Luo Peiran, Zhang Fuping, Yang Guo, Chen Yue, Li Min, Luo Yan, Jiang Liang, Zhou Qian, Wang Yi, Xing Bo
School of Chemistry Engineering, Sichuan University of Science & Engineering, Zigong 643000, Sichuan, P. R. China.
National Engineering Laboratory of Circular Economy, Sichuan University of Science and Engineering, Zigong 643000, Sichuan, P. R. China.
Langmuir. 2025 Jul 22;41(28):18809-18820. doi: 10.1021/acs.langmuir.5c02120. Epub 2025 Jul 7.
The electro-Fenton process is considered one of the most reliable techniques for eliminating organic pollutants from water. However, its performance is still not up to par with its potential due to the lack of cathodic catalysts with the essential cycling catalytic functionality required for sustained Fenton reactions. Herein, Fe and FeO heterojunctions embedded in N-doped carbon nanotubes stitched on porous nitrogen-doped carbon (denoted Fe/FeO@PNC) are fabricated and employed as a bifunctional cathode catalyst for the highly efficient degradation of organic pollutants. The N-doped carbon with rich pyridinic-N sites enables in situ generation of HO via a two-electron oxygen reduction reaction (ORR), while Fe/FeO heterojunctions with multivalent states promote the cycling efficiency of Fe/Fe for activating HO to produce reactive oxidative species (ROS) of O and O. Benefitting from the synergistic effects between Fe/FeO heterojunctions and N-doped carbon nanotubes, along with abundant mass transfer channels and rapid Fe/Fe cycling, Fe/FeO@PNC, as a heterogeneous cathode electrocatalyst, displays superior catalytic activity, achieving a favorable organic pollutant removal efficiency of 98.72% within 1 h. This study provides a feasible way to the rational design of Fe-based heterojunction cathode materials for an efficient electro-Fenton process.
电芬顿法被认为是从水中去除有机污染物最可靠的技术之一。然而,由于缺乏具有持续芬顿反应所需基本循环催化功能的阴极催化剂,其性能仍未达到其潜力。在此,制备了嵌入在多孔氮掺杂碳上缝合的氮掺杂碳纳米管中的铁和氧化亚铁异质结(表示为Fe/FeO@PNC),并将其用作双功能阴极催化剂用于高效降解有机污染物。具有丰富吡啶氮位点的氮掺杂碳能够通过双电子氧还原反应(ORR)原位生成羟基自由基(HO),而具有多价态的铁/氧化亚铁异质结促进铁/亚铁的循环效率,以激活羟基自由基生成单线态氧(O)和超氧阴离子(O)的活性氧化物种(ROS)。受益于铁/氧化亚铁异质结与氮掺杂碳纳米管之间的协同效应,以及丰富的传质通道和快速的铁/亚铁循环,Fe/FeO@PNC作为一种非均相阴极电催化剂,表现出优异的催化活性,在1小时内实现了98.72%的良好有机污染物去除效率。本研究为合理设计用于高效电芬顿过程的铁基异质结阴极材料提供了一条可行的途径。