School of Chemistry and Chemical engineering, Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100084, China.
School of Chemistry and Chemical engineering, Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100084, China.
J Hazard Mater. 2023 Jan 15;442:130025. doi: 10.1016/j.jhazmat.2022.130025. Epub 2022 Sep 21.
Developing efficient adsorbents with proper pore size for pharmaceutical removal is challenging. Water stable metal-organic frameworks (MOFs) are crystalline materials within the three-dimensional frameworks, which have already aroused increasing attention for their potential advantages with high surface area and abundant channels. However, whether or not the existing ones are performing their full capacities needs to be seriously considered. Herein, we precisely designed a series of fine-tuning hierarchically porous materials based on the water-stable Zr-based MOFs. The adsorption capacity and uptake rate of as-synthesized materials for pharmaceuticals are significantly improved. Fifteen isostructural frameworks with increasing finely tuned pore structures were successfully constructed with seven monocarboxylic modulators of increasing alkyl chain lengths. A strong correlated relationship between the mesoporous proportion and trapping kinetics can be found. Adsorption performance of 17 pharmaceuticals with various typical categories has been systematically studied over these as-synthesized materials. Competitors in natural wastewater were studied systematically. The competitive adsorption can selectively trap the target compounds in HA (humic acid), BSA (bovine serum albumin), and BHB (bovine hemoglobin) by an efficient size exclusion effect. Thus, this study offers helpful guidance for MOF modification to enhance the removal of micropollutants in natural wastewater and a fundamental understanding of the porosity-performance relationships.
开发具有适当孔径的高效吸附剂以去除药物具有挑战性。水稳定的金属-有机骨架（MOFs）是三维骨架内的结晶材料，由于其具有高表面积和丰富的通道，因此已经引起了越来越多的关注。然而，现有的 MOFs 是否能够充分发挥其潜力，还需要认真考虑。在此，我们基于水稳定的 Zr 基 MOFs 精确设计了一系列精细调谐的分级多孔材料。所合成材料对药物的吸附容量和摄取率得到了显著提高。通过使用七种烷基链长度逐渐增加的单羧酸调节剂，成功构建了十五个具有精细调谐孔结构的同构框架。可以发现介孔比例和捕集动力学之间存在很强的相关性。对这些合成材料进行了 17 种具有各种典型类别的药物的系统吸附性能研究。系统研究了天然废水中的竞争性吸附物。通过有效的尺寸排除效应，竞争吸附可以选择性地在 HA（腐殖酸）、BSA（牛血清白蛋白）和 BHB（牛血红蛋白）中捕获目标化合物。因此，这项研究为 MOF 改性提供了有用的指导，以增强对天然废水中微污染物的去除，并为孔隙率-性能关系提供了基本的理解。
