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
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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