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高密度分散的 CuN 位点用于 HO 的活化,以增强抗生素污染物降解中的光芬顿性能。

High-density dispersion of CuN sites for HO activation toward enhanced Photo-Fenton performance in antibiotic contaminant degradation.

机构信息

School of Environmental Sciences and Engineering, Nanjing Tech University, Nanjing 211816, China.

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.

出版信息

J Hazard Mater. 2022 Feb 5;423(Pt A):127039. doi: 10.1016/j.jhazmat.2021.127039. Epub 2021 Aug 28.

Abstract

In this study, a copper-based catalyst (CuCN) with CuN active sites highly dispersed in a porous carbon nitride matrix was synthesized and applied to a heterogeneous photo-assisted Photo-Fenton (PF) system to degrade tetracycline (TET). The results showed that the CuCN/PF system degraded up to 93.6% of TET within 60 min for ultrapure water matrix under the best experimental conditions, and more than 70% of TET for both river and lake water matrix. Toxicological tests suggested that the environmental risk caused by TET can be effectively inhibited by the CuCN/PF system. The good visible-light response and charge transport abilities of CuCN catalyst were identified in photoelectrochemical experiments. Free radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy indicated that the active species in the degradation process were·OH, h,·O and O. Density functional theory (DFT) calculations revealed the positive effect of CuN sites in CuCN on the formation of hydroxyl radicals by activating HO. This work will provide a new insight for the development of high-efficiency heterogeneous catalysts in wastewater environmental remediation.

摘要

在这项研究中,合成了一种铜基催化剂(CuCN),其具有高度分散在多孔氮化碳基质中的 CuN 活性位,用于非均相光辅助光-Fenton(PF)系统来降解四环素(TET)。结果表明,在最佳实验条件下,CuCN/PF 体系在超纯水基质中 60 分钟内可将 TET 降解高达 93.6%,在河水和湖水基质中也可降解超过 70%。毒理学测试表明,CuCN/PF 体系可有效抑制 TET 引起的环境风险。光电化学实验表明,CuCN 催化剂具有良好的可见光响应和电荷传输能力。自由基清除实验和电子顺磁共振(EPR)光谱表明,降解过程中的活性物质是·OH、h、·O 和 O。密度泛函理论(DFT)计算表明,CuCN 中 CuN 位通过激活 HO 对形成羟基自由基具有积极作用。这项工作将为开发废水环境修复中的高效非均相催化剂提供新的思路。

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