过硫酸盐
生物炭
热解
过氧二硫酸盐
电子转移
化学
电子顺磁共振
光化学
激进的
羟基自由基
碳纳米管
无机化学
材料科学
化学工程
催化作用
纳米技术
有机化学
工程类
物理
核磁共振
作者
Tong Liu,Qi Wang,Chen‐Xuan Li,Minshu Cui,Yawen Chen,Rui Liu,Kangping Cui,Ke Wu,Xianbao Nie,Sanliu Wang
标识
DOI:10.1016/j.jclepro.2022.131669
摘要
Nitrogen-doped magnetic carbon nanotubes-bridged biochar (Fe 3 O 4 @NCNTs-BC) was prepared by facile impregnation and pyrolysis strategies and showed an excellent capacity in activating persulfate for sulfamethoxazole (SMX) degradation. The airtight structure of iron oxide (Fe 3 O 4 ) nanoparticles embedded in N-doped CNTs (NCNTs) was supported by biochar ( BC ) that could both promote the electron transfer and avoid large amounts of metal leaching. Quenching experiments, electron spin resonance (ESR) and in situ Raman spectroscopy analysis were performed to explore the dominant active species . In contrast to the superoxide radical (O 2 • - ) dominated radical mechanism in the peroxymonosulfate (PMS) activation process , a direct electron transfer regime involving surface-bound metastable complexes was found to play a decisive role in the Fe 3 O 4 @NCNTs-BC 800 /peroxydisulfate (PDS) system. HSO 5 − was decomposed to active radicals for SMX oxidation in the Fe 3 O 4 @NCNTs-BC 800 /PMS/SMX system, yet carbon-PDS* complexes could be consumed by extracting electrons from the SMX. The surface hydroxyl groups of carbon-based catalysts and the structure discrepancies between PMS and PDS could lead to the differences in degradation performances and activation regimes. The degradation intermediates of SMX were also evaluated, and the toxicity analysis was undertaken. This work provides insight into the underlying mechanisms of persulfate activation and mediated electron transfer by carbon-metal nanohybrids. • Fe 3 O 4 @NCNTs-BC 800 was synthesized by impregnation and pyrolysis strategies. • SMX could be efficiently removed in the Fe 3 O 4 @NCNTs-BC 800 /PS systems. • O 2 .• - dominated the degradation of SMX in the Fe 3 O 4 @NCNTs-BC 800 /PMS system. • Surface-bound carbon-PDS* complexes could directly extract electrons from SMX. • The environmental toxicity of SMX reduced in the Fe 3 O 4 @NCNTs-BC 800 /PMS system.
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