Experimental and kinetic analysis of Hg0 removal by CoFe2O4 nanoparticles as an efficient activator of persulfate

IF 3.5 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Atmospheric Pollution Research Pub Date : 2025-02-08 DOI:10.1016/j.apr.2025.102453
Qianqian Zhang, Haixing Du, Anchao Zhang, Hongyu Zheng, Haixia Li, Weiwei Zhang, Zhijun Sun
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Abstract

The sulfate radical (SO4•−) and hydroxyl radical (OH), derived from the oxidation of persulfate (PS), are significant active substances in the treatment of pollution. In this study, magnetic CoFe2O4 nanoparticles (CFO NPs) were synthesized by a hydrothermal method and applied to activate PS for Hg0 removal from the simulated flue gas. The results exhibited that the Hg0 removal efficiency can reach as high as 99.5% within 60 min under the optimal condition of 6 mM of PS, 0.8 g/L of CFO dose, 20 °C of reaction temperature and 7 of initial pH. The characterizations demonstrated that the large surface area and coexistence of Co/Fe mixed valence were generated after the formation of CFO nanostructure, improving the amount of active sites and facilitating the adsorption and activation of PS. Scavenging tests indicated that SO4•− and OH were the main active radicals on Hg0 removal, where the OH radicals primarily originated from the conversion of SO4•−. Moreover, the circulation of ≡Co(III)/≡Co(II) and ≡Fe(III)/≡Fe(II) resulted in a superior Hg0 removal activity. Based on the experiments and characterization analysis, the reaction mechanism was proposed. In addition, the kinetic model for Hg0 removal was systematically analyzed, and the role of SO4•− and OH was further verified. This study provided new insights toward efficient activation of persulfate for removal of Hg0 from coal-fired flue gas.

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CoFe2O4纳米颗粒作为过硫酸盐高效活化剂去除Hg0的实验及动力学分析
过硫酸盐(PS)氧化产生的硫酸盐自由基(SO4•−)和羟基自由基(•OH)是治理污染的重要活性物质。本研究采用水热法合成了磁性CoFe2O4纳米颗粒(CFO NPs),并应用于活化PS去除模拟烟气中的Hg0。结果表明,在PS用量为6 mM、CFO用量为0.8 g/L、反应温度为20℃、初始ph为7的最佳条件下,60 min内Hg0去除率可达99.5%。表征表明,CFO纳米结构形成后产生了较大的比表面积和Co/Fe混合价态共存;清除试验表明,SO4•−和•OH是去除Hg0的主要活性自由基,其中•OH自由基主要来源于SO4•−的转化。此外,≡Co(III)/≡Co(II)和≡Fe(III)/≡Fe(II)的循环导致了较好的Hg0去除活性。在实验和表征分析的基础上,提出了反应机理。此外,系统分析了Hg0脱除的动力学模型,并进一步验证了SO4•−和•OH的作用。该研究为过硫酸盐高效活化脱除燃煤烟气中Hg0提供了新的见解。
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来源期刊
Atmospheric Pollution Research
Atmospheric Pollution Research ENVIRONMENTAL SCIENCES-
CiteScore
8.30
自引率
6.70%
发文量
256
审稿时长
36 days
期刊介绍: Atmospheric Pollution Research (APR) is an international journal designed for the publication of articles on air pollution. Papers should present novel experimental results, theory and modeling of air pollution on local, regional, or global scales. Areas covered are research on inorganic, organic, and persistent organic air pollutants, air quality monitoring, air quality management, atmospheric dispersion and transport, air-surface (soil, water, and vegetation) exchange of pollutants, dry and wet deposition, indoor air quality, exposure assessment, health effects, satellite measurements, natural emissions, atmospheric chemistry, greenhouse gases, and effects on climate change.
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