利用过硫酸盐介导的封闭 Fe0 催化剂进行磺胺甲噁唑降解的超快 Fenton 类反应

Chundi Zhou, Yali Guo, Songhang Du, Minghao Sui
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摘要

在此,研究人员采用了一种纳米融合策略来封装纳米零价铁(封闭铁),以便通过过一硫酸盐(PMS)介导的类似芬顿反应快速降解磺胺甲噁唑(SMX)。该封闭态铁催化剂采用液相还原法原位合成,并加入了硝基三乙酸(NA)修饰的羧基碳纳米管(FOC-N-6)。综合实验分析和表征表明,FOC-N-6 催化剂促进了电子通过碳框架和表面 PMS 反应复合物(FOC-N-6-PMS*)的快速转移。这一过程加速了铁(III)/铁(II)氧化还原循环,促进了表面铁(II)活性位点(Fe-OCNT-COOFe(II)-)的形成,而这些位点是 PMS 的主要吸附位点。密度泛函理论(DFT)计算表明,约束铁结构可以降低 PMS 在 FOC-N-6 表面的吸附能()。FOC-N-6-PMS* 可通过非自由基和自由基途径促进 SMX 的快速降解。这种封闭铁催化策略有望成为控制新兴污染物的一种可行方法。
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Ultrafast Fenton-like reaction using a peroxymonosulfate-mediated confined-Fe0 catalyst for the degradation of sulfamethoxazole
Herein, a nanoconfinement strategy was employed to encapsulate nano zero-valent iron (confined-Fe) for the rapid degradation of sulfamethoxazole (SMX) through a peroxymonosulfate (PMS)-mediated Fenton-like reaction. The confined-Fe catalyst was synthesized in situ using a liquid-phase reduction method, incorporating nitrilotriacetic acid (NA) modified carboxylated carbon nanotube (FOC-N-6). Comprehensive experimental analyses and characterizations demonstrated the FOC-N-6 catalyst facilitated rapid electron transfer through the carbon framework and the surface PMS reactive complex (FOC-N-6-PMS*). This process accelerated the Fe(III)/Fe(II) redox cycle and promoted the formation of surface Fe(II) active sites (Fe-OCNT-COOFe(II)-), which served as dominant adsorption sites for PMS. Density functional theory (DFT) calculations revealed that the confined-Fe structure can decrease the adsorption energy () of PMS on the FOC-N-6 surface. And the FOC-N-6-PMS* facilitated the rapid degradation of SMX through both non-radical and radical pathways. This confined-Fe catalytic strategy holds promise as a viable method for controlling emerging contaminants.
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