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Switching Reactive Oxygen Species Reactions Derived from Mn–Pt Anchored Zeolite for Selective Catalytic Ozonation

Environmental Pollution(2024)

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摘要
Rationally switching reactive oxygen species (ROS) reactions in advanced oxidation processes (AOPs) is urgently needed to improve the adaptability and efficiency for the engineering application. Herein we synthesized bimetallic Mn-Pt catalysts based on zeolite to realize the switching of ROS reactions in catalytic ozonation for sustainable degradation of organic pollutants from water. The ROS reactions switched from singlet oxygen (1O2, 71.01%) to radical-dominated (93.79%) pathway by simply introducing defects and changing Pt/Mn ratios. The oxygen vacancy induced by anchoring Mn-Pt species from zeolite external surface (MnPt/H-Beta) to internal framework (MnPt@Si-Beta) exposes more electron-rich Pt2+/Pt4+ redox sites, accelerating the decomposition of O3 to generate •OH via electron transfer and switching ROS reactions. The Mn site acted as a bridge plays a critical role in conducting electrons from organic pollutants to Pt sites, which solidly solves the electron loss of catalysts, facilitating the efficient degradation of pollutants. A 34.7-fold increase in phenol degradation compared with the non-catalytic ozonation and an excellent catalytic stability are achieved by MnPt@Si-Beta/O3. The 1O2-dominated ROS reaction originated from MnPt/H-Beta/O3 exhibits superior performances in anti-interference for Cl-, HCO3-, NO3-, and SO4-. This work establishes a novel strategy for switching ROS reactions to expand the targeted applications of O3 based AOPs for environmental remediation.
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关键词
Switching reaction,Reactive oxygen species,Zeolite,Bimetal Mn-Pt,Catalytic ozonation
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