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

作者：Shuo Li, Yalun Yang, Junfeng Niu, Heshan Zheng, Wen Zhang, Yoong Kit Leong, Jo‐Shu Chang, Bo Lai · 发表于：Environmental Science & Technology · 年份：2024 · DOI：10.1021/acs.est.4c08224 · 被引用次数：82 · 研究领域：Advanced Photocatalysis Techniques、Advanced Nanomaterials in Catalysis、Carbon and Quantum Dots Applications

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-C 3 N 4 ) 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-C 3 N 4 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.