Latest ArticlesThe simultaneous removal of antibiotics and heavy metals from wastewater remains a complex and challenging task. A stable α-Fe2O3/Cd0.9Zn0.1S catalyst with rod structure is constructed for simultaneous oxidation of ciprofloxacin and reduction of Cr(Ⅵ) via the in situ growth of α-Fe2O3 nanodots on Cd0.9Zn0.1S nanorod using lattice matching. The unique in situ growth pattern not only strengthens light absorption but also improves electron transfer capacity. The formed iron-sulfur (Fe-S) bonds improved the poor contact at the heterojunction interface, effectively promoted charge separation, and successfully suppressed photocorrosion. Consequently, the S-scheme heterojunction with the synergistic effect of rod structure and chemical bonds significantly enhances photocatalytic performance. Under the coexisting pollutant system, photocatalytic reaction rate constants of α-Fe2O3/Cd0.9Zn0.1S under optimal composite ratio conditions were 1.5-times (ciprofloxacin) and 5.1-times (Cr(Ⅵ)) higher than Cd0.9Zn0.1S. Benefiting from the dual action of active free radicals and the internal electric field stimulating electron transfer and utilization, the photocatalytic membrane technology has demonstrated the possibility of practical wastewater in a photocatalytic system.
Herein, a novel type of flexible network hydrogel was formed by cross-linking of chitosan (CS) and acrylamide (AM) monomer through non-covalent bond, and was named CS/PAM/hydrogel (CPH). Subsequent functional modification of the CPH was then undertaken through the implementation of in-situ green growth technology, and the cobalt organic framework (ZIF-67) was successfully grown on the hydrogel. Ultimately, the composite hydrogel CS/PAM/ZIF-67/hydrogel (CPZH) was prepared. Subsequently, an electrochemical sensor was developed by combining a composite hydrogel with a glassy carbon electrode, and it was demonstrated that this combination exhibited excellent performance, especially in the electrochemical detection of the target molecule 2,4.6-trichlorophenol. Excellent linear ranges (0.01–10 and 10–1000 μmol/L) and low detection limit (0.003 μmol/L) were achieved. The excellent electrochemical performance can be attributed to (ⅰ) 3D network structure of the hydrogel provides an effective mass transfer channel for the electrochemical reactants; (ⅱ) The MOF layer provides a wealth of catalytic active sites, resulting in electrochemical signal amplification of the CPZH composite, (ⅲ) The growth of ZIF-67 in the original location of the hydrogel network successfully solved the problem that traditional ZIF-67 particles are prone to agglomeration and exhibit weak bonding force with the substrate, which significantly improved the stability and electrochemical performance.
Recently, iron-based heterogenous catalysts have attracted widespread attention in the activation of peracetic acid (PAA) for generating reactive oxygen species (ROS) to degrade pollutants. However, in heterogeneous PAA activation systems, the role of coexisting H2O2 in PAA is often overlooked. To clarify the dynamic roles of both PAA and H2O2, herein, iron boride (FeB) was employed as a heterogeneous activator of PAA for carbamazepine (CBZ) degradation. The generation of high valent iron (Fe(Ⅳ)), hydroxyl radicals (•OH) and organic radicals (RO•) in the FeB/PAA system were identified through quenching experiments, electron paramagnetic resonance (EPR) spectroscopy, and semi-quantitative analysis. At the initial stage of the reaction, the active sites of FeB preferentially reacted with PAA, rather than H2O2, primarily generating Fe(Ⅳ) to oxidize CBZ. Subsequently, PAA was gradually depleted, dissolved Fe(Ⅱ) slowly released from FeB reacts with H2O2 in the solution to generate •OH. Besides, density functional theory (DFT) calculations and masking experiments revealed that the surface Fe(Ⅱ) (≡Fe(Ⅱ)) acts as the dominant active center for PAA activation. Moreover, the selective oxidation of various pollutants by these ROS is governed by the differing sensitivities of the contaminants to ROS. The electron-donating B–B bonds in FeB can effectively promote the Fe(Ⅲ)/Fe(Ⅱ) redox cycling, exhibiting exceptional catalytic performance. Additionally, the possible degradation pathways of CBZ were proposed by combining ultra-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry (UPLC-QTOF-MS/MS) and DFT calculations. This work provides new insights into the activation mechanism of PAA by FeB, offering a sustainable and efficient approach for the treatment of emerging pollutants.
