Applied Surface Science ( IF 6.3 ) Pub Date : 2022-05-04 , DOI: 10.1016/j.apsusc.2022.153494
Menghan Qin 1 , Yumiao Shi 1 , Dingkun Lu 1 , Jingjing Deng 1, 2 , Guoyue Shi 3 , Tianshu Zhou 1, 2
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Due to the excessive use, cephalosporin antibiotics have been detected in various aquatic environments, which may result in environmental and health concern. In this study, bimetallic metal–organic frameworks (MOFs), Hf-UiO-66 and Ti-UiO-66, were successfully designed and obtained via post-synthetic method from UiO-66 for the adsorption of cefoperazone. A serious of adsorption experiments were investigated. The adsorption kinetics and isotherms demonstrated that the adsorption process followed pseudo-second-order kinetic model and Langmuir isotherm model. Hf/Ti-UiO-66 exhibited much better adsorption performance than the undoped UiO-66. Particularly, Hf-UiO-66 had the highest adsorption capacity (346.0 mg g−1). With the introduction of Hf or Ti, the chemical coordination environment changed, which resulted in defective structures of MOFs. Such defective structures increased the adsorption active sites, changed the surface charges and enlarged pores. Based on the characterization by FT-IR, XPS, and zeta potential, it was identified that the electrostatic attraction, π-π stacking, hydrogen bonding and metal complexation were the driving force for the high adsorption capacity of the bimetallic MOFs. The as-prepared MOFs displayed good stability and reusability. This work provides a great prospect for the design and application of bimetallic defective MOFs in cephalosporins removal in environmental water.
中文翻译:

用于头孢哌酮吸附的高性能 Hf/Ti 掺杂缺陷 Zr-MOF:行为和机制
由于过度使用,已在各种水生环境中检测到头孢菌素类抗生素,这可能会导致环境和健康问题。在这项研究中,成功设计并通过后合成方法从 UiO-66 获得了双金属金属有机骨架 (MOF) Hf-UiO-66 和 Ti-UiO-66,用于吸附头孢哌酮。研究了一系列吸附实验。吸附动力学和等温线表明吸附过程遵循准二级动力学模型和Langmuir等温线模型。Hf/Ti-UiO-66比未掺杂的UiO-66表现出更好的吸附性能。特别是,Hf-UiO-66 具有最高的吸附容量(346.0 mg g -1)。随着 Hf 或 Ti 的引入,化学配位环境发生了变化,导致 MOFs 结构缺陷。这种有缺陷的结构增加了吸附活性位点,改变了表面电荷并扩大了孔隙。基于FT-IR、XPS和zeta电位的表征,确定了静电引力、π-π堆积、氢键和金属络合是双金属MOFs高吸附能力的驱动力。所制备的 MOF 表现出良好的稳定性和可重复使用性。该工作为双金属缺陷型MOFs在环境水中头孢菌素去除中的设计和应用提供了广阔的前景。