Pore opening and breathing transitions in metal-organic frameworks: Coupling adsorption and deformation
Pore opening and breathing transitions in metal-organic frameworks: Coupling adsorption and deformation
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DOI：
10.1016/j.jcis.2020.05.105
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发表时间：
2020-10-15
影响因子：
9.9
通讯作者：
Kuchta, Bogdan
中科院分区：
文献类型：
--
作者：
Formalik, Filip;Neimark, Alexander V.;Kuchta, Bogdan
软质多孔晶体在各种物理刺激下发生大的结构转变。呼吸般的转变，发生大的体积变化，已与双稳态或多稳态晶体结构的存在。了解这些转变的机理对于它们在气体吸附、分离和储存中的潜在应用至关重要。然而，通用描述仍然缺失。在这里，我们提供了一个详细的，多尺度的定性和定量分析的吸附诱导的“呼吸”转换在两个金属有机框架（MOFs）：MIL-53（铝），这是我们的方法的参考案例，最近合成的JUK-8，没有吸附物，不显示任何双稳态。所提出的方法是基于原子模拟，不需要任何经验或可调参数。它允许预测潜在的结构转变的MOFs，包括吸附引起的变形来自吸附应力模型。我们还表明，计算和实验结果之间的定量协议严重依赖于色散能量校正的质量。我们的方法代表了一种新的，强大的工具，用于设计和筛选柔性材料，替代和补充实验方法。(C)2020作者爱思唯尔公司出版
Soft porous crystals undergo large structural transformations under a variety of physical stimuli. Breathing-like transformations, occurring with a large volume change, have been associated with an existence of bi-stable or multi-stable crystal structures. Understanding of the mechanism of these transformations is essential for their potential applications in gas adsorption, separation and storage. However, the generic description is still missing. Here, we provide a detailed, multiscale qualitative and quantitative analysis of the adsorption-induced "breathing" transformations in two metal organic frameworks (MOFs): MIL-53(Al) which is a reference case of our approach, and recently synthesized JUK-8, which does not show any bistability without adsorbate. The proposed approach is based on atomistic simulations and does not require any empirical or adjustable parameters. It allows for a prediction of potential structural transformations in MOFs including the adsorption induced deformations derived from adsorption stress model. We also show that the quantitative agreement between calculated and experimental results critically depends on the quality of the dispersion energy correction. Our methodology represents a new, powerful tool for designing and screening of flexible materials, alternative and complimentary to experimental approaches. (C) 2020 The Authors. Published by Elsevier Inc.