Carbon-chain rubbers have been widely used in many fields including transportation, medicine, construction, and everyday life, owing to their excellent flexibility. Now, waste rubbers have caused serious environmental pollution and resource waste. Chemical recovery is expected to provide a solution to solve these problems fundamentally. Here, the recent progress in selective chain scissions of the waste sulfur-vulcanized carbon-chain rubbers for reuse was reviewed. Based on the different devulcanization approaches, the polysulfide crosslinking chains or carbon chains were broken and the linear or branched degraded products could be obtained as structural prepolymers for new rubber products. After a comprehensive literature review on the effect of the molecular composition and topology of the devulcanized and degraded products on the new rubbers, the future perspectives were proposed.
Metal-organic frameworks (MOFs) and their derivatives have emerged as promising platforms for constructing heterojunctions in photocatalytic CO2 reduction (PCR). This review systematically summarizes the latest research progress in MOFs and their derivative heterostructures for PCR, focusing on material design, underlying mechanisms, and diverse applications. Besides, this review, by introducing various synthesis methods, emphasizes the significance of controllable synthesis strategies. Furthermore, the in-situ characterization techniques and theoretical calculations in photocatalysis are introduced and summarized, including the study of the morphology and chemical structure of photocatalysts, the transfer of photogenerated charges, spatial distribution, and surface reaction pathways. Systematic reviews of the advantages and disadvantages, features, and applications of various types of MOFs and their derivative heterostructures are conducted in accordance with the band arrangement characteristics. In addition, the discussion scope is expanded to related catalytic systems, including electrocatalysis, photoelectrocatalysis, and photothermal catalysis, fully demonstrating the multifunctionality of MOFs and their derivative heterostructures. Finally, future research directions are proposed from aspects such as material design and synthesis, performance optimization and mechanism research, correlation with practical applications, as well as the interdisciplinary collaboration. We hope it can provide valuable references for the rational design of high-performance MOFs and their derivative heterostructures materials with the wide range of applications.
Emerging pollutants—including PFAS, microplastics, antibiotics, and endocrine-disrupting chemicals (EDCs)—pose escalating ecological and health risks while embodying untapped elemental value. Traditional remediation strategies focus on destruction, often overlooking opportunities for resource recovery. In contrast, catalytic upcycling leverages advances in photocatalysis, electrocatalysis, mechanochemistry, and hybrid bio-abiotic systems to selectively convert pollutants into value-added products, aligning with circular economy goals. This review synthesizes overarching catalytic principles—such as C–F and C–C bond activation, ROS selectivity, and redox synergies—that are applicable across pollutant classes. We also contrast pollutant-specific challenges: the chemical inertness of PFAS, the heterogeneity of microplastics, the toxicity and complexity of antibiotic intermediates, and the trace-level persistence of EDCs. Despite these differences, recent breakthroughs demonstrate promising upcycling pathways: PFAS into fluorochemicals, microplastics into olefins and graphitic materials, antibiotics into hydrogen and organic acids, and EDCs into polymeric and pharmaceutical precursors. We further highlight emerging techno-economic and life-cycle assessments, showing that upcycling can reduce CO2 emissions by up to 80% and generate substantial economic returns. By reframing pollutants as chemical feedstocks, this review outlines a transformative strategy for pollution control, resource recovery, and sustainable chemical production.
