Laboratori d'Electroquímica dels Materials i del Medi Ambient, Departament de Química Física, Facultat de Química, Universitat de Barcelona, Martí i Franquès 1-11, 08028, Barcelona, Spain; Barrer Centre, Department of Chemical Engineering, Imperial College London, South Kensington Campus, London, SW7 2AZ, UK.
Barrer Centre, Department of Chemical Engineering, Imperial College London, South Kensington Campus, London, SW7 2AZ, UK.
Water Res. 2020 Oct 1;184:115986. doi: 10.1016/j.watres.2020.115986. Epub 2020 Jul 10.
This work reports the novel application of an Fe-based 2D metal-organic framework (MOF), prepared with 2,2'-bipyridine-5,5'-dicarboxylate (bpydc) as organic linker, as highly active catalyst for heterogeneous photoelectro-Fenton (PEF) treatment of the lipid regulator bezafibrate in a model matrix and urban wastewater. Well-dispersed 2D structures were successfully synthesized and their morphological, physicochemical and photocatalytic properties were assessed. UV/Vis PEF using an IrO/air-diffusion cell with an extremely low catalyst concentration (0.05 g L, tenfold lower than reported 3D MOFs) outperformed electro-oxidation with electrogenerated HO, electro-Fenton and visible-light PEF. Its excellent performance was explained by: (i) the enhanced mass transport of HO (and organic molecules) at the 2D structure, providing active sites for heterogeneous Fenton's reaction and in-situ Fe(II) regeneration; (ii) the ability of photoinduced electrons to reduce HO to OH, and Fe(III) to Fe(II); and (iii) the enhanced charge transfer and excitation of Fe-O clusters, which increased the number of electron-hole pairs. LC-QToF-MS and GC-MS allowed the identification of 16 aromatic products of bezafibrate. The complete removal of four micropollutants mixed in urban wastewater at pH 7.4 revealed the great potential of (Fe-bpydc)-catalyzed PEF process.
这项工作报道了一种新型的基于铁的二维金属有机骨架(MOF)的应用,该 MOF 以 2,2'-联吡啶-5,5'-二甲酸(bpydc)为有机配体,作为非均相光电芬顿(PEF)处理模型基质和城市废水中脂质调节剂苯扎贝特的高效催化剂。成功合成了分散良好的二维结构,并对其形态、物理化学和光催化性能进行了评估。使用 IrO/空气扩散池的紫外/可见 PEF,催化剂浓度极低(0.05 g/L,比报道的 3D MOFs 低十倍),优于电生成 HO 的电氧化、电芬顿和可见光 PEF。其优异的性能可以通过以下几个方面来解释:(i)在二维结构中增强了 HO(和有机分子)的传质,为非均相芬顿反应和原位 Fe(II)再生提供了活性位点;(ii)光诱导电子将 HO 还原为 OH 和 Fe(III)还原为 Fe(II)的能力;(iii)增强了 Fe-O 簇的电荷转移和激发,增加了电子-空穴对的数量。LC-QToF-MS 和 GC-MS 允许鉴定苯扎贝特的 16 种芳香产物。在 pH 7.4 的城市废水中混合去除四种微量污染物,显示了(Fe-bpydc)催化的 PEF 过程的巨大潜力。