Tao Xumei, Yuan Xinjie, Huang Liang, Shang Shuyong, Xu Dongyan
State Key Laboratory Base for Eco-Chemical Engineering, College of Chemical Engineering, Qingdao University of Science and Technology Qingdao 266042 Shandong China
College of Electromechanical Engineering, Qingdao University of Science and Technology Qingdao 266042 Shandong China.
RSC Adv. 2020 Oct 2;10(60):36363-36370. doi: 10.1039/d0ra07402k. eCollection 2020 Oct 1.
Fe-based metal organic frameworks (Fe-MOFs) were successfully synthesized with the dielectric barrier discharge (DBD) plasma method and FeSO·7HO as the Fe precursor. Fe-MOFs were used as Fenton-like catalysts in DBD plasma/Fenton-like technology to treat wastewater, which addressed the issues with iron solubility. Since the valence state of iron will affect the catalytic performance, the Fe precursor FeSO·7HO was added to regulate the valence state and adjust the catalytic performance by improving the availability of active sites. The influences of discharge voltage, catalyst addition amount, HO addition amount and pH on the degradation efficiency of methyl orange (MO) were systematically examined. Through free radical capture experiments, the reaction mechanism of the plasma/Fenton-like catalytic degradation process was deduced primarily as the coordinated oxidation process of hydroxyl radicals (·OH), photo-generated holes (h) and superoxide radicals (·O ). The reusability experiments proved that the catalyst was stable and reusable. The possible degradation pathways were proposed based on the identification of intermediate products generated in the degradation process by liquid chromatography-mass spectrometry (LC-MS) analyses.
以硫酸亚铁七水合物(FeSO₄·7H₂O)为铁源前驱体,采用介质阻挡放电(DBD)等离子体法成功合成了铁基金属有机框架材料(Fe-MOFs)。Fe-MOFs被用作DBD等离子体/类芬顿技术中的类芬顿催化剂来处理废水,解决了铁溶解性的问题。由于铁的价态会影响催化性能,因此添加铁源前驱体FeSO₄·7H₂O来调节价态,并通过提高活性位点的可用性来调整催化性能。系统研究了放电电压、催化剂添加量、过氧化氢添加量和pH值对甲基橙(MO)降解效率的影响。通过自由基捕获实验,初步推断等离子体/类芬顿催化降解过程的反应机理为羟基自由基(·OH)、光生空穴(h⁺)和超氧自由基(·O₂⁻)的协同氧化过程。可重复使用性实验证明该催化剂稳定且可重复使用。基于液相色谱-质谱联用(LC-MS)分析对降解过程中产生的中间产物进行鉴定,提出了可能的降解途径。