Latest ArticlesEmerging contaminants (ECs) present significant environmental and health risks due to their widespread impact. Catalytic Fenton-like reactions using carbon-based catalysts offer a promising and sustainable solution for EC removal. This review synthesizes recent advancements in heteroatom-doped carbon (HDC) catalysts for peroxymonosulfate (PMS) activation, critically evaluating the merits and limitations of HDC-mediated Fenton-like reactions. The review explores how doping affects catalyst porosity, electronic properties, PMS activation efficiency, and overall effectiveness in EC removal. Innovative strategies for identifying key reactive species in HDC/PMS systems are discussed, including the use of chemical probes, spin-trapping agents, and SETP-based methodologies. Additionally, density functional theory (DFT) is utilized to investigate the electronic structures of ECs and their interactions with reactive oxygen species (ROS). The practical potential of HDCs in remediating contaminated groundwater and wastewater is also addressed, alongside a discussion of the challenges and future research directions to enhance their scalable applications, offering a roadmap for advancing sustainable environmental remediation technologies.
The worldwide utilization of antibiotics and the generation of antibiotic-resistant bacteria necessitate the development of alternative wastewater treatment strategies, in which the cycling of metallic ions and the precise modulation of Fe active sites remain critically important factors to be concerned. In this work, Mo incorporation is strategically employed to modulate Fe-O covalency through charge redistribution driven by strong Fe-Mo interactions over graphite carbon ring/CN (CCN). This design achieves an exceptional degradation rate constant, which arises from synergistic Fe/Mo catalytic-co-catalytic interactions that facilitate sustainable metal redox cycling, enhance bonding orbital overlap, and optimize surface adsorption characteristics. The Mo-modified catalyst (FeMoCCN) exhibits a greater contribution to bonding orbitals compared to the singly Fe-doped counterpart (FeCCN). The introduction of Mo enhances Fe-O covalency, thereby facilitating electron transfer for peroxymonosulfate (PMS) activation and subsequent degradation processes. Remarkably, complete electron transfer is achieved through the Fe2+/Fe3+, Mo6+/Mo4+, Fe3+/Mo4+ redox couples, further implying the robust adaptability of this Fenton-like system for antibiotic degradation while providing mechanistic insights into the synergistic effects between light irradiation, oxidant activation, and bimetallic doping modulation in advanced wastewater treatment.
Triclosan (TCS) is an emerging environmental pollutant that has been widely used in personal care products and is frequently detected in the human body. As a marker on DNA and RNA, nucleic acid modifications are crucial for the versatile regulation of gene expression. However, the epigenetic mechanisms underlying TCS-induced adverse effects remain largely unclear. In this study, we systematically investigate the impact of TCS on DNA and small RNA modifications from C57BL/6 N mice at doses of 0, 50, and 200 mg kg−1 d−1, using liquid chromatography-tandem mass spectrometry (LC-MS/MS). We quantitatively quantified 23 nucleic acid modifications in seven tissues, including heart, liver, kidneys, lungs, brain, intestine, and testis. The results indicated that TCS exposure significantly suppressed body weight gain and altered organ coefficients in a dose-dependent manner. Multiple DNA and RNA modifications exhibit significant changes by TCS exposure across different tissues and display tissue-specific patterns. Notably, TCS exposure led to liver inflammation and lipid accumulation, accompanied by decreased levels of RNA N6-methyladenine (m6A) and elevated expression of fat mass and obesity-associated gene (FTO) in both mouse liver and HepG2 cells, suggesting its involvement in TCS-mediated epigenetic imbalance and hepatotoxicity. Our study provides the first comprehensive epigenetic evaluation of TCS-induced nucleic acid modification alterations across multiple organs in mammals, providing a new perspective for understanding the toxicological mechanisms of TCS from an epigenetic perspective.
