Key Laboratory of Groundwater Resources and Environment, Ministry of Education, Jilin University, Changchun, 130021, Jilin, China; Jilin Provincial Key Laboratory of Water Resources and Environment, Jilin University, Changchun, 130021, Jilin, China.
Engineering Lab for Water Pollution Control and Resources Recovery of Jilin Province, School of Environment, Northeast Normal University, Changchun, 130117, China.
Environ Res. 2022 Sep;212(Pt C):113399. doi: 10.1016/j.envres.2022.113399. Epub 2022 May 10.
Heterogeneous photo-Fenton technology has drawn tremendous attention for removal of recalcitrant pollutants. Fe-based metal-organic frameworks (Fe-MOFs) are regarded to be superior candidates in wastewater treatment technology. However, the central metal sites of the MOFs are coordinated with the linkers, which reduces active site exposure and decelerates HO activation. In this study, a series of 2, 5-dioxido-1, 4-benzenedicarboxylate (HDOBDC)-functionalized MIL-100(Fe) with enhanced degradation performance was successfully constructed via solvothermal strategy. The modified MIL-100(Fe) displayed an improvement in photo-Fenton behaviors. The photocatalytic rate constant of optimized MIL-100(Fe)-1/2/3 are 2.3, 3.6 and 4.4 times higher compared with the original MIL-100(Fe). The introduced HDOBDC accelerates the separation and transfer in photo-induced charges and promotes Fe(II)/Fe(III) cycle, thus improving the performance. •OH and •O are main reactive radicals in tetracycline (TCH) degradation. Dealkylation, hydroxylation, dehydration and dealdehyding are the main pathways for TCH degradation.
非均相光芬顿技术因其对难降解污染物的去除效果而备受关注。基于铁的金属有机骨架（Fe-MOFs）被认为是废水处理技术中的优秀候选材料。然而，MOFs 的中心金属位点与配体配位，这降低了活性位点的暴露，减缓了 HO 的活化。在这项研究中，通过溶剂热策略成功构建了一系列具有增强降解性能的 2,5-二氧代-1,4-苯二甲酸酯（HDOBDC）功能化 MIL-100(Fe)。改性后的 MIL-100(Fe)表现出更好的光芬顿行为。与原始 MIL-100(Fe)相比，优化后的 MIL-100(Fe)-1/2/3 的光催化速率常数分别提高了 2.3、3.6 和 4.4 倍。引入的 HDOBDC 加速了光生载流子的分离和转移，并促进了 Fe(II)/Fe(III)循环，从而提高了性能。•OH 和•O 是四环素（TCH）降解中的主要活性自由基。TCH 降解的主要途径是脱烷基化、羟化、脱水和脱醛。
