The microenvironment regulation of Fe-N single atom catalysts (SACs) critically governs peroxymonosulfate (PMS) activation. Although conventional heteroatom substitution in primary coordination enhances activity, it disrupts Fe-N symmetry and compromises stability. Herein, we propose oxygen doping in the secondary coordination shell to construct Fe-N-CO SAC, which amplifies the localized electric field while preserving the pristine coordination symmetry, thus trading off its activity and stability. This approach suppresses Fe-N bond structural deformation (bond amplitude reduced from 0.875-3.175 Å to 0.925-2.975 Å) during PMS activation by lowering Fe center electron density to strengthen Fe-N bond, achieving extended catalytic durability (>240 h). Simultaneously, the weakened coordination field lowers the Fe=O σ* orbital energy, promoting electrophilic σ-attack of high-valent iron-oxo towards bisphenol A, and increasing its degradation rate by 41.6-fold. This work demonstrates secondary coordination engineering as a viable strategy to resolve the activity-stability trade-off in SAC design, offering promising perspectives for developing environmental catalysts.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1038/s41467-025-57643-7 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
A novel layered porous Fe, Cu dual-loading biochar heterogeneous catalyst to guided non-free radical pathway for peroxymonosulfate activation.
J Colloid Interface Sci
March 2025
Institute of Yellow River Delta Earth Surface Processes and Ecological Integrity, College of Safety and Environment Engineering, Shandong University of Science and Technology, Qingdao 266590, China; College of Geography and Environment, Shandong Normal University, Jinan 250358, China. Electronic address:
Engineering active sites on catalyst surface to enhance selective oxidation pathways in advanced oxidation processes (AOPs) is key to the efficient removal of pollutants. In this work, a method of loading bimetallic ions and simultaneously activating the surface of swine manure biochar using cetyltrimethylammonium bromide (CTAB) was developed. By applying SiO templating method to increase the surface area and pore size of the catalyst, this study prepared a copper-iron-loaded layered porous catalyst (CFBC-0.
View Article and Find Full Text PDFDual Defect-Engineered BiVO Nanosheets for Efficient Peroxymonosulfate Activation.
Nanomaterials (Basel)
February 2025
Shandong Provincial Key Laboratory of Molecular Engineering, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China.
Defects and heteroatom doping are two refined microstructural factors that significantly affect the performance of photocatalytic materials. Coupling defect and doping engineering is a powerful approach for designing efficient photocatalysts. In this research, we successfully construct dual defect-engineered BiVO nanosheets (BVO-N-OV) by introducing N doping and oxygen vacancies through ammonium oxalate-assisted thermal treatment of BiVO nanosheets.
View Article and Find Full Text PDFEffect of persulfate dosage on organic degradation using N-doped biochar: Reaction pathway and environmental implications.
Water Environ Res
March 2025
State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Beijing, P. R. China.
Persulfate-based advanced oxidation processes (PS-AOPs) catalyzed by carbon-based catalysts are promising for removing organic pollutants via radical/non-radical pathways. However, the activation efficiency of peroxymonosulfate (PMS) or peroxydisulfate (PDS) usage and the reaction mechanism remain insufficiently understood. In this study, the effects of PMS/PDS dosage on the degradation of bisphenol A (BPA, 10 mg/L) were evaluated using N-doped biochar (N-BC, 0.
View Article and Find Full Text PDFSurface-hydroxylated single-atom catalyst with an isolated Co-O-Zn configuration achieves high selectivity in regulating active species.
Nat Commun
March 2025
Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing, China.
Single-atom catalysts (SACs) are emerging as potent tools for the selective regulation of active species, offering substantial promise for green and sustainable Fenton catalysis. However, current SACs face limitations due to the specificity of their supports, which only allow selective regulation within certain oxidant systems. This constraint makes targeted regulation across different systems challenging.
View Article and Find Full Text PDFUnveiling the synergistic mechanism of Fe-Cu bimetallic catalysts for degradation of tetracycline antibiotic with ultralow peroxymonosulfate dosage consumption: Key contribution of electron transfer process.
J Colloid Interface Sci
March 2025
School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China. Electronic address:
Developing low-oxidant, high efficiency catalysts is critical to meet the green-circular goal in water treatments. Heteroatom-doped graphite-based carbon nitride carrier catalysts are among the most promising candidate materials in water purification catalysis. In this research, a bimetallic catalyst (Fe-Cu@SNC), featuring dual reaction centers, was prepared using a mass-producible co-precipitation method.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!