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The generation of carbon/oxygen double defects in FeP/CoP-N-C enhanced by β particles for photic driving degradation of levofloxacin

X射线光电子能谱 氧气 拉曼光谱 碳纤维 电子顺磁共振 催化作用 化学 煅烧 化学工程 分析化学(期刊) 材料科学 有机化学 工程类 核磁共振 复合材料 复合数 物理 光学
作者
Jing Wang,Juntao Wang,Wenlei Wang,Xinyu Hu,Yao Deng,Hui Wang,Yiqiang Wu
出处
期刊:Separation and Purification Technology [Elsevier BV]
卷期号:303: 122186-122186 被引量:13
标识
DOI:10.1016/j.seppur.2022.122186
摘要

• 1. A precursor was prepared by the polymerization of pyrrole and phytic acid with Fe and Co. • 2. FeP/CoP-N-C rich in carbon/oxygen double defects was prepared by a calcination method. • 3. Carbon/oxygen double defects improve the conductivity and charge separation efficiency. • 4. FeP/CoP-N-C preferentially dissociates the piperazine group in levofloxacin. • 5. Carbon/oxygen double defects in FeP/CoP-N-C were regenerated by electron beam irradiation. Carbon-based materials have been widely studied for their special electronic structure and excellent catalytic performance. In this work, polypyrrole carbon-based precursors were prepared by the polymerization of pyrrole and phytic acid with the high coordination ability of Fe and Co. Then, an FeP/CoP-N-C-X catalyst with a three-dimensional net][work structure was obtained by high-temperature calcination, which was used for the degradation of levofloxacin (LEV). The obtained results showed that FeP/CoP-N-C-700 could completely remove LEV within 40 min. XPS, Raman spectroscopy and EPR spectroscopy demonstrated the existence of a typical carbon/oxygen double-defect structure in FeP/CoP-N-C-700. XPS results shows that the percentage of oxygen defects in the O element of FeP/CoP-N-C-700 was 73.05%. DFT calculation results shows that the d-band center of FeP/CoP-N-C-700 with carbon/oxygen double defect was -1.35 eV , while that of FeP/CoP-N-C-700 without carbon/oxygen double defect was -1.78 eV. These results indicates that the carbon/oxygen double defects could change the distribution of local electrons in FeP/CoP-N-C-700, which made it exhibit higher n-type conductivity and charge separation efficiency. After each five photocatalytic cycles, FeP/CoP-N-C-700 was treated by electron beam irradiation, and the removal rate of LEV increased from 81.2% to 96.32%. XPS, Raman spectroscopy and EPR spectroscopy demonstrate that carbon/oxygen double defects in FeP/CoP-N-C-700 can be regenerated by electron beam irradiation, which could greatly improve the service life of the catalyst.. Furthermore, LC-MS results indicates that FeP/CoP-N-C-700 preferentially dissociates the piperazinyl group in levofloxacin and exhibits a single degradation pathway for it. This work not only provides a new idea for the regeneration of materials and the improvement of cycle performance, but also provides a new strategy for the application of electron beam irradiation in the field of photocatalysis.
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