Activation of peroxydisulfate for selective degradation of organic pollutants using magnetic acetylene black in sp2 configuration: Synthesis, performance, and mechanism

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-01-22 DOI:10.1016/j.seppur.2025.131737
Fengkai Yang, Chenlin Hou, Liang Sun, Jinlong Yang, Tianxing Chen, Lipeng Wang, Xiaowei Kong, Yang Zhang
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Abstract

Carbon materials have garnered increasing attention due to their capacity for activating persulfate in pollutant degradation. Among these materials, acetylene black (AB), which possesses a distinct sp2 configuration compared to conventional carbon materials, has been reported as an efficient activator for PDS. However, challenges pertaining to separation and reusability impede its practical application. In this study, we synthesized magnetic acetylene black (MAB) through a facile hydrothermal method. Batch experiments demonstrated that MAB exhibits excellent adsorption performance for the target pollutant and can effectively activate PDS, resulting in over 99 % degradation of BPA when using 1 g/L of MAB and 1 mM PDS. Furthermore, MAB exhibited remarkable efficacy over a broad pH range, superior tolerance towards inorganic anionic species, and easy separation from solution facilitated by an external magnet. The results of radical quenching experiments and electron paramagnetic resonance confirmed the significant role played by an electron transfer pathway in the removal process. Additionally, the OAbstract ImageCAbstract ImageO groups of MAB (such as carboxyl) acted as reaction sites, facilitating this electron transfer mechanism. Moreover, the MAB + PDS system displayed exceptional selectivity for degrading electron-rich organic compounds, and the quantitative structure–activity relationships (QSAR) analysis revealed a strong linear correlation between removal performance and ionization potentials of these organics, further supporting the predominant contribution of the electron transfer pathway involved. Overall, this work not only presents a successful strategy for applying carbon materials in wastewater treatment but also contributes to understanding the mechanisms underlying persulfate activation using highly graphitized carbon materials.

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磁性乙炔黑在sp2结构下活化过硫酸氢盐选择性降解有机污染物:合成、性能和机理
碳材料因其在污染物降解中活化过硫酸盐的能力而受到越来越多的关注。在这些材料中,乙炔黑(AB)与传统碳材料相比具有明显的sp2构型,被报道为PDS的有效活化剂。然而,与分离和可重用性相关的挑战阻碍了它的实际应用。本研究采用水热法合成磁性乙炔黑(MAB)。批量实验表明,MAB对目标污染物具有良好的吸附性能,可有效活化PDS,当MAB用量为1 g/L, PDS用量为1 mM时,BPA的降解率可达99% %以上。此外,MAB在较宽的pH范围内表现出显著的功效,对无机阴离子具有较强的耐受性,并且在外部磁铁的帮助下易于从溶液中分离。自由基猝灭实验和电子顺磁共振的结果证实了电子转移途径在去除过程中起重要作用。此外,MAB的OCO基团(如羧基)作为反应位点,促进了这种电子转移机制。此外,MAB + PDS系统对富含电子的有机化合物表现出优异的选择性,定量结构-活性关系(QSAR)分析显示,这些有机物的去除性能与电离势之间存在很强的线性关系,进一步支持了电子转移途径的主要贡献。总的来说,这项工作不仅提出了在废水处理中应用碳材料的成功策略,而且有助于理解使用高度石墨化的碳材料进行过硫酸盐活化的机制。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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