The Generation of Carbon/Oxygen Double Defects in FeP/CoP-N-C enhanced by β particles for Photic Driving Degradation of Levofloxacin
The Generation of Carbon/Oxygen Double Defects in FeP/CoP-N-C enhanced by β particles for Photic Driving Degradation of Levofloxacin
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DOI：
10.1016/j.seppur.2022.122186
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发表时间：
2022-09
影响因子：
8.6
通讯作者：
Jing Wang;Juntao Wang;Wen-lei Wang;Xinyu Hu;Yao-Hua Deng;Hui Wang;Yiqiang Wu
中科院分区：
文献类型：
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作者：
Jing Wang;Juntao Wang;Wen-lei Wang;Xinyu Hu;Yao-Hua Deng;Hui Wang;Yiqiang Wu
碳基材料因其特殊的电子结构和优异的催化性能而受到广泛的研究。本文利用Fe和Co的高配位能力，通过吡咯和植酸的聚合反应制备了聚吡咯碳基前驱体，然后通过高温煅烧得到具有三维网状结构的FeP/CoP-N-C-X催化剂，并将其用于左氧氟沙星（LEV）的降解。结果表明，FeP/CoP-N-C-700可在40 min内完全去除LEV。XPS、拉曼光谱和EPR光谱表明FeP/CoP-N-C-700存在典型的碳/氧双缺陷结构。XPS结果表明，FeP/CoP-N-C-700的O元素中氧缺陷的百分比为73.05%。DFT计算结果表明，具有碳/氧双缺陷的FeP/CoP-N-C-700的d带中心为−1.35 eV，而不具有碳/氧双缺陷的FeP/CoP-N-C-700的d带中心为−1.78 eV。结果表明，碳氧双缺陷改变了FeP/CoP-N-C-700的局域电子分布，使其具有较高的n型导电性和电荷分离效率。在每5次光催化循环后，FeP/CoP-N-C-700经电子束辐照，LEV的去除率从81.2%提高到96.32%。XPS、拉曼光谱和EPR光谱表明，电子束辐照可使FeP/CoP-N-C-700中的碳/氧双缺陷再生，从而大大提高催化剂的使用寿命。LC-MS结果表明，FeP/CoP-N-C-700优先解离左氧氟沙星中的哌嗪基，并表现出单一的降解途径，这不仅为材料的再生和循环性能的改善提供了新思路，也为电子束辐照在生物降解领域的应用提供了新的策略.
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 highern-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.