations, creating an urgent demand for efficient and rapid treatment technologies. In this work, a high-entropy Prussian blue analogue (HE-PBA) is prepared and systematically investigated as an adsorbent for the removal of aqueous Tl(I). By incorporating six transition metals (Fe, Co, Ni, Cu, Mn, and Zn) into a high-entropy framework, the HE-PBA achieves a maximum adsorption capacity of 792.43 mg/g at neutral pH, surpassing conventional analogues. Tl(I) uptake is rapid, with adsorption equilibrium attained within 30 min, attributed to fast hydrated ion transport through open pore channels rather than sluggish lattice diffusion. The material exhibits stable removal performance over a wide pH range (1-12) and strong selectivity in the presence of high concentrations of coexisting ions and natural organic matter. Tests conducted using Tl(I)spiked Pearl River water demonstrate that HE-PBA can effectively reduce Tl(I) concentrations to below the drinking water guideline value of 0.1 mu g/L. The adsorption kinetics and equilibrium behavior are well described by the pseudo-second-order kinetic model and the Freundlich isotherm, respectively, indicating a chemisorptiondominated process involving multilayer uptake. Characterization results obtained from XRD, FTIR, XPS, and BET analyses suggest that Tl(I) removal proceeds via a synergistic mechanism dominated by lattice intercalation and Tl+/K+ ion exchange, which are facilitated by zeolitic water molecules and the structural adaptability of the high-entropy framework. Overall, the high adsorption capacity, rapid kinetics, and strong selectivity highlight the potential of HE-PBA for the remediation of Tl(I)-contaminated waters.

Nonradical pathway-dominated peracetic acid (PAA) advanced oxidation processes (AOPs) with efficient degradation, strong adaptability and ecological safety, offer a promising strategy in antibiotic wastewater treatment. In this study, cobalt (Co) single-atom anchored g-C3N4 (CN) with low loading of Co, named CoCN catalyst, was successfully synthesized with a typical Co-N4 moiety and applied as a PAA activator for the oxidation of sulfadimethoxine (SDM) at a low-dose of PAA (0.04 mM). The experiments and theoretical calculations implied the formation of singlet oxygen (1O2), high-valent cobalt-oxo species (CoIV=O), surface reactive complex (CoCN-PAA*) and organic radicals (R-O center dot) during the oxidation process, and 1O2 was the dominant reactive species for the degradation of SDM. Mechanistic investigations revealed a novel nonradical pathway in PAA activation with the formation of CoCN-O* intermediate that favored 1O2 generation. The CoCN/PAA system exhibited favorable SDM degradation and detoxification, broad-spectrum degradation capability for various SAs, high durability in a continuous-flow fixed-bed reactor after 36-hour run, strong resistance to certain coexisting matter, and less than satisfied SDM removal in real water caused by the presence of HCO3-and natural organic matter (NOM). The study offers novel insights into the nonradical mechanism involved in cobalt single-atom catalyst-mediated PAA activation processes for water decontamination.

A magnetic shell-structured nano-catalyst was prepared by self-polymerization of dopamine wrapped by ferric oxide as the carrier, which was loaded with palladium nanoparticles (Pd/PDA@Fe3O4). The presence of magnetic Fe3O4 made it easy for nanoscale palladium particles to recover and prevent the loss of palladium nanoparticles that is unavoidable in traditional usage and preparation procedures. The catalyst was characterized by X-ray diffraction, fourier transform infrared spectroscopy, scanning electron microscopy, thermal weight loss analysis, Raman spectroscopy, X-ray photo-electron spectroscopy, and magnetic properties analysis. The catalytic performance of the prepared catalyst was investigated taking 4-nitrophenol (10 mg/L) and rhodamine B (15 mg/L) as the target pollutants. The results showed that under the conditions of 35 °C, pH = 7 and a catalyst dosage of 3 mg, the catalytic reduction efficiency of 4-nitrophenol, rhodamine B, and the mixture of them all can reach 99%. The catalytic efficiency of Pd/PDA@Fe3O4 remained above 90% after being used 10 times. The shell structure of Fe3O4 made it possible and easy to recover and recycle the nanoscale palladium, which was a real problem in the usage of nano-catalysts. At the same time, the problem of separation and recovery of palladium nano-catalyst is solved by magnetism, which provides research ideas for the recycling and utilization of nano-materials.

