Rogge Sven M J
Center for Molecular Modeling, Ghent University, Technologiepark 46, Zwijnaarde, 9052, Belgium.
Faraday Discuss. 2021 Feb 1;225:271-285. doi: 10.1039/c9fd00148d. Epub 2020 Oct 26.
Computational insight into the impact of cooperative phenomena and correlated spatial disorder on the macroscopic behaviour of metal-organic frameworks (MOFs) is essential in order to consciously engineer these phenomena for targeted applications. However, the spatial extent of these effects, ranging over hundreds of nanometres, limits the applicability of current state-of-the-art computational tools in this field. To obtain a fundamental understanding of these long-range effects, the micromechanical model is introduced here. This model overcomes the challenges associated with conventional coarse-graining techniques by exploiting the natural partitioning of a MOF material into unit cells. By adopting the elastic deformation energy as the central quantity, the micromechanical model hierarchically builds on experimentally accessible input parameters that are obtained from atomistic quantum mechanical or force field simulations. As a result, the here derived micromechanical equations of motion can be adopted to shed light on the effect of long-range cooperative phenomena and correlated spatial disorder on the performance of mesoscale MOF materials.
为了有针对性地设计这些现象以实现特定应用，深入了解协同现象和相关空间无序对金属有机框架（MOF）宏观行为的影响至关重要。然而，这些效应的空间范围达数百纳米，限制了当前该领域最先进计算工具的适用性。为了从根本上理解这些长程效应，本文引入了微机械模型。该模型通过利用MOF材料自然划分为晶胞的方式，克服了与传统粗粒化技术相关的挑战。通过采用弹性变形能作为核心量，微机械模型基于从原子量子力学或力场模拟获得的、可通过实验获取的输入参数进行分层构建。因此，本文推导的微机械运动方程可用于阐明长程协同现象和相关空间无序对中尺度MOF材料性能的影响。
