In this study, traditional Monte Carlo simulation and density functional theory-based structural optimization methods were combined to screen computation-ready experimental metal-organic framework (MOF) database for the application of natural gas purification. Our results show that about half of the good performing computation-ready experimental MOF structures displayed various degrees of deformation (even collapse) after the structure optimization. This phenomenon attributed to the strong attraction of unsaturated metals which attract nearby organic components. For some materials with deformation, unsaturated metals form new bonds with the adjacent organic linkers creating distortions that would be unrealistic in the experimental materials. For the remaining relatively stable materials whose structural characteristics did not change too much, we further studied the adsorption performance of their optimized structures. Finally, 12 good-performing MOF materials with high stability were found which could greatly improve the possibility for constructing robust MOFs that could hold open metal sites by experiments.

中文翻译：

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用于天然气净化的可计算、实验性金属有机框架的多级筛选

在本研究中，将传统的蒙特卡罗模拟和基于密度泛函理论的结构优化方法相结合，筛选出用于天然气净化应用的可计算的实验金属有机框架 (MOF) 数据库。我们的结果表明，在结构优化后，大约一半性能良好的计算就绪实验 MOF 结构显示出不同程度的变形（甚至倒塌）。这种现象归因于吸引附近有机成分的不饱和金属的强烈吸引力。对于一些变形的材料，不饱和金属与相邻的有机连接体形成新的键，从而产生扭曲，这在实验材料中是不现实的。对于其余结构特性变化不大的相对稳定的材料，我们进一步研究了它们优化结构的吸附性能。最后，发现了 12 种具有高稳定性的高性能 MOF 材料，它们可以极大地提高通过实验构建可以保持开放金属位点的坚固 MOF 的可能性。