Precise modulation of interfacial electron transfer in heterogeneous catalysts is crucial for efficient degradation of persistent organic pollutants in persulfate-based advanced oxidation processes. In this work, we introduced a photoswitching strategy that in situ regulates electron transfer in single-atom Co-TiO2 catalysts, optimizing the production of reactive oxidative species during peroxymonosulfate (PMS) activation, thereby improving pollutant mineralization efficiency. Theoretical calculations revealed that the formation of high-valent Co-oxo species during PMS activation was thermodynamically favorable. By modulating photogenerated electron flow, the process dynamically shifted between nonradical and radical pathways. A dark-light interval system derived from this photoswitching approach significantly improved contaminant removal, with bisphenol A mineralization efficiency increasing from 29.50% in the dark and 47.81% under continuous light to 62.62% with the interval system. Similar improvements were observed in the treatment of practical coking wastewater. This study proposes a novel light-modulated PMS activation strategy that offers a promising solution for advanced pollutant degradation and sustainable wastewater treatment.

Metal-free g-C3N4 semiconductor has been extensively utilized as green catalyst for visible-light-driven degradation of various organic contaminants. However, its application has been constrained due to its inherent shortcomings, including weak visible light adsorption, low specific surface area and high recombination rate of electron-hole pairs. Herein, a novel carbon nitride (C2N3) photocatalyst was synthesized via a one-step calcination method utilizing 3-amino-1,2,4-triazole (3-AT) as precursor for the first time. Unlike widely reported two-dimensional carbon nitride materials, the obtained C2N3 exhibited a granular-like morphology with relatively high specific surface area. Under visible light (lambda > 420 nm) irradiation, C2N3 exhibited an excellent photocatalytic activity for Rhodamine B (RhB) degradation, due to its stronger visible-light absorption, faster photogenerated electron-hole separation and easier charge transfer, surpassing that of the popular g-C3N4. After 5 cycles, the degradation efficiency of RhB still remained over 94 %, suggesting high stability and reusability. Moreover, the C2N3/Vis system had high adaptabilities to temperature, solution pH and organic pollutant, even in the presence of high concentration of common matrix species like Cl-, NO3-, SO42- and humic acid. center dot O-2(-) and O-1(2) were revealed to be the main reactive species generated in the C2N3/Vis system, a combination process of radical and non-radical pathways for organic degradation. This work developed a novel granular-like C2N3 material for visible light photocatalysis, which showed an incredible potential in photocatalytic degradation of organic pollutants.

Despite growing interest in single-atom catalysts (SACs) for Fenton-like reactions, zinc (Zn)-based SACs remain unexplored due to the inherent inertness of Zn2+, whose fully occupied 3d10 electronic configuration limits redox activity. Here, we overcome this limitation by introducing boron (B) atoms to reconfigure the electronic structure of Zn-N4 coordination sites, yielding an activated catalyst denoted as Zn-NBC. This electronic modulation transforms inert Zn-N4 sites into catalytically active centers (Zn-NxB4- x), enabling significantly enhanced Fenton-like activity. Compared to the unmodified Zn-N4 catalyst (Zn-N4C), Zn-NBC exhibits a 26-fold increase in the rate of organic pollutant degradation. Density functional theory (DFT) calculations and experimental results reveal that Zn-N4C and Zn-NBC exhibit distinct PDS adsorption behaviors, with B incorporation tuning both adsorption strength and electronic interactions at the Zn center. Crystal orbital Hamilton population (COHP) analysis further demonstrates that the Zn-NBC facilitates the activation of the S─O bonds in peroxydisulfate (PDS), promoting the generation of reactive oxygen species, including peroxide radicals and singlet oxygen. These findings establish a new paradigm for activating electronically inert metal centers and position Zn-NBC as a promising platform for efficient and sustainable environmental remediation.

TS-1 zeolites with different grain sizes were prepared under hydrothermal conditions by tuning the amount of template agent, chelating agent, and temperature, which were further used as supports for the NiMo/TS-1 catalysts. The optimization of synthesis conditions has achieved controllable synthesis of grain sizes from nano-scale to micron-scale. TS-1 with smaller grain sizes possess larger specific surface area, external specific surface area, and pore volume, which can effectively shorten the diffusion path of the sulfide with complex structure. Nano-scale TS-1 has more highly-coordinated Ti species, acting as electronic additives to increase the sulfidation degree of the catalyst. Nano-scale NiMo/TS-1 exhibits higher acidity, which is beneficial for hydrodesulfurization (HDS) reactions. Among the series of NiMo/TS-1 catalysts, NiMo/TS-1 (120 nm) catalyst exhibits the highest dibenzothiophene (DBT, 88.4 %) and 4,6-dimethylbenzothiophene (4,6-DMDBT, 62.1 %) HDS activities.

