Department of Chemistry and Chemical Engineering, Jining University, Qufu 273100, PR China.
Dalton Trans. 2019 Mar 5;48(10):3476-3485. doi: 10.1039/c8dt04269a.
Herein, a novel Ce3+ self-doped CeOx/FeOCl composite was successfully prepared by a facile method for the first time, which showed remarkable catalytic activity as a Fenton catalyst in the degradation of phenol under the conditions of a neutral solution, room temperature and natural light. In CeOx/FeOCl, 5.23% CeOx is the optimal condition, and the degradation constant (k) of CeOx/FeOCl is greater than that of FeOCl by a factor of 10.8. CeOCl in the composite plays a more important role than CeO2, which greatly increases the production of ˙OH radicals. Furthermore, the Ce-doping in FeOCl accelerates the separation efficiency of the photogenerated electron-hole pairs. The increased surface area and surface potential of CeOx/FeOCl than those of FeOCl effectively promote the adsorption of phenol, which is 4.05 times that of FeOCl. According to the DFT calculations, the Ce-doping in FeOCl enhances the structural stability by increasing the strength of the chemical bonds. The adsorption of H2O2 with Ce3+ is energetically favorable, which promotes the production of ˙OH radicals. A synergistic mechanism for the enhanced catalytic performance of CeOx/FeOCl is proposed.
本文首次通过一种简便的方法成功制备了一种新型的 Ce3+自掺杂 CeOx/FeOCl 复合材料，该复合材料作为芬顿催化剂在中性溶液、室温及自然光条件下对苯酚的降解表现出显著的催化活性。在 CeOx/FeOCl 中，CeOx 的最佳掺杂量为 5.23%，CeOx/FeOCl 的降解常数（k）是 FeOCl 的 10.8 倍。复合材料中的 CeOCl 比 CeO2 发挥更重要的作用，大大增加了˙OH 自由基的生成。此外，Ce 掺杂在 FeOCl 中加速了光生电子-空穴对的分离效率。CeOx/FeOCl 的比表面积和表面电势均高于 FeOCl，有效促进了苯酚的吸附，其吸附量是 FeOCl 的 4.05 倍。根据 DFT 计算，Ce 掺杂在 FeOCl 中通过增加化学键的强度来增强结构稳定性。Ce3+与 H2O2 的吸附是能量有利的，这促进了˙OH 自由基的生成。提出了 CeOx/FeOCl 增强催化性能的协同机制。
