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Reticular Chemistry with Art: A Case Study of Olympic Rings-Inspired Metal–Organic Frameworks
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2022-11-23 , DOI: 10.1021/jacs.2c09832
Jincheng Si 1, 2 , Hai-Lun Xia 2 , Kang Zhou 2 , Jingbai Li 2 , Kai Xing 3 , Jiafeng Miao 2 , Jian Zhang 2 , Hao Wang 2 , Lu-Lu Qu 1 , Xiao-Yuan Liu 2 , Jing Li 2, 4
Affiliation  

Herein, we demonstrate the successful utilization of reticular chemistry as an excellent designing strategy for the deliberate construction of a zirconium–tetracarboxylate metal–organic framework (MOF) inspired by the Olympic rings. HIAM-4017, with an unprecedented (4,8)-c underlying net topology termed jcs, was developed via insightful reconstruction of the rings and judicious design of a nonsymmetric organic linker. HIAM-4017 exhibits high porosity and excellent chemical and thermal stability. Furthermore, excited-state intramolecular proton transfer (ESIPT) was achieved in an isoreticular MOF, HIAM-4018, with a large Stokes shift of 155 nm as a result of introducing the hydroxyl group to the linker skeleton to induce OH···N interactions. Such interactions were analyzed thoroughly by employing the time-dependent density functional theory (TD-DFT). Because of their good thermal and chemical stability, and strong luminescence, nanosized HIAM-4017 and HIAM-4018 were fabricated and used for Cr2O72– detection. Both MOFs demonstrate excellent sensitivity and selectivity. This work represents a neat example of building structure- and property-specific MOFs guided by reticular chemistry.

中文翻译:

网状化学与艺术:以奥林匹克五环为灵感的金属有机骨架案例研究

在这里,我们展示了网状化学的成功利用作为一种优秀的设计策略,用于受奥林匹克五环启发的锆-四羧酸盐金属-有机框架(MOF)的有意构建。HIAM-4017,具有前所未有的 (4,8)-c 底层网络拓扑,称为jcs, 是通过对环的有见地的重建和非对称有机连接器的明智设计而开发的。HIAM-4017 具有高孔隙率和出色的化学和热稳定性。此外,在等网状 MOF HIAM-4018 中实现了激发态分子内质子转移 (ESIPT),由于将羟基引入接头骨架以诱导 OH···N 相互作用,斯托克斯位移高达 155 nm . 通过采用时间相关密度泛函理论 (TD-DFT) 对此类相互作用进行了彻底分析。由于其良好的热稳定性和化学稳定性以及强发光性,纳米级 HIAM-4017 和 HIAM-4018 被制备并用于 Cr 2 O 7 2–检测。两种 MOF 均表现出出色的灵敏度和选择性。这项工作代表了在网状化学的指导下构建特定于结构和特性的 MOF 的一个很好的例子。
更新日期:2022-11-23
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