Climate change and global warming constitute formidable global challenges, predominantly driven by the excessive dependence on conventional fossil fuels, which results in substantial carbon dioxide (CO2) emissions. Addressing these environmental issues is a paramount priority for researchers. Single-atom catalysts (SACs) have attracted significant attention due to their high atomic efficiency and unique performance in various catalytic reactions. As an emerging two-dimensional (2D) carbon material, graphdiyne (GDY) has gained favor in environmental remediation applications in recent years. GDY comprises sp- and sp2-hybridized carbon atoms, which form benzene rings and diacetylenic linkages (–C≡C–C≡C–) within a two-dimensional planar network, endowing it with high π-conjugation, distinctive and tunable electronic properties, and excellent chemical and thermal stability. In this review, we investigate the environmental catalytic reactions and applications of GDY-based SACs. We provide a detailed account of the current methodologies for synthesizing GDY and examine the catalytic applications of GDY-based SACs in CO2 reduction reactions. Specifically, we systematically categorize the photocatalytic and electrocatalytic CO2 reduction processes using metal-doped GDY and metal-free doped GDY. Finally, we discuss the challenges and future developments of GDY within the context of SACs.
Micro/nano plastics as an emerging contaminant have attracted the attention of researchers worldwide. However, a variety of detection methods have been derived based on the properties of micro/nano plastics, such as micro-infrared spectroscopy, micro-Raman spectroscopy, gas chromatography-mass spectrometry, liquid chromatograph-mass spectrometry, optical-photothermal infrared. Compared with spectroscopy and mass spectrometry detection methods, many new detection methods have emerged with the advantages of low cost, high speed, and high sensitivity. But the detection process often only reflects part of the properties of micro/nano plastics, which limits our comprehensive understanding of the environmental behaviors of micro/nano plastics such as carrying contamination and interfacial properties. In this review, we critically summarize the existing literature on traditional and rapid detection methods, focusing on their current research status, applicability conditions, detection limits, and mechanisms. We emphasize that weathering behavior, migration behavior, deposition, adhesion, and adsorption of micro/nano plastics in the environment will change the physicochemical properties of micro/nano plastics, which will have an impact on current rapid detection and analysis methods. Rapid detection and analysis methods require consideration of the interfacial evolution behavior of micro/nano plastics in the environment to enhance the universality of their application. In addition, rapid detection methods are complementary to traditional standardized detection methods. After understanding the types of micro/nano plastics, we are more concerned about the quantity, dispersion behavior, carrying contamination, and interfacial properties in the environment. These properties are crucial for the environmental assessment and prevention of micro/nano plastics. It is recommended that further comprehensive research be conducted based on the optical and interfacial properties of micro/nano plastics, combined with machine learning and computer modeling, to provide a reliable basis for micro/nano plastic research.
The determination and quantification of sugars are important for quality control and assurance of food. Here we present a gas-free electrodialytic eluent generation (EG) platform for sugar analysis by anion exchange chromatography equipped with pulsed amperometric detector. It consists of a gas-free EG for automatic production of highly pure KOH eluent with wide concentration range up to at least 210 mmol/L required for ionization and elution of sugars. The only routine reagent needed is deionized water, driven by a simple isocratic pump to realize isocratic or gradient elution. This platform overcomes many drawbacks associated with common manner of manually prepared KOH eluent driven by gradient pump, and offers an easy way for sugar profiling with improved precision and accuracy. The method was successfully applied to quantification of sugars in biscuits.
