开发类MOF-5超微孔金属方形框架，用于高效乙炔储存和分离,Journal of Materials Chemistry A

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开发类MOF-5超微孔金属方形框架，用于高效乙炔储存和分离
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-09-06 , DOI: 10.1039/d3ta04732f
Hai-Peng Li _{1,

2} , Jia-Wen Wang ₁ , Quan-Guo Zhai ₁

Affiliation

尽管MOF-5及其相关家族成员是具有里程碑意义的金属有机框架（MOF），但它们具有大的比表面积和高的孔隙率，这长期以来一直是其不稳定性的问题。除了经典的 [Zn ₄ O(COO) ₆ ] 之外，引入新的无机构件是保持 MOF-5 极具吸引力的结构的一种有前途的方法。在此，利用方酸（SQ）和过渡金属盐合成了一系列新型MOF-5类骨架，即{(NH(CH ₃ ) ₂ ) ₂ [M ₄ X ₄ (SQ) ₃ ]} _n (SNNU-505-M，M = Zn、Co 和 Ni，X = F ⁻和 OH ⁻）。该SNNU-505-M系列化合物中，除SNNU-505-Zn的μ _{3桥原子为F}^-离子外，其余均为OH ^-离子。与MOF-5相比，SNNU-505-M在有机溶剂和水溶液（pH = 3–13）中表现出良好的稳定性。此外，得益于其超微孔径和多个极性的F ^- /OH ^-吸附位点，SNNU-505-M表现出高C ₂ H ₂吸附能力和优异的分离性能。其中SNNU-505-Zn表现出最好的C ₂ H ₂ /C ₂ H ₄ (1 : 1)分离性能，其突破间隔时间为51 min g^-1于 298 K，流速为 2 mL min^-1。GCMC计算进一步表明SNNU-505-Zn优异的C₂ H₂吸收和C₂ H₂ /C₂ H₄分离性能主要归因于C₂ H_{之间的多个C–H⋯F氢键2}分子和MOF骨架。

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Development of MOF-5-like ultra-microporous metal-squarate frameworks for efficient acetylene storage and separation

Although MOF-5 and its related family members are landmark metal–organic frameworks (MOFs), they have large specific surface area and high porosity, which have long been a subject regarding their instability. The introduction of new inorganic building blocks, in addition to classical [Zn₄O(COO)₆], is a promising way to maintain the highly attractive architecture of MOF-5. Herein, a family of new MOF-5-like frameworks were synthesized by using squaric acid (SQ) and transition metal salts, namely, {(NH(CH₃)₂)₂[M₄X₄(SQ)₃]}_n (SNNU-505-M, M = Zn, Co and Ni, X = F⁻ and OH⁻). In this SNNU-505-M series of compounds, except for the μ₃-bridging atom of SNNU-505-Zn being an F⁻ ion, all the others are OH⁻. Compared with MOF-5, SNNU-505-M exhibits good stability in organic solvent and aqueous solutions (pH = 3–13). Furthermore, benefiting from its ultra-micropore size and multiple polarity F⁻/OH⁻ adsorption sites, SNNU-505-M shows high C₂H₂ adsorption capacity and excellent separation performance. In particular, SNNU-505-Zn exhibits the best C₂H₂/C₂H₄ (1 : 1) separation performance and its breakthrough interval time is 51 min g⁻¹ at 298 K at a flow rate of 2 mL min⁻¹. The GCMC calculations further demonstrate that the excellent C₂H₂ uptake and C₂H₂/C₂H₄ separation performance of SNNU-505-Zn can be mainly attributed to the multiple C–H⋯F hydrogen bonds between the C₂H₂ molecules and MOF skeleton.

更新日期：2023-09-06

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