部分连接子取代策略构建四元类 HKUST MOF 用于高效乙炔储存和分离,ACS Applied Materials & Interfaces

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部分连接子取代策略构建四元类 HKUST MOF 用于高效乙炔储存和分离
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-08-03 , DOI: 10.1021/acsami.2c10346
Lizhen Liu ₁ , Susu Wu ₁ , Dandan Li ₁ , Yunbin Li ₂ , Hao Zhang ₂ , Lu Li ₂ , Shaowei Jin ₃ , Zizhu Yao ₂

Affiliation

多组分金属有机框架（MOF）作为能够精确编程精细结构和特定功能的新兴材料而备受关注。在这里，我们通过将双功能配体引入众所周知的 HKUST-1 结构中，应用部分接头替换策略来编译类似 HKUST-1 的四元 MOF。FUT-1是一种新的类似 HKUST 的tbo拓扑 MOF，由桨轮 [Cu ₂ (COO) ₄ ]、三角形金属环吡唑簇 Cu ₃ (μ ₃ -OH) (NN) ₃构建块和两个不同的接头组装而成。FUT-1在水溶液中表现出良好的机械稳定性、水稳定性和化学稳定性（pH = 3-12）。此外，由这种多组分基元创造的多孔环境赋予FUT-1高 C ₂ H _{2存储和显着的 C}₂ H ₂ /CO ₂选择性分离性能。动态突破实验和理想吸附溶液理论计算进一步证明FUT-1可以选择性地从 C ₂ H ₂ /CO ₂中捕获 C ₂ H ₂环境条件下的混合物。基于大正则蒙特卡罗模拟，FUT-1的高C ₂ H ₂分离性能归因于C ₂ H ₂分子与壁上的三核金属环簇之间形成的π-络合物，这为C提供了更强的亲和力₂ H ₂识别比CO ₂分子大。

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Partial Linker Substitution Strategy to Construct a Quaternary HKUST-like MOF for Efficient Acetylene Storage and Separation

Multicomponent metal–organic frameworks (MOFs) have received much attention as emerging materials capable of precisely programing exquisite structures and specific functions. Here, we applied a partial linker substitution strategy to compile an HKUST-1-like quaternary MOF by introducing a bifunctional ligand into the well-known HKUST-1 structure. FUT-1, a new HKUST-like tbo topology MOF, was assembled with paddlewheel [Cu₂(COO)₄], triangular metallocycle pyrazole cluster Cu₃(μ₃-OH) (NN)₃ building blocks, and two distinct linkers. FUT-1 exhibited good mechanical stability, water stability, and chemical stability (pH = 3–12) in aqueous solutions. Moreover, the porous environments created by this multicomponent primitive endow FUT-1 with high C₂H₂ storage and significantly selective separation performance of C₂H₂/CO₂. Dynamic breakthrough experiments and ideal adsorbed solution theory calculations further demonstrate that FUT-1 can selectively capture C₂H₂ from C₂H₂/CO₂ mixtures under ambient conditions. Based on grand canonical Monte Carlo simulations, the high C₂H₂ separation performance of FUT-1 is attributed to the π-complex formed between the C₂H₂ molecule and the trinuclear metallocycle clusters on the wall, which provides stronger affinity for C₂H₂ recognition than the CO₂ molecule.

更新日期：2022-08-03

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