This work reports the solvothermal synthesis of UiO-66-based MOFs with three different ligands and its application to the breakdown of aqueous acetaminophen under simulated sunlight. This pharmaceutical is a representative contaminant of emerging concern that enters water bodies mainly through wastewater treatment plant discharges. The synthesis approach of the MOFs was fitted using a zirconium alkoxide as metal cluster precursor and 2-aminoterephthalic and 2,5-dihydroxyterephthalic acids as ligands to prepare UiO-66-NH₂ and UiO-66-(OH)₂ MOFs, respectively. These new MOFs have enhanced visible light harvesting and narrower band gap than the UiO-66. Among all, UiO-66-NH₂ yielded the highest removal of acetaminophen under simulated solar irradiation in batch test. The activity and stability of UiO-66-NH₂ were demonstrated for the first time in a continuous flow test, where stable performance was observed upon 30-h on stream. The degradation pathway of acetaminophen was elucidated based on coupling, ring-opening, and oxidation reactions. DFT calculation confirmed that the indirect semiconductor behavior of UiO-66-NH₂ upon light excitation occurred through ligand-ligand charge transfer. Overall, promising UiO-66-based MOFs photocatalysts were obtained for effective degradation of acetaminophen with the assistance of solar light.

这项工作报告了具有三种不同配体的基于 UiO-66 的 MOF 的溶剂热合成及其在模拟阳光下分解水性对乙酰氨基酚的应用。这种药物是一种新出现的具有代表性的污染物，主要通过废水处理厂排放进入水体。MOFs 的合成方法是使用锆醇盐作为金属簇前体和 2-氨基对苯二甲酸和 2,5-二羟基对苯二甲酸作为配体，分别制备 UiO-66-NH ₂和 UiO-66-(OH) ₂ MOFs。这些新的 MOF 比 UiO-66 具有增强的可见光捕获和更窄的带隙。其中，UiO-66-NH ₂在批量测试中模拟太阳辐射下产生最高的对乙酰氨基酚去除率。UiO-66-NH ₂的活性和稳定性首次在连续流动测试中得到证明，在运行 30 小时后观察到稳定的性能。基于偶联、开环和氧化反应阐明了对乙酰氨基酚的降解途径。DFT 计算证实，UiO-66-NH ₂在光激发下的间接半导体行为是通过配体-配体电荷转移发生的。总体而言，获得了有前景的基于 UiO-66 的 MOF 光催化剂，可在太阳光的帮助下有效降解对乙酰氨基酚。