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层状 δ-MnO 中嵌入的钴激活过一硫酸盐降解邻苯二甲酸二甲酯:机制、降解途径和 DFT 计算。

Activation of peroxymonosulfate with cobalt embedded in layered δ-MnO for degradation of dimethyl phthalate: Mechanisms, degradation pathway, and DFT calculation.

机构信息

College of Resource and Environment, Qingdao Agricultural University, Qingdao 266109, China; Key Lab of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao 266100, China.

College of Resource and Environment, Qingdao Agricultural University, Qingdao 266109, China.

出版信息

J Hazard Mater. 2023 Jun 5;451:130901. doi: 10.1016/j.jhazmat.2023.130901. Epub 2023 Jan 31.

DOI:10.1016/j.jhazmat.2023.130901
PMID:36881985
Abstract

The sulfate radical-based advanced oxidation processes (SR-AOPs) offer huge potential for the removal of organic pollutants. In this study, Co(II)-intercalated δ-MnO (Co-δ-MnO) catalyst was successfully prepared by a simple cation exchange reaction. The obtained Co-δ-MnO exhibited high catalytic performance for the removal of dimethyl phthalate (DMP) under the activation of peroxymonosulfate (PMS), with the degradation efficiency reaching 100% within 6 h. Experiments and theoretical calculations revealed that interlayer Co(II) provided unique active sites in Co-δ-MnO. In addition, radical and non-radical pathways were confirmed to play a role in Co-δ-MnO/PMS system. OH, SO, and O were identified to be the dominating reactive species in Co-δ-MnO/PMS system. This study provided new insights into the design of catalysts and laid a foundation for developing modifiable layered heterogeneous catalysts.

摘要

基于硫酸根自由基的高级氧化工艺 (SR-AOPs) 为去除有机污染物提供了巨大的潜力。在本研究中,通过简单的阳离子交换反应成功制备了 Co(II)插层 δ-MnO (Co-δ-MnO) 催化剂。所得 Co-δ-MnO 在过一硫酸盐 (PMS) 的活化下,对二甲苯二甲酸二甲酯 (DMP) 的去除具有很高的催化性能,在 6 h 内降解效率达到 100%。实验和理论计算表明,层间 Co(II)在 Co-δ-MnO 中提供了独特的活性位。此外,确认了自由基和非自由基途径在 Co-δ-MnO/PMS 体系中发挥作用。在 Co-δ-MnO/PMS 体系中,OH、SO 和 O 被鉴定为主要的反应性物质。本研究为催化剂的设计提供了新的思路,并为开发可修饰的层状多相催化剂奠定了基础。

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