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碳酸氢根增强铁酸铜纳米粒子对过一硫酸盐的非均相活化用于水中难降解有机污染物的高效去除。

Bicarbonate enhanced heterogeneous activation of peroxymonosulfate by copper ferrite nanoparticles for the efficient degradation of refractory organic contaminants in water.

机构信息

Department of Environmental Science and Engineering, Hubei Water Systematic Pollution Control and Remediation Technology Engineering Center, China University of Geosciences, Wuhan, 430074, China.

Department of Environmental Science and Engineering, Hubei Water Systematic Pollution Control and Remediation Technology Engineering Center, China University of Geosciences, Wuhan, 430074, China.

出版信息

Chemosphere. 2023 Jan;312(Pt 1):137285. doi: 10.1016/j.chemosphere.2022.137285. Epub 2022 Nov 17.

Abstract

Nowadays, the treatment of residual refractory organic contaminants (ROCs) is a huge challenge for environmental remediation. In this study, a potential process is provided by copper ferrite catalyst (CuFeO) activated peroxymonosulfate (PMS, HSO) in the bicarbonate (HCO) enhanced system for efficient removal of Acid Orange 7 (AO7), 2,4-dichlorophenol, phenol and methyl orange (MO) in water. The impact of key reaction parameters, water quality components, main reactive oxygen species (ROS), probable degradation mechanism, rational degradation pathways and catalyst stability were systematically investigated. A 95.0% AO7 (C = 100 mg L) removal was achieved at initial pH (pH) of 5.9 ± 0.1 (natural pH), CuFeO dosage of 0.15 g L, PMS concentration of 0.98 mM, HCO concentration of 2 mM, and reaction time of 30 min. Both sulfate radical (SO) and hydroxyl radical (OH) on the surface of catalyst were proved as the predominant radical species through radical quenching experiments and electron paramagnetic resonance (EPR) analysis. The buffer nature of HCO was partially contributed for the enhanced degradation of AO7 under CuFeO/PMS/HCO system. Importantly, according to C nuclear magnetic resonance (NMR) and EPR analysis, the positive effect of bicarbonate may be mainly attributed to the formation of peroxymonocarbonate (HCO), which may enhance the generation of OH. The magnetic CuFeO particles can be well recycled and the leaching concentration of Cu was acceptable (<1 mg L). Considering the widespread presence of bicarbonate in water environment, this work may provide a safe, efficient, and sustainable technique for the elimination of ROCs from practical complex wastewater.

摘要

如今,处理残留的难处理有机污染物(ROCs)是环境修复的一大挑战。在本研究中,通过在碳酸氢盐(HCO)增强体系中用铁酸铜(CuFeO)催化剂活化过一硫酸盐(PMS,HSO),提供了一种潜在的处理工艺,用于有效去除水中的酸性橙 7(AO7)、2,4-二氯苯酚、苯酚和甲基橙(MO)。系统研究了关键反应参数、水质成分、主要活性氧物质(ROS)、可能的降解机制、合理的降解途径和催化剂稳定性的影响。在初始 pH 值(pH)为 5.9±0.1(自然 pH)、CuFeO 用量为 0.15 g·L、过一硫酸盐浓度为 0.98 mM、HCO 浓度为 2 mM、反应时间为 30 min 的条件下,可实现 95.0%的 AO7(C=100 mg·L)去除率。通过自由基猝灭实验和电子顺磁共振(EPR)分析,证明催化剂表面的硫酸根自由基(SO)和羟基自由基(OH)是主要的自由基物种。HCO 的缓冲性质部分有助于在 CuFeO/PMS/HCO 体系下增强 AO7 的降解。重要的是,根据 C 核磁共振(NMR)和 EPR 分析,HCO 的正效应可能主要归因于过单碳酸根(HCO)的形成,这可能增强 OH 的生成。磁性的 CuFeO 颗粒可以很好地回收,Cu 的浸出浓度可以接受(<1 mg·L)。考虑到 HCO 在水环境中的广泛存在,这项工作可能为从实际复杂废水中消除 ROCs 提供一种安全、高效和可持续的技术。

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