State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun, 130012, P. R. China.
Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, 189 Songling Road, Laoshan District, Qingdao, Shandong, 266101, P. R. China.
Small. 2021 Jun;17(22):e2006112. doi: 10.1002/smll.202006112. Epub 2021 Feb 19.
Developing functionalized 3D covalent organic frameworks (3D COFs) is critical to broaden their potential applications. However, the introduction of specific functionality in 3D COFs remains a great challenge because most of the functional groups are not compatible with the synthesis conditions. Herein, for the first time 3D thioether-based COFs (JUC-570 and JUC-571) for mercury (Hg ) removal from aqueous solution is reported. These 3D thioether-based COFs prepared by the bottom-up approach display high Hg uptakes (972 mg g for JUC-570 and 970 mg g for JUC-571 at pH = 5), fast adsorption kinetics (distribution coefficient K value of 2.29 × 10 mL g for JUC-570 and 2.07 × 10 mL g for JUC-571), and favorable selectivity. In particular, JUC-570 is periodically decorated with isopropyl groups around imine bonds that markedly improve its chemical stability and effectively prevent the pore collapse, and thus endows high Hg adsorption capacity (619 mg g ) and excellent cycle performance even at pH = 1. This study not only puts forward a new route to construct stable functionalized 3D COFs, but also promotes their potential applications in areas related to the environment.
开发功能化的 3D 共价有机骨架(3D COFs)对于拓宽其潜在应用至关重要。然而,在 3D COFs 中引入特定功能仍然是一个巨大的挑战,因为大多数功能基团与合成条件不兼容。在此,首次报道了用于从水溶液中去除汞(Hg)的基于 3D 硫醚的 COFs(JUC-570 和 JUC-571)。这些通过自下而上方法制备的基于 3D 硫醚的 COFs 在 pH = 5 时显示出高的 Hg 吸附量(JUC-570 为 972mg g,JUC-571 为 970mg g)、快速的吸附动力学(分配系数 K 值分别为 2.29×10 mL g和 2.07×10 mL g)和良好的选择性。特别地,JUC-570 周期性地在亚胺键周围用异丙基修饰,这显著提高了其化学稳定性并有效地防止了孔塌陷,从而赋予其高的 Hg 吸附容量(619mg g)和优异的循环性能,即使在 pH = 1 时也是如此。这项研究不仅提出了构建稳定功能化 3D COFs 的新途径,而且还促进了它们在与环境相关的领域中的潜在应用。