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通过锚定在新型木质素基石墨生物炭上的Fe-N结构活化过一硫酸盐实现双酚A的高效催化降解:电子转移机制

Highly effective catalytic degradation of bisphenol A through activation of peroxymonosulfate by an Fe-N structure anchored on novel lignin-based graphitic biochar: Electron transfer mechanism.

作者信息

Li Zhenrui, Wang Zhihui, Dai Linxin, Ma Jianfeng, Liu Xing'e

机构信息

International Centre for Bamboo and Rattan, Beijing 100102, China; Key Laboratory of National Forestry and Grassland Administration/Beijing for Bamboo & Rattan Science and Technology, Beijing 100102, China.

International Centre for Bamboo and Rattan, Beijing 100102, China; Key Laboratory of National Forestry and Grassland Administration/Beijing for Bamboo & Rattan Science and Technology, Beijing 100102, China.

出版信息

Int J Biol Macromol. 2025 Jan;286:138322. doi: 10.1016/j.ijbiomac.2024.138322. Epub 2024 Dec 3.

Abstract

A lignin-based Fe/N co-doped carbonaceous catalyst was synthesized via freeze-drying followed by pyrolysis to activate peroxymonosulfate (PMS) for efficient degradation of bisphenol A (BPA). The Fe/N co-doped biochar exhibited a high specific surface area (364.84 m/g), hierarchical porous structures, and abundant oxygen-containing functional groups (hydroxyl and carboxyl groups), which enhancing the dispersion of FeO nanoparticle and exposure of catalytic site. The Fe-N-C/PMS system achieved 100 % BPA degradation within 20 min with a corresponding first-order reaction rate constant (k) of 0.4056 min, which outperformed most reported catalysts in efficiency. Quenching and EPR analyses revealed that both free radicals (OH, SO, and O) and non-radical (O) were rate-limiting steps, while graphitic N and Fe-N structures facilitated direct electron transfer from BPA to PMS in electrochemical tests. XPS results confirmed that pyrrolic N, rather than pyridinic N, played a crucial role in forming the Fe-N structure. Moreover, the catalyst showed excellent stability, regeneration capability, and adaptability under diverse conditions, highlighting the potential of the Fe-N-C/PMS system for practical wastewater treatment applications.

摘要

通过冷冻干燥然后热解合成了一种木质素基铁/氮共掺杂碳质催化剂,以活化过一硫酸盐(PMS)用于高效降解双酚A(BPA)。铁/氮共掺杂生物炭具有高比表面积(364.84 m/g)、分级多孔结构和丰富的含氧官能团(羟基和羧基),这增强了FeO纳米颗粒的分散性和催化位点的暴露。Fe-N-C/PMS体系在20分钟内实现了100%的BPA降解,相应的一级反应速率常数(k)为0.4056 min,其效率优于大多数已报道的催化剂。淬灭和电子顺磁共振分析表明,自由基(OH、SO和O)和非自由基(O)均为限速步骤,而在电化学测试中,石墨氮和铁-氮结构促进了双酚A向过一硫酸盐的直接电子转移。X射线光电子能谱结果证实,吡咯氮而非吡啶氮在形成铁-氮结构中起关键作用。此外,该催化剂在不同条件下表现出优异的稳定性、再生能力和适应性,突出了Fe-N-C/PMS体系在实际废水处理应用中的潜力。

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