School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China.
School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 401331, China.
J Colloid Interface Sci. 2022 Mar;609:86-101. doi: 10.1016/j.jcis.2021.11.178. Epub 2021 Nov 30.
The toxic metal ions leaching and metal nanoparticles agglomeration were the critical issues for metal-based carbon materials during the peroxymonosulfate (PMS) activation processes. Herein, a facile strategy was first proposed that zero-dimensional Fe/FeC nanoparticles were embedded in one-dimensional N-doped carbon nanofiber (Fe/FeC@NCNF) to solve the above challenges. The as-obtained Fe/FeC@NCNF-800 possessed a low E value (11.7 kJ/mol) and exhibited high activity for activating PMS to degrade tetracycline (TC) in a wide range of pH 3-11. As expected, the iron ions leaching concentration of Fe/FeC@NCNF-800 was very low (0.082 mg/L). Meanwhile, the Fe/FeC@NCNF-800 was easily recovered from the reaction solution due to its magnetic properties. Both superoxide radicals (O) and non-radical of singlet oxygen (O) were the primary reactive oxygen species (ROS) in the Fe/FeC@NCNF-800/PMS system via quenching tests and electron spin resonance spectroscopy (ESR). The catalytic mechanism suggested that the Fe/FeC and graphitic N were the main active sites in the Fe/FeC@NCNF-800 for PMS activation. This work provided a facile method for the preparation of Fe-based carbon materials with high catalytic ability, low metal leaching and easy recycling, showing a broad prospect for environmental applications.
有毒金属离子浸出和金属纳米颗粒团聚是金属基碳材料在过一硫酸盐(PMS)活化过程中面临的关键问题。本文首次提出了一种简便的策略,即将零维的 Fe/FeC 纳米颗粒嵌入一维的氮掺杂碳纳米纤维(Fe/FeC@NCNF)中,以解决上述挑战。所获得的 Fe/FeC@NCNF-800 具有较低的 E 值(11.7 kJ/mol),并在很宽的 pH 值 3-11 范围内表现出高活性,可用于活化 PMS 降解四环素(TC)。不出所料,Fe/FeC@NCNF-800 的铁离子浸出浓度非常低(0.082 mg/L)。同时,由于其磁性,Fe/FeC@NCNF-800 很容易从反应溶液中回收。通过淬灭实验和电子顺磁共振波谱(ESR),Fe/FeC@NCNF-800/PMS 体系中的主要活性氧物质(ROS)为超氧自由基(O)和单重态氧的非自由基(O)。催化机理表明,Fe/FeC 和石墨 N 是 Fe/FeC@NCNF-800 中 PMS 活化的主要活性位点。这项工作为制备具有高催化能力、低金属浸出和易于回收的 Fe 基碳材料提供了一种简便的方法,为环境应用展示了广阔的前景。