Mediating peroxymonosulfate activation path in Fenton-like reaction via doping different metal atoms into g-C3N5

• Published in: Journal of colloid and interface science 2024-11, Vol.674, p.416-427
• Main Authors: Lv, Wenwen, Cao, Huijun, Guan, Yina, Wu, Maoquan, Liu, Hongyan, Guo, Xu, Yao, Tongjie, Chen, Peng, Sheng, Li, Wu, Jie
• Format: Article
• Language: English
• Subjects: Fenton-like reaction; g-C3N5; Non-radical activation path; PMS activation; Radical activation path
• ISSN: 0021-9797; 1095-7103; 1095-7103
• DOI: 10.1016/j.jcis.2024.06.160

Peroxymonosulfate activation paths in Fenton-like reaction were successfully mediated via simply altering the doped metal atoms into g-C3N5. Fe-C3N5 followed a non-radical activation path displayed superior catalytic activity than Co-C3N5 followed a radical path. [Display omitted] •PMS activation paths are mediated by altering doped metal atoms in g-C3N5.•k value in TC degradation over Fe-C3N5 is 3.14 times higher than Co-C3N5.•Co-C3N5 follows radical activation path, while Fe-C3N5 follows non-radical one.•ROS contributions over Fe-C3N5 and Co-C3N5 are calculated and compared.•DFT study and experimental data support varied activation path on Fe-C3N5 and Co-C3N5. Peroxymonosulfate (PMS) could be activated by either radical path or non-radical path, how to rationally mediate these two routines was an important unresolved issue. This work has introduced a simple way to address this problem via metal atom doping. It was found that Fe-doped nitrogen-rich graphitic carbon nitride (Fe-C3N5) exhibited high activity towards PMS activation for tetracycline degradation, and the degradation rate was 3.14 times higher than that of Co-doped nitrogen-rich graphitic carbon nitride (Co-C3N5). Radical trapping experiment revealed the contributions of reactive species over two catalysts were different. Electron paramagnetic resonance analysis further uncovered the non-radical activation path played a dominated role on Fe-C3N5 surface, while the radical activation path was the main routine on Co-C3N5 surface. Density functional theory calculations, X-ray photoelectron spectroscopy analysis, and electrochemical experiments provided convincing evidence to support these views. This study supplied a novel method to mediate PMS activation path via changing the doped metal atom in g-C3N5 skeleton, and it allowed us to better optimize the PMS activation efficiency.