Unique role of doped Mo into Fe-based catalyst to intensify peroxydisulfate activation for micropollutants degradation: Promote the conversion of SO4•- to FeIV = O

被引：0

作者：

Li, Taozhen ^{[1
]}

Wang, Xinyuan ^{[1
]}

Fan, Zihao ^{[1
]}

Wang, Xiaoning ^{[1
]}

Wu, Zhuohang ^{[1
]}

Akram, Muhammad ^{[2
]}

Wang, Lei ^{[1
]}

Liu, Juan ^{[1
]}

Pan, Jingwen ^{[1
]}

Gao, Baoyu ^{[3
]}

机构：

[1] Qingdao Univ Sci & Technol, Coll Environm & Safety Engn, Key Lab Ecochem Engn, Qingdao 266042, Peoples R China

[2] Nanjing Univ Sci & Technol, Sch Chem & Chem Engn, Nanjing 210094, Peoples R China

[3] Shandong Univ, Sch Environm Sci & Engn, Shandong Key Lab Water Pollut Control & Resource R, Qingdao 266237, Peoples R China

来源：

CHEMICAL ENGINEERING JOURNAL | 2024年 / 500卷

基金：

中国国家自然科学基金;

关键词：

Fe-based catalyst; Sulfate radical; Mo doping; Peroxydisulfate; High-valent iron species;

D O I：

10.1016/j.cej.2024.157255

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Herein, Fe/Mo-based composite catalyst (FeMo@CN) was synthesized to catalyze peroxydisulfate (PDS) for efficient bisphenol A (BPA) degradation. Within 1 h, the FeMo@CN/PDS system could degrade BPA fully (k(obs) = 0.12 min(-1), which was 129 times higher than system without Mo introduction). Probe experiments and Fe-57 Mossbauer indicated that BPA degradation was dominated by SO4 center dot- and Fe-IV = O converted from SO4 center dot- (Fe(II)-PDS -> Fe(III)-SO4 center dot--> Fe-IV = O-HSO4-). This finding broke down the boundary between radical and non-radical, proposing a new path from SO4 center dot- to Fe-IV = O. As Density functional theory (DFT) calculations revealed, Mo in FeMo@CN promoted PDS adsorption and reduced generation energy barrier of SO4 center dot- and Fe-IV = O, achieving a dual improvement. Besides, the stable and efficient BPA degradation in dynamic degradation experiment demonstrated the application potential of FeMo@CN. This work provides a novel method to solve blocked Fe(II)/Fe(III) cycle and re-reveals Fe-IV = O generation mechanism in SR-AOPs.

引用

页数：10