Efficient degradation of sulfamethoxazole by a peroxymonosulfate system activated by g-C3N4@polyethylene glycol-derived carbon-nitrogen nanosheets: The key roles of N and O groups

被引：7

作者：

Guo, Yanfei ^{[1
,2
]}

Guo, Zhuang ^{[2
,3
]}

Wei, Jian ^{[2
,3
]}

Zhang, Jiali ^{[2
,3
]}

Huang, Yihan ^{[2
,3
]}

Hao, Tong ^{[2
]}

Xu, Dongyao ^{[1
]}

机构：

[1] China Univ Min & Technol Beijing, Coll Chem & Environm Engn, Xueyuan Rd 11, Beijing 100083, Peoples R China

[2] Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China

[3] Chinese Res Inst Environm Sci, Inst Water Ecol & Environm, Beijing 100012, Peoples R China

来源：

SEPARATION AND PURIFICATION TECHNOLOGY | 2024年 / 337卷

基金：

中国国家自然科学基金;

关键词：

Metal -free catalyst; Peroxymonosulfate; Sulfamethoxazole; Singlet oxygen; Active site; DOPED GRAPHENE; CATALYTIC-OXIDATION;

D O I：

10.1016/j.seppur.2024.126267

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

A simultaneous thermal polymerization reaction was performed with graphitic carbon nitride and polyethylene glycol to synthesize a novel metal-free carbon-nitrogen (CN) material, and the prepared material was applied to activate a peroxymonosulfate (PMS) system. Sulfamethoxazole (SMX) removal by CN7/PMS reached 93.75 % in 10 min, which was 39.86 times higher than that achieved by PMS systems alone. Material characterization showed that the pyrolysis temperature could be adjusted to modulate the N atom and functional group contents. As determined by experimental validation and DFT calculations, C = O/C-N, graphitic N and defects were the main active sites. This finding indicates that CN7 activated PMS to produce hydroxyl radicals (center dot OH), sulfate radicals (SO4 center dot-) and singlet oxygen (1O2) through electrostatic interactions, nucleophilic addition, electron transfer and other pathways. Moreover, 1O2 was dominant, with a 91.58 % contribution. In addition, the materials maintained high catalytic stability in different water matrices and multiple cycling experiments. The present study innovatively illustrated the mechanism by which nitrogen-doped carbon materials activated PMS, providing a new insight into the development of highly active metal-free catalysts applied in PMS systems.

引用

页数：11