Efficient degradation of micropollutants in CoCaAl-LDO/peracetic acid (PAA) system: An organic radical dominant degradation process

过氧乙酸 降级(电信) 化学 激进的 高级氧化法 环境化学 化学工程 核化学 有机化学 过氧化氢 电信 计算机科学 催化作用 工程类
作者
Zhihui Xie,Chuan-Shu He,Dan-Ni Pei,Yunzhe Zheng,Xiaoyu Wu,Zhaokun Xiong,Ye Du,Zhicheng Pan,Gang Yao,Bo Lai
出处
期刊:Journal of Hazardous Materials [Elsevier BV]
卷期号:452: 131286-131286 被引量:51
标识
DOI:10.1016/j.jhazmat.2023.131286
摘要

As a novel strategy, peracetic acid (PAA) based advanced oxidation processes (AOPs) are being used in micropollutant elimination due to their high oxidation and low toxicity. In this study, Co2Ca1Al1-LDO as a kind of layered double oxides (LDOs) was successfully synthesized, and it is the first time to apply Co2Ca1Al1-LDO for activating PAA. The Co2Ca1Al1-LDO/PAA system showed excellent removal efficiencies for various micropollutants with removal ratios ranging from 90.4% to 100% and k values from 0.087 min-1 to 0.298 min-1. In the degradation period, various reactive oxygen species (ROS) are involved in the system, while organic radicals (R-O•) with a high concentration of 5.52 × 10-13 M are the dominant ROS in the contaminants degradation process. Compared to other ROS, R-O• had the largest contribution ratio (more than 85%) to pollutant degradation. Further analysis demonstrated that C1, C2, C3, C4, C5, C6 and N11 concentrated on the aniline group of SMX are the main attack sites based on the density functional theory (DFT) results, which is consistent with the degradation products. The toxicity of contaminants was obviously reduced after removing in this system. Furthermore, Co2Ca1Al1-LDO showed good reusability and stability, and Co2Ca1Al1-LDO/PAA system had excellent removal ability in actual water bodies containing inorganic anions, showing good application potential. Importantly, this study explored the feasibility of applying LDO catalysts in PAA-based AOPs for micropollutants elimination, providing new insights for subsequent research.
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