College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.
Hunan Modern Environmental Technology Co. Ltd, Changsha 410004, PR China.
J Hazard Mater. 2022 Feb 15;424(Pt C):127503. doi: 10.1016/j.jhazmat.2021.127503. Epub 2021 Oct 14.
The application of traditional powder catalysts is limited by particle agglomeration and difficult recovery. In this work, a three-dimensional porous aerogel catalyst for organic pollutants degradation in water by activating peroxydisulfate (PDS) was successfully synthesized, which was obtained via directly mixing of MIL-88B(Fe) with sol precursors followed by vacuum freeze-drying and low-temperature calcination. MIL-88B(Fe)/gelatin aerogel-150/PDS (MGA-150/PDS) system displayed satisfactory norfloxacin (NOR) degradation performance, which could remove 98.7% of NOR in 90 min. Its reaction rate constant was 23.2 times higher than the gelatin aerogel/PDS (GA/PDS) system. In addition, Electron paramagnetic resonance (EPR) results and radical trapping experiments revealed both radicals (SO, •OH) and non-radical (O) pathways had participated in NOR degradation, of which •OH was dominant. Possible degradation pathways were proposed. Moreover, the high degradation efficiency of NOR by MGA-150 composites could still be reached more than 90.0% even after 10 cycles, and the morphology and chemical structure of MGA-150 composites exhibited no significant changes, indicating the arrestive stability of aerogel composites. This progress not only proposed an effective catalyst for PDS activation, but also expanded views for the design and development of 3D functional materials.
传统粉末催化剂的应用受到颗粒团聚和难以回收的限制。在这项工作中,通过直接混合 MIL-88B(Fe)与溶胶前体,然后进行真空冷冻干燥和低温煅烧,成功合成了一种用于水相激活过二硫酸盐(PDS)降解有机污染物的三维多孔气凝胶催化剂。MIL-88B(Fe)/明胶气凝胶-150/PDS(MGA-150/PDS)体系对诺氟沙星(NOR)的降解表现出令人满意的性能,在 90 分钟内可去除 98.7%的 NOR。其反应速率常数是明胶气凝胶/PDS(GA/PDS)体系的 23.2 倍。此外,电子顺磁共振(EPR)结果和自由基捕获实验表明,NOR 的降解途径既有自由基(SO、•OH)也有非自由基(O)途径,其中•OH 是主要途径。提出了可能的降解途径。此外,即使经过 10 次循环,MGA-150 复合材料对 NOR 的高降解效率仍能达到 90.0%以上,而且 MGA-150 复合材料的形貌和化学结构没有明显变化,表明气凝胶复合材料具有良好的稳定性。这一进展不仅为 PDS 激活提出了一种有效的催化剂,也为 3D 功能材料的设计和开发提供了新的思路。