Chen Hai, Wang Jianlong
Collaborative Innovation Center for Advanced Nuclear Energy Technology, INET, Tsinghua University, Beijing 100084, China.
Collaborative Innovation Center for Advanced Nuclear Energy Technology, INET, Tsinghua University, Beijing 100084, China; Beijing Key Laboratory of Radioactive Waste Treatment, Tsinghua University, Beijing 100084, China.
J Hazard Mater. 2021 Feb 5;403:123697. doi: 10.1016/j.jhazmat.2020.123697. Epub 2020 Aug 15.
Metal-organic frameworks (MOFs) ZIF-67-derived CoO-C@FeOOH composite was prepared, characterized and used as an efficinet catalyst for ozonation of norfloxacin (NOF). Results showed that ZIF-67-derived CoO-C composite maintained the polyhedral structure of ZIF-67. After modification, abundant amorphous FeOOH nanowire attached on the surface of CoO-C composite, resulting in CoO-C@FeOOH interwoven polyhedrons. Furthermore, the specific surface area of the formed composite was about 2.5 times that of CoO-C composite, which might provide more active sites for catalytic reaction. Compared with single ozonation system, the catalytic ozonation process (CoO-C@FeOOH/O) had better performance in NOF mineralization under the same operating conditions. Moreover, in the presence of CoO-C@FeOOH, faster O decomposition and higher •OH concentration were observed, which could explain the significant enhancement of TOC removal. The co-existence of Fe and Co in various valence states in catalyst might improve the conversion of Co(III)/Co(II) and Fe(III)/Fe(II), which would increase the catalytic activity in catalytic ozonation process. Besides, several main intermediate products were detected and possible NOF degradation pathway was proposed.
制备了金属有机框架（MOFs）ZIF-67衍生的CoO-C@FeOOH复合材料，对其进行了表征，并将其用作诺氟沙星（NOF）臭氧化的高效催化剂。结果表明，ZIF-67衍生的CoO-C复合材料保持了ZIF-67的多面体结构。改性后，大量无定形FeOOH纳米线附着在CoO-C复合材料表面，形成了CoO-C@FeOOH交织多面体。此外，所形成复合材料的比表面积约为CoO-C复合材料的2.5倍，这可能为催化反应提供更多活性位点。与单一臭氧化体系相比，在相同操作条件下，催化臭氧化过程（CoO-C@FeOOH/O）在NOF矿化方面具有更好的性能。此外，在CoO-C@FeOOH存在下，观察到更快的O分解和更高的•OH浓度，这可以解释TOC去除率的显著提高。催化剂中不同价态的Fe和Co共存可能会提高Co(III)/Co(II)和Fe(III)/Fe(II)的转化率，从而提高催化臭氧化过程中的催化活性。此外，检测到了几种主要中间产物，并提出了可能的NOF降解途径。
