Insight into the synergistic acceleration effects of EDTA and hydroxylamine in heterogeneous Fenton-like reaction over a wide initial pH range

IF 3.6 4区环境科学与生态学 Q3 ENGINEERING, ENVIRONMENTAL

Environmental Engineering Research Pub Date : 2025-05-14 DOI:10.4491/eer.2025.008

Siling Luo, Jianping Ai, Yang Kuang, Li-Hong Cheng, Lixing Liang, Yi Wang, Hongzhan Dai, Quan Sun, Zehua Zhou, Wenkui Li

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引用次数: 1

Abstract

Chelating agent modification and reductant enhancement are effective strategies to improve the narrow working pH and Fe3+/Fe2+ cycle delay of a heterogeneous Fenton system. However, the different mechanisms for the promotional effects between disodium ethylenediaminetetraacetate (EDTA) and hydroxylamine (HA) are rarely reported. Herein, the effects of EDTA and HA on the degradation kinetics of the selected probe compounds were compared in the CoFe2O4/H2O2 system for the first time. This paper found that the EDTA-chelated CoFe2O4 Fenton-like system enhanced the activation rate of H2O2 via reducing the redox potential of Fe2+/Fe3+ and Co2+/Co3+ pairs. The apparent rate constant of methyl orange (MO) in the CoFe2O4/H2O2/HA system was approximately 84-fold higher than that in the CoFe2O4/H2O2 system under the reaction conditions with 1.0 mM of HA and pH 6.4 within 180 min. This result was attributed to the dynamic equilibrium of Fe3+/Fe2+ and Co3+/Co2+ redox cycles after the addition of HA. Based on quenching experiments and electron paramagnetic resonance (EPR), these superior activities are due to the hydroxyl radicals (•OH) and singlet oxygen (1O2) under circumneutral pH, whereas •OH is the major reactive oxygen species (ROS) at pH values <4 or >10. The potential mechanism of CoFe2O4/H2O2/EDTA/HA systems was elucidated.

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在较宽的初始pH范围内，EDTA和羟胺在非均相fenton样反应中的协同加速效应

螯合剂改性和还原剂增强是改善非均相Fenton体系窄工作pH和Fe3+/Fe2+循环延迟的有效策略。然而，关于乙二胺四乙酸二钠（EDTA）和羟胺（HA）促进作用的不同机制鲜有报道。本文首次比较了EDTA和HA对所选探针化合物在CoFe2O4/H2O2体系中降解动力学的影响。本文发现edta螯合CoFe2O4 Fenton-like体系通过降低Fe2+/Fe3+和Co2+/Co3+对的氧化还原电位来提高H2O2的活化率。在1.0 mM HA和pH 6.4条件下，180 min内，CoFe2O4/H2O2/HA体系中甲基橙（MO）的表观速率常数比CoFe2O4/H2O2体系中甲基橙（MO）的表观速率常数高约84倍。这一结果归因于添加HA后Fe3+/Fe2+和Co3+/Co2+氧化还原循环的动态平衡。根据淬火实验和电子顺磁共振（EPR），这些优越的活性是由于在环中性pH下羟基自由基（•OH）和单线态氧（1O2），而在pH值为<；4或>；10时，•OH是主要的活性氧（ROS）。阐明了CoFe2O4/H2O2/EDTA/HA体系的潜在机理。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Environmental Engineering Research Environmental Science-Environmental Engineering

CiteScore

7.50

自引率

5.70%

发文量

期刊介绍： The Environmental Engineering Research (EER) is published quarterly by the Korean Society of Environmental Engineers (KSEE). The EER covers a broad spectrum of the science and technology of air, soil, and water management while emphasizing scientific and engineering solutions to environmental issues encountered in industrialization and urbanization. Particularly, interdisciplinary topics and multi-regional/global impacts (including eco-system and human health) of environmental pollution as well as scientific and engineering aspects of novel technologies are considered favorably. The scope of the Journal includes the following areas, but is not limited to: 1. Atmospheric Environment & Climate Change: Global and local climate change, greenhouse gas control, and air quality modeling. 2. Renewable Energy & Waste Management: Energy recovery from waste, incineration, landfill, and green energy. 3. Environmental Biotechnology & Ecology: Nano-biosensor, environmental genomics, bioenergy, and environmental eco-engineering. 4. Physical & Chemical Technology: Membrane technology and advanced oxidation. 5. Environmental System Engineering: Seawater desalination, ICA (instrument, control, and automation), and water reuse. 6. Environmental Health & Toxicology: Micropollutants, hazardous materials, ecotoxicity, and environmental risk assessment.