Metal-support active interfaces provide unique sites that enhance catalytic oxidation reactions. However, designing a catalyst that simultaneously promote both benzene ring cleavage and C−H bond scission remains a challenge. Herein, porous SiO2 derived from waste rice husk was used to disperse CeO2 nanoparticles, onto which Pt nanoparticles were deposited via ethylene glycol reflux reduction combined with steam redispersion to prepare a Pt/CeO2/SiO2 catalyst with abundant Pt−O−Ce active interfaces. Characterization and experimental results show that well-dispersed CeO2 and Pt nanoparticles increase oxygen vacancy concentration and Pt–O–Ce interfaces, thereby enhancing oxygen spillover from CeO2 to Pt and promoting styrene oxidation. The Pt–O–Ce interface accelerates the rate-determining C−H bond cleavage in benzaldehyde during styrene oxidation. Pt/CeO2/SiO2-H2O catalyst with abundant oxygen vacancies and Pt–O–Ce interfaces achieves excellent catalytic performance (T90 = 222 ℃, WHSV = 120,000 mL h−1 g−1). Moreover, it demonstrates superior thermal stability over 40 h and water-resistance against 10 vol% H2O, highlighting its industrial potential. This study offers a strategy for constructing supported catalysts with tailored active interfaces and high stability.
Protein fatty acylation encompasses S/N/O-acylation modifications that regulate diverse cellular functions, yet current methods cannot simultaneously capture all three types. Here, we present a dual-identification strategy that integrates metabolic labeling with click chemistry, hydroxylamine mediated selective hydrolysis, and cleavable bioorthogonal probes for comprehensive fatty acylation site detection. Using Alk-C16:0 and Alk-C18:0 probes in HepG2 cells, we identified 1310 and 1131 total fatty acylation sites respectively, including 588 and 674 S-acylation sites substantially exceeding single method coverage. Integration of open and closed searches revealed probe intracellular conversion induced acyl chain heterogeneity, improving identification accuracy. We discovered diagnostic ions revealing acyl chain structure and N-acylation specific cyclic immonium ions that discriminate between modification subtypes. This strategy enables unprecedented comprehensive protein fatty acylation characterization, providing a robust platform for investigating molecular mechanisms of these essential modifications.
Pyranocoumarins are a characteristic class of pyranophenolic compounds predominantly found in plants of the Moraceae, Umbelliferae, and Rutaceae families. These pyranophenolics not only exhibit diverse physiological activities, but also have a wide range of pharmacological activities such as anti-cancer, anti-spasmatic, and anticoagulant. However, the biosynthetic mechanism of pyranocoumarins, especially the formation mechanism of the pyran core in the final step, remains unclear. It was hypothesized the pyran core is formed by dehydration of decursinol after oxidation and cyclization of demethylsuberosin. Here we characterized a berberine bridge enzyme (BBE)-like enzyme namely FcBBElike4 from Ficus carica. FcBBElike4 could catalyze direct cyclization of 6- and 8-isoprenyl coumarins into corresponding pyranocoumarins, which functionally characterized as an oxidocyclase (OC). This finding elucidated the final step in the biosynthetic pathway for pyranocoumarins. The catalytic mechanism of FcBBElike4 was investigated and a general key active site of aspartic acid residue determining the cyclization activity of BBE-like enzymes was identified. Diverse BBE-like enzymes with diene synthesis activities were mined and further engineered into rare OCs with high catalytic activity and broad substrate spectra. What is more, an enzymatic approach to synthesize pyranophenolics was constructed based on engineered OCs and applied in the synthesis of drug molecules. This study not only elucidates the key biosynthetic steps of pyranocoumarins but also offers insights into engineering common BBE-like enzymes into rare and useful OCs.
Extracellular vesicles (EVs) released by cells are widely present in body fluids and serve as mediators of cell communication and markers in disease diagnosis. However, it remains challenging to separate high-purity and structurally intact EVs from complex biological samples. Recently, microfluidics has shown excellent performance in the separation and analysis of EVs due to its precise control and integration capabilities. Microfluidic methods hold promise for clinical diagnostics owing to their integrated and convenient properties. In this review, we first introduce microfluidic-based label-free and affinity-based strategies for EV separation. Next, the common EV analysis methods integrated with microfluidics are summarized, including fluorescence, electrochemistry, surface plasmon resonance (SPR), and surface-enhanced Raman spectroscopy (SERS). Then, some microfluidics-based systems (valves, traps, and droplets) for single-cell EV analysis are concluded. Finally, we present the challenges and trends of microfluidics in EV research.
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