Activation of PAA at the Fe-N x Sites by Boron Nitride Quantum Dots Enhanced Charge Transfer Generates High-Valent Metal-Oxo Species for Antibiotics Degradation

被引:2
|
作者
Li, Shuo [1 ]
Yang, Yalun [2 ]
Niu, Junfeng [2 ]
Zheng, Heshan [1 ]
Zhang, Wen [3 ]
Leong, Yoong Kit [4 ,5 ]
Chang, Jo-Shu [4 ,5 ,6 ]
Lai, Bo [7 ]
机构
[1] Qiqihar Univ, Coll Food & Bioengn, Qiqihar 161006, Peoples R China
[2] North China Elect Power Univ, Coll Environm Sci & Engn, Beijing 102206, Peoples R China
[3] New Jersey Inst Technol, John A Reif Jr Dept Civil & Environm Engn, Newark, NJ 07102 USA
[4] Tunghai Univ, Dept Chem & Mat Engn, Taichung 407, Taiwan
[5] Tunghai Univ, Res Ctr Smart Sustainable Circular Econ, Taichung 407, Taiwan
[6] Yuan Ze Univ, Dept Chem Engn & Mat Sci, Chungli 320, Taiwan
[7] Sichuan Univ, Sch Architecture & Environm, Dept Environm Sci & Engn, Chengdu 610065, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
peracetic acid; high-valent iron-oxo species; Fe-N <italic>x</italic> sites; selectiveattack; PERACETIC-ACID; OXIDATION; G-C3N4;
D O I
10.1021/acs.est.4c08224
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Advanced oxidation processes (AOPs) based on peracetic acid (PAA) offer a promising strategy to address antibiotic wastewater pollution. In this study, Fe-doped graphitic carbon nitride (g-C3N4) nanomaterials were used to construct Fe-N x sites, and the electronic structure was tuned by boron nitride quantum dots (BNQDs), thereby optimizing PAA activation for the degradation of antibiotics. The BNQDs-modified Fe-doped g-C3N4 catalyst (BNQDs-FCN) achieved an excellent reaction rate constant of 0.0843 min-1, marking a 21.6-fold improvement over the carbon nitride (CN)-based PAA system. DFT calculations further corroborate the superior adsorption capacity of the Fe-N x sites for PAA, facilitating its activation. Charge transfer mechanisms, with PAA serving as an electron acceptor, were identified as the source of high-valent iron-oxo species. Moreover, the BNQDs-FCN system preferentially targets oxygen-containing functional groups in antibiotic structures, elucidating the selective attack patterns of these highly electrophilic species. This research not only elucidates the pivotal role of high-valent iron-oxo species in pollutant degradation within the PAA-AOPs framework but also pioneers a wastewater treatment system characterized by excellent degradation efficiency coupled with low ecological risk, thereby laying the groundwork for applications in wastewater management and beyond.
引用
收藏
页码:21871 / 21881
页数:11
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