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 (Co-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-N-C active sites through a catalytic pathway (PMS→PMS∗→OH∗→O∗→OO∗→O) exhibits selective oxidation of phenols and sulfonamides, achieving >90% removal rates. Our findings elucidate a multi-layered functional architecture within the Co-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 Co-NCNT-CM/PMS systems in advanced wastewater treatment frameworks, specifically for targeted EOCs removal, heralding a new direction for sustainable water management.
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http://dx.doi.org/10.1016/j.ese.2024.100416 | DOI Listing |
Adv Sci (Weinh)
January 2025
State Key Laboratory for Chemo/Biosensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education and College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, P. R. China.
The cobalt-nitrogen-carbon (Co─N─C) single-atom catalysts (SACs) are promising alternatives to precious metals for catalyzing the hydrogen evolution reaction (HER) and their activity is highly dependent on the coordination environments of the metal centers. Herein, a NaHCO etching strategy is developed to introduce abundant in-plane pores within the carbon substrates that further enable the construction of low-coordinated and asymmetric Co─N sites with nearby vacancy defects in a Co─N─C catalyst. This catalyst exhibits a high HER activity with an overpotential (η) of merely 78 mV to deliver a current density of 10 mA cm, a Tafel slope of 45.
View Article and Find Full Text PDFEcotoxicol Environ Saf
January 2025
School of Eco-Environment, Hebei Key Laboratory of Close-to-Nature Restoration Technology of Wetlands, Hebei University, Baoding 071002, China. Electronic address:
Imidacloprid (IMI), as an emerging pollutant, is frequently detected in pesticide wastewater. Cobalt-based single-atom catalysts (Co-SACs) doped with sulfur atoms can serve as an efficient strategy to activate peroxymonosulfate (PMS) and degrade organic pollutants. The paper employed density functional theory and computational toxicology to deeply explore the mechanism and ecotoxicity of IMI when S atoms were introduced into Co-SACs for PMS activation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Westlake University, Chemistry, No.18 Shilongshan Road, 310024, Hangzhou, CHINA.
Efficient methods for synthesizing allenes from readily available starting materials pose a persistent challenge in organic chemistry. In this work, we present a novel two-stage protocol for allene synthesis involving the single-atom insertion into alkenes, facilitated by synergistic photoredox and cobalt catalysis. Diverging from conventional methods such as the Doering-LaFlamme reaction, this photochemical rearrangement approach operates efficiently under mild conditions in a radical-based manner.
View Article and Find Full Text PDFNat Commun
January 2025
CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
Single-atom catalysts (SACs) have been increasingly acknowledged for their performance in sustainable Fenton-like catalysis. However, SACs face a trade-off between activity and stability in peroxymonosulfate (PMS)-based systems. Herein, we design a nano-island encapsulated single cobalt atom (Co-ZnO) catalyst to enhance the activity and stability of PMS activation for contaminant degradation via an "island-sea" synergistic effect.
View Article and Find Full Text PDFMacromol Rapid Commun
December 2024
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214122, China.
Diatomic catalysts enhance photocatalytic CO reduction through synergistic effects. However, precisely regulating the distance between two catalytic centers to achieve synergistic catalysis poses significant challenges. In this study, a series of one-dimensional (1D) covalent organic frameworks (COFs) are designed with adjustable micropores to facilitate efficient CO photoreduction.
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