Fe-Mn oxycarbide anchored on N-doped carbon for enhanced Fenton-like catalysis: Importance of high-valent metal-oxo species and singlet oxygen

被引：118

作者：

He, Yangzhuo ^{[1
,2
]}

Qin, Hong ^{[1
,2
]}

Wang, Ziwei ^{[1
,2
]}

Wang, Han ^{[3
]}

Zhu, Yuan ^{[1
,2
]}

Zhou, Chengyun ^{[1
,2
]}

Zeng, Ying ^{[1
,2
]}

Li, Yicheng ^{[1
,2
]}

Xu, Piao ^{[1
,2
]}

Zeng, Guangming ^{[1
,2
]}

机构：

[1] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Peoples R China

[2] Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Peoples R China

[3] Cent South Univ, Sch Met & Environm, Changsha 410083, Hunan, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2024年 / 340卷

基金：

中国国家自然科学基金;

关键词：

Peroxymonosulfate activation; Bimetal catalyst; Singlet oxygen; High-valent metal; Wastewater treatment; WASTE-WATER TREATMENT; NONRADICAL ACTIVATION; SELECTIVE DEGRADATION; BISPHENOL-A; OXIDATION; PEROXYMONOSULFATE; POLLUTANTS;

D O I：

10.1016/j.apcatb.2023.123204

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A nonradical oxidation-based peroxymonosulfate (PMS) activation is an attractive process for pollutant elimination. Herein, a dual-metal-organic framework (MOF) assisted strategy to construct magnetic Fe-Mn oxycarbide anchored on N-doped carbon (FeMn@NC) was proposed for PMS activation. It was found that FeMn@NC-800 displayed superior activity than other comparable counterparts, with nearly 100 % degradation of sulfamethazine (SMZ) within 30 min. Electron paramagnetic resonance and quenching tests revealed that nonradical oxidation (1O2 and high-valent metal-oxo species) dominated the SMZ degradation process. Experimental and theoretical calculations demonstrated that FeMn oxycarbide preferred adsorbing the terminal O of PMS, which could improve the PMS oxidization to produce SO5 & BULL;, further generating 1O2. Moreover, dual active sites could lower the energy barrier to cleave the O  O bond of PMS to form high-valent FeMn=O species. The present study provided a clue to rationally design high-performance heterogeneous catalysts and proposed a novel nonradical-based catalytic oxidation for environmental cleaning.

引用

页数：12

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