Ferrocene doped ZIF-8 derived Fe-N-C single atom catalyst to active peroxymonosulfate for removal of bisphenol A

• Published in: Separation and purification technology Vol. 305; p. 122402
• Main Authors: Huang, Zhikun, Yu, Haojie, Wang, Li, Wang, Mingyuan, Liu, Xiaowei, Shen, Di, Shen, Sudan, Ren, Shuning, Lin, Tengfei, Lei, Shuangying
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 15.01.2023
• Subjects: Advanced oxidation process; Bisphenol A; DFT calculations; Single atom catalyst; Bisphenol A; Single atom catalyst; DFT calculations; Advanced oxidation process
• ISSN: 1383-5866; 1873-3794
• DOI: 10.1016/j.seppur.2022.122402

•The Fe content of Fe-N-C SACs can be precisely controlled during synthesis process.•The BPA can be removed entirely within 10 min using low content of Fe-N-C SACs.•The optimal apparent rate constant of Fe-N-C was 9.48 times faster than that of N-C.•The interactions between Fe-N-C and PMS/BPA were studied by DFT calculations. Heterogeneous advanced oxidation process (AOP) technique exhibits a great potential to degrade recalcitrant and toxic bisphenol A (BPA) in water; however, traditional catalysts seriously suffer from agglomeration, leaching of active metal ions and poor stability. Herein, a serial of single atom catalysts (SACs) based on single Fe atoms anchored on N-doped porous carbon matrix (Fe-N-C) were successfully prepared through simple pyrolysis method. The Fe content of Fe-N-C could be accurately controlled by changing the doped ferrocene (Fc) in ZIF-8 precursor. The obtained Fe-N-C exhibited outstanding catalytic activity to active peroxymonosulfate (PMS) for BPA degradation, 94.3% BPA could be removed within 10 min, the reaction rate constant (k) of Fe-N-C reached to 0.395 min−1, which was 9.5 times faster than that of counterpart N-C, which derived from the synergistic effect of radical pathway, non-radical pathway and electron-transfer. In Fe-N-C/PMS system, the singlet oxygen (1O2) has been proved as the main reactive oxygen species (ROS) to dominate the BPA degradation process. Besides, the Fe-N-C/PMS and Fe-N-C/BPA interfacial interactions were investigated by density functional theory (DFT) calculations, which disclosed the formation of high-valent iron-oxo species (Fe(IV)=O) and interfacial electron-transfer to comprehensively and thoroughly investigate the mechanism of BPA degradation. This work aims to providing novel insight for investigation of BPA degradation mechanism in AOP system.