Zuo Shiyu, Wang Yan, Wan Jinquan
School of Environment and Energy, South China University of Technology, Guangzhou, China.
School of Environment and Energy, South China University of Technology, Guangzhou, China; Guangdong Plant Fiber High-Valued Cleaning Utilization Engineering Technology Research Center, Guangzhou, China; State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou, China.
J Colloid Interface Sci. 2025 Jan 15;678(Pt A):713-721. doi: 10.1016/j.jcis.2024.08.181. Epub 2024 Aug 28.
Peroxymonosulfate (PMS) activation technology has important application value in treating emerging contaminant (ECs), but it still faces challenges in achieving efficient electron transfer and metal valence cycling. In this study, the interfacial electric field characteristics of FeNC catalysts were adjusted by introducing NC defects to affect the electron transfer process, thereby enhancing the catalytic performance of PMS. It is found that in the FeNC structure, the shift of the charge generates an interfacial electric field, which can promote the directional transfer of electrons. Through quantitative structure-activity relationship (QSAR) analysis, it was confirmed that the defect played a decisive role in regulating the interfacial electric field and improving the catalytic reaction efficiency. The interfacial electric field-mediated superexchange interaction realizes the electron donor effect of organic pollutants and the effective electron transfer between the Fe site, accelerates the electron cycling of the Fe site, and realizes the rapid and stable catalysis of PMS. The increase of the occupancy state distribution of d orbitals near the Fermi level provides favorable conditions for electron transitions and catalytic activation of PMS. ECs can be converted into environmentally friendly, non-toxic and harmless substances through. This defect-controlled interface electric field strategy realizes rapid electron directional transfer, which provides a new solution for improving the catalytic efficiency of PMS and the safe treatment of ECs in water.
过一硫酸盐（PMS）活化技术在处理新兴污染物（ECs）方面具有重要的应用价值，但在实现高效电子转移和金属价态循环方面仍面临挑战。在本研究中，通过引入NC缺陷来调节FeNC催化剂的界面电场特性，以影响电子转移过程，从而提高PMS的催化性能。研究发现，在FeNC结构中，电荷的转移产生了界面电场，可促进电子的定向转移。通过定量构效关系（QSAR）分析，证实缺陷在调节界面电场和提高催化反应效率方面起决定性作用。界面电场介导的超交换相互作用实现了有机污染物的电子供体效应以及Fe位点之间的有效电子转移，加速了Fe位点的电子循环，实现了PMS的快速稳定催化。费米能级附近d轨道占据态分布的增加为电子跃迁和PMS的催化活化提供了有利条件。新兴污染物可通过该过程转化为环境友好、无毒无害的物质。这种缺陷控制的界面电场策略实现了快速的电子定向转移，为提高PMS的催化效率及水中新兴污染物的安全处理提供了新的解决方案。