The development of solid propellants is of strategic importance for supporting rocket application in aerospace field. However, the currently employed propellant materials inevitably encounter microcracks and defects generated in the storage, transportation and loading process, resulting in possible local overheating and undesired explosion accidents. Herein, a robust, strong and fast room-temperature self-healing polyurea-urethane (PU) adhesive was constructed based on the synergy of multiple hydrogen bonds reorganization and disulfide exchange reactions. The PU adhesive owns mechanical strength (38.13 MPa), elongation at break (947.17%), and toughness (109.65 MJ m-3) and rapid room-temperature (RT) self-healing efficiency (83.19% at RT for 24 h), forming strong RT self-healing propellant adhesive and surpassing many reported propellant adhesive systems to date. Moreover, benefiting from the dynamic recombination of widely dispersed hydrogen bonds and disulfide bonds, the as-prepared simulated propellant exhibits satisfactory crack-healing performance at RT for 24 h. This work provides valuable insight and achievable approach for promoting the exploring of highperformance RT self-healing propellants.

AuNPs/rGO composite cathode was prepared using in-situ reduction method and was applied for H2O2 generation through molecular oxygen (O2) undergoing a 2-electron reduction reaction in the electro-Fenton system. The results showed the AuNPs/rGO cathode exhibited good activity and stability. The size and loading amount of AuNPs, as well as applied voltages were considered for evaluating the catalytic activity of AuNPs/rGO cathode. AuNPs2:1/rGO with the smallest size (2.8 +/- 0.6 nm) exhibited higher catalytic activity in the electro-Fenton system when the AuNPs2:1 loading amount was 2.7 %, pH= 3, and applied voltage was-0.6 V (vs. SCE), resulting in an H2O2 yield of 19.3 +/- 0.1 mmol g- 1. The synergistic effect of AuNPs2:1 and rGO enhanced the activation of H2O2, generating a large number of hydroxyl radicals (center dot OH) for efficient degradation of rhodamine B (RhB), corresponding to a degradation efficiency of 100 % within 30 min. In addition, AuNPs2:1/rGO exhibited excellent stability and reusability in cyclic experiments. The quenching experiment and the radical spin trap test showed center dot OH and superoxide anion (center dot O2 and in-situ FTIR were used to analyze the intermediate products of the degradation process and determine the reaction mechanism. ) as the active species during the reaction process. Furthermore, LC-MS

Non-invasive inactivation of bacteria by photodynamic therapy (PDT) and photothermal therapy (PTT) has been recently concerned for biomaterials. A polymethyltrimethoxysilane (PMTMS)-crosslinked sodium copper chlorophyllin (SCC) coating was prepared on micro arc oxidation (MAO) coated magnesium alloy AZ31 by one-step dipping method. Results showed that the MAO/PMTMS-SCC coating had high corrosion resistance with two magnitudes decrease in corrosion current density. Profound physical barrier and sealing effects of PMTMS-SCC coating in the initial stage of immersion prevented in-diffusion of Cu2+, thus, primeval renegaded Cu was released to corrosive solution, instead of triggering galvanic corrosion. Antibacterial ratios under irradiation of 808 nm near infrared light against E. coli and S. aureus were 99.6% and 99.1%, respectively, which is ascribed to a triple antibacterial mechanism. Such a composite coating also displays high biocompatibility, which will promote the application of magnesium alloys in biomedical fields.

Fucoidan, a sulfated polysaccharide predominantly derived from brown algae, has garnered significant research interest due to its diverse biological activities and potential biomedical applications. This review systematically examines both established and novel extraction methods for fucoidan. Traditional techniques, including hot water, acid, and alkaline extraction, are summarized, alongside emerging approaches such as enzymatic hydrolysis, ultrasound-assisted, microwave-assisted, and subcritical water extraction, which demonstrate enhanced efficiency and yield. The paper further synthesizes the extensive research on the compound's multifaceted physiological functions, highlighting its immunomodulatory, anti-tumor, antioxidant, anticoagulant, lipid-lowering, and antiviral properties. These findings collectively underscore the critical relationship between fucoidan's structural characteristics—influenced by its monosaccharide composition, molecular weight, and sulfation pattern—and its resultant bioactivities. The conclusion affirms fucoidan's substantial value and broad applicability, particularly within the biomedical sector, for advancing health and therapeutic strategies.

