化学
催化作用
碳酸氢盐
光化学
普鲁士蓝
X射线光电子能谱
密度泛函理论
傅里叶变换红外光谱
电子转移
羟基自由基
反应机理
无机化学
激进的
电化学
计算化学
物理化学
化学工程
有机化学
工程类
电极
作者
Yiqiong Yang,Xingyu Li,Borui Jie,Zenghui Zheng,Jiding Li,Ce Zhu,Shubin Wang,Jingcheng Xu,Xiaodong Zhang
标识
DOI:10.1016/j.jhazmat.2022.129372
摘要
Although several strategies have been developed to improve the efficiency of heterogeneous Fenton-like reactions, investigating the relationship among the electronic properties of the catalyst surface, the complex water matrix and catalytic activity remains challenges. Herein, the electron density of the active site Co(II) in Co Prussian blue analogs (Co-PBAs) is proved to be modulated by the anion source method. The elevated electron density of Co(II) and the higher metallicity of the catalyst lead to an increase in electron transport efficiency as revealed by X-ray photoelectron spectra (XPS), Fourier transform infrared spectroscopy (FT-IR), and density functional theory (DFT) calculations. Furthermore, the negative shift of the D-band center of Co(II) can effectively release intermediates to avoid catalyst poisoning. Bicarbonate has been demonstrated to activate peroxymonosulfate (PMS) by weakening the peroxide bond. Its activation mechanism involves free radical mechanism and non-radical mechanism: the first step is the generation of HCO4-, then it is further hydrolyzed to generate •OH and 1O2, and the other is HCO4- interact with Co(III) to form Co(IV)=O. In addition, the degradation pathways of target contaminants p-nitrophenol and toxicity verification of intermediate products have been investigated. This study provides guidance for the research of Fenton-like reactions.
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