College of Environment and Ecology, Hunan Agricultural University, Changsha, 410128, PR China; Laboratory of Environmental Technology, INET, Tsinghua University, Beijing, 100084, PR China.
Laboratory of Environmental Technology, INET, Tsinghua University, Beijing, 100084, PR China; Beijing Key Laboratory of Radioactive Waste Treatment, INET, Tsinghua University, Beijing, 100084, PR China.
Environ Pollut. 2024 Aug 15;355:124198. doi: 10.1016/j.envpol.2024.124198. Epub 2024 May 21.
Electro-Fenton (EF) can in-situ produce HO and effectively activate HO to generate powerful reactive species for the destruction of contaminants under acidic conditions, however, the production of iron-containing sludge and requirement of low working pH significantly hinder its practical application. Herein, a novel Cu, N co-doped carbon (Cu-N@C) with metal organic framework (MOF) as a precursor was constructed and adopted for the elimination of pefloxacin (PEF) in the heterogeneous electro-Fenton (HEF) process. PEF could be almost completely removed within 1 h and total organic carbon (TOC) removal efficiency was 48.57% within 6 h. Meanwhile, Cu-N@C had good repeatability and environmental adaptability, it can still maintain excellent catalytic performance after 10 cycles, and it exhibited satisfactory remediation performance in simulated water matrix. In addition, the HEF process catalyzed by Cu-N@C also showed satisfactory degradation effect on other organic pollutants including atrazine, methylene blue, and chlorotetracycline. Under the action of impressed current, the HEF system could generate HO in-situ, and the active species could be generated in the redox cycle of Cu/Cu/Cu. Electron paramagnetic resonance and quenching experiments confirmed that •OH was the dominant active species in the degradation of organic compounds. The degradation process of PEF was studied by mass spectrometry analysis of intermediate products. This study provided a simple method to prepare MOF-based electrocatalyst, which exhibits promising application potential for treatment wastewater.
电芬顿(EF)可以原位产生 HO,并有效激活 HO 以产生强大的反应性物质,用于在酸性条件下破坏污染物,然而,含铁污泥的产生和低工作 pH 值的要求显著阻碍了其实际应用。在此,构建了一种以金属有机骨架(MOF)为前驱体的新型 Cu、N 共掺杂碳(Cu-N@C),并将其用于非均相电芬顿(HEF)过程中消除培氟沙星(PEF)。PEF 在 1 h 内几乎完全去除,TOC 去除效率在 6 h 内达到 48.57%。同时,Cu-N@C 具有良好的重复性和环境适应性,经过 10 次循环后仍能保持优异的催化性能,在模拟水基质中表现出令人满意的修复性能。此外,Cu-N@C 催化的 HEF 过程对其他有机污染物(包括莠去津、亚甲基蓝和盐酸四环素)也表现出令人满意的降解效果。在电流作用下,HEF 体系可以原位产生 HO,活性物质可以在 Cu/Cu/Cu 的氧化还原循环中产生。电子顺磁共振和猝灭实验证实,•OH 是有机化合物降解的主要活性物质。通过对中间产物进行质谱分析研究了 PEF 的降解过程。这项研究为制备基于 MOF 的电催化剂提供了一种简单的方法,为处理废水展示了有前景的应用潜力。