Two isomeric metal–organic frameworks bearing stilbene moieties for highly volatile iodine uptake,Inorganic Chemistry Frontiers

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Two isomeric metal–organic frameworks bearing stilbene moieties for highly volatile iodine uptake
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-05-27 , DOI: 10.1039/d2qi00835a
Jianping Tang _{1,

2} , Shenghua Zhou _{1,

3} , Mengyi Huang _{1,

4} , Zhenxin Liang ₁ , Shaodong Su ₁ , Yuehong Wen _{1,

3} , Qi-Long Zhu _{1,

3} , Xintao Wu _{1,

3}

Affiliation

Efficient, green, and economical removal of radioactive iodine (I₂) has drawn worldwide attention for the safe development of nuclear energy. Metal–organic frameworks (MOFs) have been demonstrated to be potential candidates for I₂ capture. Herein we report the synthesis of two novel isomeric MOFs bearing stilbene moieties for exceptionally high I₂ adsorption. [Cd(hsb-2)(tsbdc)]·0.5DMF (HSB-W8) and Cd(hsb-2)(tsbdc) (HSB-W9), which exhibit two-dimensional and twofold interpenetrated three-dimensional structures, respectively, have been assembled from hydrogenated Schiff base ligands, hsb-2 (1,2-bis(4′-pyridylmethylamino)-ethane) and trans-stilbene-4,4-dicarboxylate (tsbdc), and Cd(NO₃)₂ by the diffusion method. Such isomers arise from the different conformations of hsb-2 ligands controlled by diffusion temperatures. The π-electron-rich stilbene moieties render these Cd-MOFs ideal platforms for I₂ capture. The adsorption capacities of HSB-W8 and HSB-W9 in I₂ vapor at room temperature can reach up to 2.32 and 1.92 g g⁻¹, respectively, which are comparable to the best-performing MOF materials reported so far. Furthermore, pseudo-second-order (PSO) kinetic model analysis, Fourier transform infrared (FT-IR) spectroscopy, Raman spectral analysis, density functional theory (DFT) calculations, and control experiments were performed to shed light on host–guest interactions and the iodine adsorption mechanism. This work develops a rational strategy to design and synthesise functional MOF materials for iodine adsorption.

中文翻译：

两种带有二苯乙烯部分的异构金属-有机骨架，用于高挥发性碘吸收

高效、绿色、经济地去除放射性碘（I ₂）已引起全球核能安全发展的关注。_{金属有机框架 (MOF) 已被证明是 I 2}捕获的潜在候选者。在这里，我们报告了两种新型异构 MOFs 的合成，这些 MOFs 具有非常高的 I ₂吸附性。[Cd(hsb-2)(tsbdc)]·0.5DMF ( HSB-W8 ) 和 Cd(hsb-2)(tsbdc) ( HSB-W9 )，分别表现出二维和双重互穿的三维结构，已由氢化席夫碱配体 hsb-2（1,2-双（4'-吡啶基甲基氨基）-乙烷）和反式 stilbene-4,4-二羧酸盐（tsbdc）和 Cd（NO ₃) ₂采用扩散法。此类异构体源于受扩散温度控制的 hsb-2 配体的不同构象。富含 π 电子的二苯乙烯部分使这些 Cd-MOF 成为 I ₂捕获的理想平台。HSB-W8和HSB-W9在室温下对I ₂蒸气的吸附量可达2.32和1.92 gg ^-1，分别与迄今为止报道的性能最佳的 MOF 材料相当。此外，还进行了伪二级 (PSO) 动力学模型分析、傅里叶变换红外 (FT-IR) 光谱、拉曼光谱分析、密度泛函理论 (DFT) 计算和控制实验，以阐明主客体相互作用和碘吸附机理。这项工作开发了一种合理的策略来设计和合成用于碘吸附的功能性 MOF 材料。

更新日期：2022-05-27

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