Institute of Environmental Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou, 310058, China.
College of Environmental Science and Engineering, Donghua University, Shanghai, 201620, China.
Environ Sci Pollut Res Int. 2018 Dec;25(34):34190-34199. doi: 10.1007/s11356-018-3323-1. Epub 2018 Oct 4.
Persulfates are recognized as promising oxidants and an alternative to Fenton reaction for water treatment. However, activation methods in hand restrict the practical application. Herein, we explore the possibility of Fe-N complexes being a catalyst for persulfate activation for the first time. The catalyst denoted as Fe-Im-SBA was synthesized from ferric chloride, imidazole, and SBA-15 at high temperature. The internal pore structure of Fe-Im-SBA was maintained well; Fe, N and C elements are evenly distributed on the catalyst. This catalyst presents an extraordinarily catalytic activity for Rh B removal by PMS activation with a removal rate of Rh B that reached up to 97.0% in the first 5 min. It also performed well in a wide pH range with complete removal of Rh B in pH ranged from 0.5 to 10, suggesting the stability of this catalyst in both acidic and alkaline conditions. It also showed high adaptability to degrade different kinds of pollutants, which could give an attractive advantage of Fe-Im-SBA for environmental implications. Through X-ray absorption spectroscopies analysis, it shows that the active sites of Fe-Im-SBA are composed of Fe-N sites and Fe-N sites. O were proved to generate in the Fe-Im-SBA/PMS system and serve as the major ROS. Meanwhile, graphitic carbon can accelerate the transfer of electrons, which may also be the reason for its high catalytic performance.
过硫酸盐被认为是一种很有前途的氧化剂，是替代芬顿反应的水处理方法。然而，现有的活化方法限制了其实际应用。本文首次探索了 Fe-N 配合物作为过硫酸盐活化催化剂的可能性。该催化剂被命名为 Fe-Im-SBA，是由三氯化铁、咪唑和 SBA-15 在高温下合成的。Fe-Im-SBA 保持了良好的内部孔结构；Fe、N 和 C 元素均匀分布在催化剂上。该催化剂对 PMS 活化罗丹明 B 的去除具有极高的催化活性，在最初的 5 分钟内罗丹明 B 的去除率达到 97.0%。它在很宽的 pH 范围内都表现出良好的性能，在 pH 为 0.5 到 10 之间可完全去除罗丹明 B，这表明该催化剂在酸性和碱性条件下都具有稳定性。它还表现出对不同种类污染物的高适应性，这为 Fe-Im-SBA 在环境方面的应用提供了有吸引力的优势。通过 X 射线吸收光谱分析，表明 Fe-Im-SBA 的活性位点由 Fe-N 位和 Fe-N-O 位组成。在 Fe-Im-SBA/PMS 体系中证明生成了含氧的 Fe-N-O 位，并作为主要的 ROS。同时，石墨碳可以加速电子转移，这也可能是其具有高催化性能的原因。
