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Nitrogen-doped CNTs enhance heterogeneous Fenton reaction for IOH removal by FeOCl: Role of NCNTs and mechanism

催化作用 化学 降级(电信) 分解 酰胺 电子顺磁共振 电子转移 水解 化学工程 无机化学 光化学 有机化学 电信 物理 计算机科学 工程类 核磁共振
作者
Dunyu Sun,Bingyu Shen,Shaogui Yang,Xinying Cheng,Qiang Zhong,Syed Azhar Abbas,Yinhao Dai,Yazi Liu,Chenmin Xu,Chengdu Qi,Huan He,Shiyin Li
出处
期刊:Separation and Purification Technology [Elsevier]
卷期号:326: 124763-124763 被引量:15
标识
DOI:10.1016/j.seppur.2023.124763
摘要

• N-doped CNTs loaded nano-FeOCl was synthesized by partial thermal decomposition . • NCNT loading significantly improves the degradation efficiency of IOH . • NCNTs facilitate Fe(III)/Fe(II) circulation by accelerating electron transfer . • The confinement structure enhances the availability of ROS . Heterogeneous Fenton has already been used extensively to remove emerging contaminants, however, sluggish Fe(III)/Fe(II) circulation and high mass-transport resistance are its two major limitations. In this study, a novel heterogeneous N-doped carbon nanotubes loaded nano-FeOCl (NCF) catalyst was synthesized by partial thermal decomposition to enhance its catalytic performance. By incorporating NCNTs, the specific surface area of NCF was significantly increased in comparison to FeOCl, which promotes the accumulation of contaminants on the catalyst surface. Similarly, the degradation rate constant ( k ) of IOH in the NCF/H 2 O 2 system was observed 114 times greater than that of the FeOCl/H 2 O 2 system. Besides not significantly increased k , excessive H 2 O 2 substantially reduced H 2 O 2 utilization. Electron paramagnetic resonance and electrochemical analysis reflected that the NCNTs facilitated the Fe(III)/Fe(II) circulation by improving electron transfer and enhanced •OH, O 2 •− and 1 O 2 availability by exerting a confinement effect. The major reactions assumed in IOH degradation include hydrogen atom abstract, amide hydrolysis, deiodination reaction, •OH radical adduct formation, and oxidation of C-OH. This study elucidates the degradation mechanism of IOH in the heterogeneous Fenton system with carbon-based co-catalysts and provides an efficient measure for removing emerging contaminants from the environment.
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