Modulation of Magnetic Behavior and Hg<sup>2+</sup> Removal by Solvent-Assisted Linker Exchange Based on a Water-Stable 3D MOF
作者:Zhichao Shao、Chao Huang、Jian Dang、Qiong Wu、Yeye Liu、Jie Ding、Hongwei Hou
DOI:10.1021/acs.chemmater.8b03621
日期:2018.11.13
SC–SC solvent-assisted linker exchange (SALE) in MOF materials is of high interest due to the potential applications. In this work, we reported an efficient transformation via SALE in a water-stable 3D MOF ([Ni1.5(L)(4,4′-azobpy)(H2O)]·6.5H2O}n (1)) (H3L = 1-aminobenzene-3,4,5-tricarboxylic acid). The reaction progress of SALE was monitored and proved by single crystal XRD, PXRD and UV–vis absorption analyses, and the structural integrity of progeny MOFs [Ni1.5(L)(4,4′-bpy)(H2O)]·6H2O}n (2), [Ni1.5(L)(bpe)(H2O)]·8.5H2O}n (3), and [Ni1.5(L)(NH2-bpy)(H2O)]·7.5H2O}n (4) were maintained very well, which is rarely in reported MOF materials. Theoretical calculations and the analyses of core–shell crystals give us better understanding of the exchange process. Interestingly, MOFs 2 and 3 obtained by SALE methods showed the different magnetic behavior comparing to parent MOF 1. Especially, because of the functional −NH2 group, progeny MOF 4 displayed the good capability to remove Hg2+ ions with an adsorption capacity of 93.693 mg/g. This work provides a new way to develop multifunctional MOF materials.
MOF 材料中的 SC-SC 溶剂辅助连接体交换(SALE)因其潜在的应用而备受关注。在这项工作中,我们报道了通过 SALE 在水稳定的三维 MOF([Ni1.5(L)(4,4′-azobpy)(H2O)]-6.5H2O}n (1))(H3L = 1-氨基苯-3,4,5-三羧酸)中的高效转化。通过单晶 XRD、PXRD 和紫外-可见吸收分析监测并证明了 SALE 的反应过程,以及原生 MOFs [Ni1.5(L)(4,4′-bpy)(H2O)]-6H2O}n(2)、[Ni1.5(L)(bpe)(H2O)]-8.5H2O}n(3)和[Ni1.5(L)(NH2-bpy)(H2O)]-7.5H2O}n(4)的结构保持得非常好,这在已报道的 MOF 材料中是很少见的。理论计算和核壳晶体分析使我们对交换过程有了更好的理解。有趣的是,与母体 MOF 1 相比,通过 SALE 方法得到的 MOF 2 和 3 表现出了不同的磁性。 特别是,由于功能性 -NH2 基团的存在,母体 MOF 4 显示出了良好的去除 Hg2+ 离子的能力,其吸附容量为 93.693 mg/g。这项研究为开发多功能 MOF 材料提供了一条新途径。