Abstract
The polymerization pathway of contaminants rivals the traditional mineralization pathway in water purification technologies. However, designing suitable oxidative environments to steer contaminants toward polymerization remains challenging. This study introduces a nitrogen‐oxygen double coordination strategy to create an asymmetrical microenvironment for Co atoms on Ti3C2Tx MXenes, resulting in a novel Co‐N2O3 microcellular structure that efficiently activates peroxymonosulfate. This unique activation capability led to the complete removal of various phenolic pollutants within 3 min, outperforming the representative Co single‐atom catalysts reported in the past three years. Identifying and recognizing reactive oxygen species highlight the crucial role of ·O2−. The efficient pollutant removal occurs through a ·O2−‐mediated radical pathway, functioning as a self‐coupling reaction rather than deep oxidation. Theoretical calculations demonstrate that the electron‐rich pollutants transfer more electrons to the catalyst surface, inducing the reduction of dissolved oxygen to ·O2− in the Co‐N2O3 microregion. In a practical continuous flow‐through application, the system achieved 100% acetaminophen removal efficiency in 6.5 h, with a hydraulic retention time of just 0.98 s. This study provides new insights into the previously underappreciated role of ·O2− in pollutant purification, offering a simple strategy for advancing aggregation removal technology in the field of wastewater treatment.
Published Version
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