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Updated: May 22, 2026

Expression and Purification of Nuclease-Free Oxygen Scavenger Protocatechuate 3,4-Dioxygenase
Published on: November 8, 2019
Cage-confined dinuclear Fe2-N6 electron shuttles for nonradical peroxydisulfate activation toward water
Yuyan Wang1, Xiang Zhou1, Manqi Liang1
1College of Chemistry and Environmental Engineering, Shenzhen University, 1066 Xueyuan Boulevard, Shenzhen 518052, China.
Abstract:
Peroxydisulfate (PDS)-based advanced oxidation is promising for water decontamination, yet its efficiency is often constrained by inefficient PDS utilization and sluggish interfacial electron transfer on conventional Fe-N-C catalysts. Herein, we aim at enhancement in efficient nonradical PDS activation by building cage-confined dinuclear Fe2-N6 motifs on ZIF-8-derived N-doped porous carbon (Fe2-N-C) via ship-in-a-bottle strategy. The structural analyses reveal predominantly paired Fe sites (∼72.4%) with a characteristic FeFe scattering contribution, confirming the dinuclear configuration. Compared with mononuclear and trinuclear analogues, Fe2-N-C/PDS system achieves ∼100% removal of 2,4,6-trichlorophenol within 30 min with a higher oxidant utilization efficiency (RSE ∼75%). It remains robust across pH 3-9 and shows favorable long-term operational stability. The modeling calculation through density functional theory further indicates optimized PDS adsorption and enhanced electron donation to PDS on Fe2-N6, rationalizing facilitated OO activation. The mechanistic experiments show weak inhibition by radical scavengers but complete suppression by thiocyanate site blocking, while the electron paramagnetic resonance spectroscopy identifies prominent 1O2 accompanied by minor •O2-/•OH signals, supporting a surface-mediated, nonradical-dominated pathway enabled by fast electron shuttling. This study provides a practical route and mechanistic basis for designing confined dinuclear metal sites to intensify selective PDS-driven water decontamination.
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