Precise assessment of tacrolimus (TAC) concentrations is critical in clinical diagnostics, and liquid chromatography–mass spectrometry (LC-MS/MS) is the preferred approach due to its high specificity and sensitivity. However, classic LC-MS/MS systems are frequently enormous, costly, and need expert operation, which restricts its applicability in numerous industries. In this paper, a liquid chromatography–miniature mass spectrometry (LC-MiniMS) system was designed and developed. The miniature linear ion trap spectrometer had a footprint of 59 × 38 × 27 cm3, which substantially reduced the instrument size and cost while maintaining quantitative performance. The LC-MiniMS system's circuit boards were integrated and the software automation was optimized, so it was more convenient to use and maintain. Results demonstrated excellent linearity over the range of 0.5–50 ng/mL with R2 > 0.99. The limit of detection and limit of quantification were 0.1 and 0.3 ng/mL, respectively. The accuracy ranged from 99.67% to 106.10%, intraday precision was between 0.70% and 2.61%, and interday precision was between 0.90% and 2.90%, all within acceptable limits, and matrix effects were negligible. The method was successfully applied to quantify TAC in 32 clinical whole-blood samples, and the results strongly agreed with those from a conventional LC-MS/MS system (QTRAP 6500+). The LC-MiniMS system can efficiently quantify TAC in whole blood and provide a tiny, cost-effective, and uncomplicated option for therapeutic drug monitoring in clinical settings, especially in decentralized or resource-limited scenarios.
Ultralong organic phosphorescence (UOP) materials have attracted increasing attention due to its potential applications in opto-electronics, bioelectronics, and security protection. However, it is still a formidable challenge to develop a material with simultaneous efficiency and lifetime enhancement under ambient conditions. Here, highly efficient UOP is achieved by doping crown ether derivatives into rigid poly(vinyl alcohol) (PVA) matrix. Two crown ether derivatives exhibited weak yellow UOP. Impressively, after doped into PVA films, the resultant PVA films demonstrated bright blue UOP with a long lifetime of 595.9 ms and high phosphorescence efficiency of 13.3%. The sharp enhancement of efficiency and lifetime can be ascribed to abundant hydrogen bonding between the crown ether derivatives and PVA polymer chains. This work provides a new avenue for developing highly efficient UOP materials.
Oxygen vacancy engineering in heterogeneous catalysts has attracted considerable interest for peroxymonosulfate (PMS) activation. In this study, nano-Co3O4-encapsulated montmorillonite catalysts with tunable oxygen vacancy (OV) concentrations (denoted as Co3O4−Mt-xOV, x = 2, 4, 6) were synthesized for enhanced PMS activation. These OV defects not only modulate the electronic structure of Co3O4 but also strengthen PMS and contaminant adsorption. The optimized Co3O4−Mt-xOV/PMS system exhibited exceptional ofloxacin (OFL) degradation efficiency, achieving 2.74–3.43-fold enhancement over OV-free Co3O4−Mt. Density functional theory calculations and experimental studies revealed that the performance improvement stemmed from OV formation, which synergistically enhanced redox pair cycling, strengthened PMS adsorption, and promoted active species generation during electron transfer. Further studies demonstrated that OV sites selectively drive PMS decomposition to generate high-valent cobalt-oxo species (Co(Ⅳ)=O) and singlet oxygen (1O2) as the dominant reactive species for OFL oxidation. The in-depth investigation into the catalytic mechanism revealed that the Co(Ⅳ)=O species facilitated O2•− generation in surpassing the reaction energy barrier, which subsequently converted to 1O2. This non-radical pathway endowed the system with robust anti-interference capability against complex water matrices. The critical role of OV in PMS activation was mechanistically confirmed through experimental and theoretical analyses. Furthermore, Co3O4−Mt-4OV demonstrated outstanding chemical stability and recyclability, highlighting its practical potential. This work provides fundamental insights into vacancy defect engineering for advanced PMS activation and offers strategic guidance for designing high-performance catalysts.