Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin, China.
State Key Lab Urban Water Resource and Environment, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, China.
J Colloid Interface Sci. 2022 Nov;625:774-784. doi: 10.1016/j.jcis.2022.06.065. Epub 2022 Jun 23.
Peroxymonosulfate (PMS)-based Fenton-like reaction is an effective technique for the pollutant degradation, and the Co-based metal organic frameworks displayed the excellent activity for the PMS activation. Nevertheless, how to further improve the catalytic activity, suppress the leaching of toxic cobalt ions, and realize the rapid separation were still challenges for practical application. In this work, a novel solution was proposed: encapsulating FeO and Prussian blue analogue (PBA) into the polypyrrole (PPy) shell and constructing a "double-yolk egg-like" FeO/PBA@PPy as a nanoreactor. In FeO/PBA@PPy-10, the catalytic performance was remarkably enhanced with the help of confinement effect, and the degradation rate (0.38 L·min·mol) was 5.1 times than that of reference FeO/PBA-10 (0.074 L·min·mol). In addition, the concentration of leached cobalt ions was reduced to only 0.174 mg/L by the protective function from the PPy shell. Moreover, the nanoreactor could be magnetically separated from the reaction solution due to the encapsulation of FeO nanospheres, and 84.5% of activity still preserved after the 4th cycle. The main active species involved in FeO/PBA@PPy-10 system was O, while that in reference FeO/PBA-10 system was OH. Electron spin resonance analysis and radical trapping experiment revealed that the different catalytic mechanisms were attributed to the confinement effect inside the hollow cavity. This work not only presents a feasible way to prepare rarely-reported double-yolk egg-like nanoreactor, but also provides a new insight to solve the bottlenecks in Fenton-like reaction.
过一硫酸盐(PMS)基类 Fenton 反应是一种有效的污染物降解技术,而基于钴的金属有机骨架显示出对 PMS 活化的优异活性。然而,如何进一步提高催化活性、抑制有毒钴离子的浸出以及实现快速分离仍然是实际应用中的挑战。在这项工作中,提出了一种新的解决方案:将 FeO 和普鲁士蓝类似物(PBA)封装在聚吡咯(PPy)壳中,并构建一种“双蛋黄样”FeO/PBA@PPy 作为纳米反应器。在 FeO/PBA@PPy-10 中,借助限域效应,催化性能得到显著提高,降解速率(0.38 L·min·mol)是参考 FeO/PBA-10(0.074 L·min·mol)的 5.1 倍。此外,通过 PPy 壳的保护作用,浸出钴离子的浓度降低到仅 0.174 mg/L。此外,由于 FeO 纳米球的封装,纳米反应器可以从反应溶液中磁性分离,并且在第 4 次循环后仍保留 84.5%的活性。FeO/PBA@PPy-10 体系中的主要活性物质是 O,而参考 FeO/PBA-10 体系中的主要活性物质是 OH。电子顺磁共振分析和自由基捕获实验表明,不同的催化机制归因于空心腔体内的限域效应。这项工作不仅提出了一种可行的方法来制备很少报道的双蛋黄样纳米反应器,而且为解决类 Fenton 反应中的瓶颈问题提供了新的见解。