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Structure of Metal–Organic Framework Glasses by Ab Initio Molecular Dynamics
Chemistry of Materials ( IF 8.6 ) Pub Date : 2020-08-25 , DOI: 10.1021/acs.chemmater.0c02950
Romain Gaillac 1, 2 , Pluton Pullumbi 2 , Thomas D. Bennett 3 , François-Xavier Coudert 1
Affiliation  

While metal–organic frameworks have been mostly studied in their crystalline form, recent advances were made on their amorphous phases both in fundamental understanding and in relation to potential applications. In particular, the zeolitic imidazolate framework (ZIF) glasses, that can be obtained from quenching liquid ZIFs, have shown promise. However, the details of their microscopic structure are very hard to probe experimentally. Here, we use ab initio molecular dynamics simulations to investigate the nature of ZIF glasses obtained from quenching molten ZIFs in silico. Through computational modeling of the melt–quench process on three different ZIF crystals, we aim to understand the effect of topology and chemistry upon the structure of the glass, compared to both the crystalline precursor and the high-temperature liquid. We report here the first direct computational description of MOF glasses at the quantum chemical level. We find that both the chemical nature of the imidazolate linker and the topology of the framework play a role in the behavior upon quenching and the properties of the glasses obtained: structure, average coordination, and pore space.

中文翻译:

从头算分子动力学的金属有机骨架玻璃结构

虽然金属-有机骨架大多以晶体形式进行研究,但无论是在基本理解还是在潜在应用方面,非晶态都取得了最新进展。特别地,可以通过淬灭液体ZIF获得的沸石咪唑酸酯骨架(ZIF)玻璃已显示出希望。然而,它们的微观结构的细节很难通过实验来探究。在这里,我们使用从头算分子动力学模拟来研究通过淬火熔融的ZIF获得的ZIF玻璃的性质。通过对三种不同的ZIF晶体进行熔体-淬火过程的计算模型,我们旨在了解与晶体前驱体和高温液体相比,拓扑和化学性质对玻璃结构的影响。我们在这里报告在量子化学水平上对MOF玻璃的第一个直接计算描述。我们发现,咪唑基连接子的化学性质和骨架的拓扑结构在淬火后的行为和所得玻璃的性质中都起作用:结构,平均配位和孔空间。
更新日期:2020-09-22
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