Guangxi Key Laboratory of Clean Pulp & Papermaking and Pollution Control, School of Light Industrial and Food Engineering, Guangxi University, Nanning 530004, China.
Guangxi Bossco Environmental Protection Technology Co., Ltd., Nanning 530007, China.
Chemosphere. 2024 Aug;361:142518. doi: 10.1016/j.chemosphere.2024.142518. Epub 2024 Jun 1.
Fe-based metal-organic frameworks (MOFs) have good photocatalytic performance, environmental friendliness, low cost, and abundance. However, their applications are limited by low water stability, particularly in the presence of light irradiation and oxidizing agents. In this study, we present a MIL-53(Fe)-based MOF using 1,4-naphthalene dicarboxylic (1,4-NDC) and 1,4-benzenedicarboxylic (HBDC) acid co-ligands, denoted MIL-53(Fe)-N, where N represents the ratio of 1,4-NDC. This MOF exhibits high water stability and good photocatalytic activity because of the hydrophobicity of naphthalene. The removal and mineralization rates for 100 mg/L 2,4-dichlorophenol reached 100% and 22%, respectively, within 60 min. After three cycles of use, the Fe leached into the solution from the catalysts was significantly lower than the maximum permissible limit indicated in the European Union standard. Of note, 1,4-NDC can be used to make a rigid MOF, thereby improving the crystallinity, porosity, and hydrophobicity of the resultant materials. It also significantly reduced the bandgap energy and improved the charge separation efficiency of the catalysts. This study provides a route to enhance the water stability of Fe-based MOFs via a mixed-ligand strategy to expand their applications in pollutant control.
基于铁的金属-有机骨架(MOFs)具有良好的光催化性能、环境友好性、低成本和丰富的资源。然而,它们的应用受到低水稳定性的限制,特别是在存在光照射和氧化剂的情况下。在这项研究中,我们提出了一种使用 1,4-萘二甲酸(1,4-NDC)和 1,4-苯二甲酸(HBDC)酸共配体的 MIL-53(Fe)-基 MOF,记为 MIL-53(Fe)-N,其中 N 代表 1,4-NDC 的比例。由于萘的疏水性,这种 MOF 表现出高的水稳定性和良好的光催化活性。对于 100mg/L 的 2,4-二氯苯酚,在 60 分钟内,去除率和矿化率分别达到 100%和 22%。在使用三个循环后,从催化剂中浸出到溶液中的铁明显低于欧盟标准规定的最大允许限度。值得注意的是,1,4-NDC 可用于制备刚性 MOF,从而提高所得材料的结晶度、孔隙率和疏水性。它还显著降低了催化剂的能带隙能量,提高了电荷分离效率。本研究通过混合配体策略提供了一种提高基于铁的 MOFs 水稳定性的途径,以扩大其在污染物控制中的应用。