State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials, School of Resources, Environment and Materials, Guangxi University, Nanning, 530004, China.
School of Nuclear Science and Technology, University of South China, 28 Changsheng West Road, Hengyang, 421001, China.
Chemosphere. 2024 Aug;362:142676. doi: 10.1016/j.chemosphere.2024.142676. Epub 2024 Jun 25.
A MOF-on-MOF composite derivative material named ZIF-67@Ce-MOF-600 was designed and synthesized. The preparation of ZIF-67@Ce-MOF-600 was optimized from the aspects of the ratio of metal and ligand, heat-treatment temperature. It was demonstrated by XRD, FT-IR, SEM-EDS and TEM. The optimum conditions for the activation of PMS by ZIF-67@Ce-MOF-600 for the degradation of tetracycline (TC) were investigated by adjusting the catalyst dosage, TC, pH, peoxymonosulfate (PMS) concentration, and different kinds of water, co-existing anions and pollution. Under optimal conditions (20 mg catalysts and 50 mg PMS added) in 100 mL of tetracyclines (TC) solvent (20 mg TC/L), the removal rate could reach up to 99.2% and after five cycles was 70.5%. The EPR results indicated the presence of free radicals and non-free radical, among which free radicals intended to play a major role in the degradation process. Its possible degradation pathways and attack sites were analyzed by liquid-phase mass spectrometry and DFT analysis.
设计并合成了一种名为 ZIF-67@Ce-MOF-600 的 MOF-on-MOF 复合衍生材料。从金属和配体的比例、热处理温度等方面优化了 ZIF-67@Ce-MOF-600 的制备。通过 XRD、FT-IR、SEM-EDS 和 TEM 进行了证明。通过调整催化剂用量、TC、pH 值、过一硫酸盐（PMS）浓度以及不同种类的水、共存阴离子和污染物，研究了 ZIF-67@Ce-MOF-600 活化 PMS 降解四环素（TC）的最佳条件。在最佳条件下（加入 20mg 催化剂和 50mg PMS），在 100mL TC 溶剂（20mg TC/L）中，去除率可达 99.2%，经过 5 次循环后，去除率可达 70.5%。EPR 结果表明存在自由基和非自由基，其中自由基在降解过程中起主要作用。通过液相质谱和 DFT 分析分析了其可能的降解途径和攻击位点。
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