Patterned quantum dots (QDs) integrated with blue or purple micro-light-emitting diodes (Micro LEDs) are pivotal for next-generation displays requiring ultrahigh brightness and resolution. However, the non-polar nature of native QDs ligands (e.g., oleic acid, oleylamine) impedes their uniform dispersion in photoresist, limiting the fabrication of high-performance QDs patterns. Here, we develop a ligand exchange strategy that replaces native ligands with 2-carboxyethylacrylate (CEA) under optimized light-shielded and ethanol-mediated conditions. The modified QDs exhibit homogeneous dispersion in photoresist, enabling the fabrication of 10 mu m x 10 mu m patterns via photolithography. Remarkably, the red QDs retain a photoluminescence quantum yield (PLQY) of 91.5 % post-exchange, with negligible shifts in emission peak wavelength or spectral linewidth. Notably, the red CEAmodified QDs maintain a PLQY of 69.3 % even after integration into photoresist and photolithographic patterning, demonstrating exceptional compatibility with device fabrication processes. This work provides a robust ligand engineering approach to advance QDs-based photolithography for high-resolution displays.

N atoms in carbonaceous catalysts are usually considered as the key active centers for catalytic/activated re -actions. However, the raise of N content in metal-carbonaceous composites is still a great challenge. In this work, the N content in Fe-embedded carbon nanotubes (Fe@CNTs) was greatly enriched via a Zn-N linkage process, giving Fe-embedded N-rich carbon nanotubes (Fe@NRCNTs). The N content of Fe@NRCNTs was up to 7.43 atom %, reaching the highest value among other Fe-embedded carbonaceous materials. Zn-N linkage could induce more active C sites in g-C3N4 intermediate for N-doping and inhibit the release of N-containing gases, resulting in N enrichment during the formation of Fe@NRCNTs. More importantly, the as-obtained Fe@NRCNTs exhibited excellent performance towards persulfate activation for tetracycline degradation, and its rate constant was four times higher than that of Fe@CNTs. The high N content provided more active site for nonradical activation, and also accelerated the electron transfer between Fe and CNTs, beneficial for radical activation. Furthermore, Fe@NRCNTs could work in a very wide pH range (2.2-10.3), accompanying with high adaptability and reus-ability. This work provided a feasible strategy to increase N content in metal-embedded carbonaceous materials for highly efficient radical and nonradical persulfate activation.

The increasingly severe antibiotic pollution has become one of the most critical issues. In this study, a zinc peroxide/peroxymonosulfate (ZnO2/PMS) double-oxidation system was developed for tetracycline (TC) degradation. A small amount of ZnO2 (10 mg) and PMS (30 mg) could effectively degrade 82.8% of TC (100 mL, 50 mg/L), and the degradation process could be well described by the pseudo-second-order kinetic model. Meanwhile, the ZnO2/PMS double-oxidation system showed high adaptability in terms of reaction temperature (2–40 °C), initial pH value (4–12), common inorganic anions (Cl−, NO3−, SO42− and HCO3−), natural water source and organic pollutant type. The quenching experiment and electron paramagnetic resonance (EPR) characterization results confirmed that the main reactive oxygen species (ROS) was singlet oxygen (1O2). Moreover, three possible pathways of TC degradation were deduced according to the analyses of intermediates. On the basis of comparative characterization and experiment results, a synergistic activation mechanism was further proposed for the ZnO2/PMS double-oxidation system, accounting for the superior degradation performance. The released OH− and H2O2 from ZnO2 could activate PMS to produce major 1O2 and minor superoxide radicals (•O2−), respectively.

The mortality of ovarian cancer (OC) has long been the highest among gynecological malignancies. Although OC is considered to be an immunogenic tumor, the effect of immunotherapy is not satisfactory. The immunosuppressive microenvironment is one reason for this, and the absence of recognized effective antigens for vaccines is another. Chemotherapy, as one of the most commonly used treatment for OC, can produce chemotherapy-associated antigens (CAAs) during treatment and show the effect of in situ vaccine. Herein, we designed an antigen capture nano-vaccine NP-TP1@M-M with tumor targeting peptide TMTP1 and dendritic cell (DC) receptor mannose assembled on the surface and adjuvant monophosphoryl lipid A (MPLA) encapsulated in the core of poly (D, L-lactide-co-glycolide) (PLGA) nanoparticles. PLGA itself possessed the ability of antigen capture. TMTP1 was a tumor-homing peptide screened by our research team, which held extensive and excellent tumor targeting ability. After these modifications, NP-TP1@M-M could capture and enrich more tumor-specific antigens after chemotherapy, stimulate DC maturation, activate the adaptive immunity and combined with immune checkpoint blockade to maximize the release of the body’s immune potential, providing an eutherapeutic strategy for the treatment of OC.