Laboratory of Environmental Technology, INET, Tsinghua University, Beijing, 100084, PR China.
Laboratory of Environmental Technology, INET, Tsinghua University, Beijing, 100084, PR China; Beijing Key Laboratory of Radioactive Waste Treatment, INET, Tsinghua University, Beijing, 100084, PR China.
Chemosphere. 2021 Oct;281:130997. doi: 10.1016/j.chemosphere.2021.130997. Epub 2021 May 26.
The development of defective structure in MOFs can offer a novel approach to tailor the properties of MOFs-type adsorbent for better adsorption performance. In this study, the contribution of defective structure in UiO-66 to the adsorptive removal of pharmaceutical pollutants from aqueous solution was investigated. The results showed that the controlled defects in UiO-66 greatly affected adsorption equilibrium time, adsorption capacity and adsorption selectivity. Slightly defected UiO-66 contained more open frameworks, and it exhibited faster adsorption equilibrium. However, a high degree of destruction to the amorphous state resulted in a longer equilibrium time, due to the interference in the diffusion process as the result of severe structural collapse and interpenetration. Moreover, a higher degree of structural damage of UiO-66 led to a higher adsorption capacity because of the increased active sites. The maximum adsorption capacity was 321 mg/g for the as-prepared defective UiO-66, which was much higher than that of perfective UiO-66 (54.5 mg/g). Furthermore, defective UiO-66 had a higher adsorption affinity for diclofenac sodium than other studied pharmaceutical pollutants. This study could provide insight into the relationship between defective property and adsorption performance. The results will deepen the understanding of the adsorption mechanism of MOFs-type adsorbents, and help the design of MOFs-type adsorbents with fast adsorption equilibrium, higher adsorption capacity and adsorption selectivity.
缺陷结构的发展为调整 MOF 型吸附剂的性能以实现更好的吸附性能提供了一种新方法。本研究考察了缺陷结构对 UiO-66 型吸附剂从水溶液中吸附去除药物污染物的贡献。结果表明,UiO-66 中的受控缺陷极大地影响了吸附平衡时间、吸附容量和吸附选择性。略有缺陷的 UiO-66 含有更多的开放骨架,因此表现出更快的吸附平衡。然而,由于严重的结构崩塌和互穿,扩散过程受到干扰,无定形状态的高度破坏导致平衡时间延长。此外,UiO-66 的结构损伤程度越高,由于活性位点增加,吸附容量越高。所制备的缺陷 UiO-66 的最大吸附容量为 321mg/g,明显高于完美 UiO-66(54.5mg/g)。此外,缺陷 UiO-66 对二氯芬酸钠的吸附亲和力高于其他研究的药物污染物。本研究可以深入了解缺陷性质与吸附性能之间的关系。研究结果将加深对 MOF 型吸附剂吸附机制的理解,并有助于设计具有快速吸附平衡、更高吸附容量和吸附选择性的 MOF 型吸附剂。