School of Environment and Energy, South China University of Technology, Guangzhou 510006, China.
School of Environment and Energy, South China University of Technology, Guangzhou 510006, China.
J Hazard Mater. 2022 Feb 15;424(Pt A):127380. doi: 10.1016/j.jhazmat.2021.127380. Epub 2021 Sep 30.
Developing high-efficient catalysts is crucial for activating peroxymonosulfate (PMS). Fe-N-C catalysts exhibit excellent performance for PMS activation because of the contribution of doped N, Fe-Nx and FeC sites. In our work, a series of Fe-N-C catalysts with high-performance was obtained by pyrolyzing Fe-Zn-MOFs precursors. During pyrolysis process, the change of chemical bonds and formation of active sites in the precursor were elucidated by characterization analysis and related catalytic experiments. Graphitic N, Fe-Nx and FeC were confirmed to activate PMS synergistically for ciprofloxacin (CIP) degradation. Besides, the catalytic performance was proportional to the amount of doped iron and calcination temperature. Moreover, the Fe-N-C-3-800/PMS system not only displayed good recycling performance, but also had high anti-interference ability. Integrated with quenching and electron paramagnetic resonance (EPR) experiments, a non-radical pathway dominated by O was proposed. Furthermore, PMS could bond to Fe-N-C-3-800 to form intermediate for charge transfer, thus accelerate electron transfer between CIP and PMS to realize degradation of CIP. Six main pathways of CIP degradation were proposed, which include bond fission of N-C on piperazine ring and direct oxidation of CIP. This study provided a new idea for the design of heterogeneous carbon catalysts in advanced oxidation field.
开发高效催化剂对于激活过一硫酸盐(PMS)至关重要。由于掺杂 N、Fe-Nx 和 FeC 位点的贡献,Fe-N-C 催化剂在 PMS 激活方面表现出优异的性能。在我们的工作中,通过热解 Fe-Zn-MOFs 前体制备了一系列具有高性能的 Fe-N-C 催化剂。在热解过程中,通过表征分析和相关催化实验阐明了前驱体中化学键的变化和活性位的形成。证实石墨 N、Fe-Nx 和 FeC 协同激活 PMS 以降解环丙沙星(CIP)。此外,催化性能与掺杂铁的量和煅烧温度成正比。此外,Fe-N-C-3-800/PMS 体系不仅表现出良好的循环性能,而且具有很强的抗干扰能力。通过淬灭和电子顺磁共振(EPR)实验相结合,提出了一种以 O 为主的非自由基途径。此外,PMS 可以与 Fe-N-C-3-800 键合形成中间体以进行电荷转移,从而加速 CIP 和 PMS 之间的电子转移,实现 CIP 的降解。提出了 CIP 降解的 6 条主要途径,包括哌嗪环上 N-C 键的断裂和 CIP 的直接氧化。本研究为高级氧化领域中异相碳催化剂的设计提供了新的思路。