Xu Shizhe, Wang Pengfei, Mi Xueyue, Bao Yueping, Zhang He, Mo Fan, Zhou Qixing, Zhan Sihui
MOE Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Carbon Neutrality Interdisciplinary Science Center, College of Environmental Science and Engineering Nankai University, Tianjin 300350, China.
MOE Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Carbon Neutrality Interdisciplinary Science Center, College of Environmental Science and Engineering Nankai University, Tianjin 300350, China.
J Hazard Mater. 2024 Mar 15;466:133321. doi: 10.1016/j.jhazmat.2023.133321. Epub 2023 Dec 20.
Heteroatom doping represents a promising strategy for enhancing the generation of singlet oxygen (O) during the activation of peroxymonosulfate (PMS) using carbon-based catalysts; however, it remains a formidable challenge. In this study, we systematically controlled the structure of metal-free carbon-based materials by introducing different heteroatoms to investigate their efficacy in degrading organic pollutants in water via PMS activation. The results of reactive oxygen species detection showed that the dominant free radical in the four samples was different: CN (•SO and •OH), CNS (•O), CNCl (O), and CNClS (O). This led to the transformation of active species from free radicals to non-free radicals. The tri-doped carbons with nitrogen, sulfur, and chlorine (CNClS) exhibited exceptional performance in PMS activation and achieved a remarkable degradation efficiency of 95% within just 6 min for tetracycline. Moreover, a strong linear correlation was observed between the ratio of pyridine-N/graphite-N and I/I with the yield of O, indicating that N species and defects play a crucial role in CNClS as they facilitate the transition from radical to non-radical pathways during PMS activation. These findings highlight the possibility that adjustable tri-heteroatom doping will expand the Fenton-like reaction for the treatment of actual wastewater.
杂原子掺杂是一种很有前景的策略，可用于增强在使用碳基催化剂活化过一硫酸盐（PMS）过程中单线态氧（O）的生成；然而，这仍然是一个巨大的挑战。在本研究中，我们通过引入不同的杂原子系统地控制了无金属碳基材料的结构，以研究它们通过PMS活化降解水中有机污染物的效果。活性氧检测结果表明，四个样品中的主要自由基各不相同：CN（•SO和•OH）、CNS（•O）、CNCl（O）和CNClS（O）。这导致活性物种从自由基转变为非自由基。氮、硫和氯三掺杂的碳（CNClS）在PMS活化方面表现出优异的性能，对于四环素，在仅6分钟内就实现了95%的显著降解效率。此外，观察到吡啶-N/石墨-N的比例与I/I与O的产率之间存在很强的线性相关性，表明N物种和缺陷在CNClS中起着关键作用，因为它们在PMS活化过程中促进了从自由基途径到非自由基途径的转变。这些发现突出了可调节的三杂原子掺杂将扩展类芬顿反应用于处理实际废水的可能性。
