Classical molecular simulations can provide significant insights into the gas adsorption mechanisms and binding sites in various metal-organic frameworks (MOFs). These simulations involve assessing the interactions between the MOF and an adsorbate molecule by calculating the potential energy of the MOF-adsorbate system using a functional form that generally includes nonbonded interaction terms, such as the repulsion/dispersion and permanent electrostatic energies. Grand canonical Monte Carlo (GCMC) is the most widely used classical method that is carried out to simulate gas adsorption and separation in MOFs and identify the favorable adsorbate binding sites. In this review, we provide an overview of the GCMC methods that are normally utilized to perform these simulations. We also describe how a typical force field is developed for the MOF, which is required to compute the classical potential energy of the system. Furthermore, we highlight some of the common analysis techniques that have been used to determine the locations of the preferential binding sites in these materials. We also review some of the early classical molecular simulation studies that have contributed to our working understanding of the gas adsorption mechanisms in MOFs. Finally, we show that the implementation of classical polarization for simulations in MOFs can be necessary for the accurate modeling of an adsorbate in these materials, particularly those that contain open-metal sites. In general, molecular simulations can provide a great complement to experimental studies by helping to rationalize the favorable MOF-adsorbate interactions and the mechanism of gas adsorption.

中文翻译：

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从经典分子模拟中洞察金属有机框架中的气体吸附机理。

经典的分子模拟可以为各种金属有机框架（MOF）中的气体吸附机理和结合位点提供重要的见识。这些模拟涉及通过使用通常包含非键合相互作用项（例如排斥/分散和永久静电能）的功能形式计算MOF-吸附物系统的势能，评估MOF与吸附物分子之间的相互作用。大经典蒙特卡洛（GCMC）是使用最广泛的经典方法，用于模拟MOF中的气体吸附和分离并确定有利的吸附物结合位点。在本文中，我们概述了通常用于执行这些模拟的GCMC方法。我们还将描述如何为MOF开发典型的力场，这是计算系统经典势能所必需的。此外，我们重点介绍了一些常用的分析技术，这些技术已用于确定这些材料中优先结合位点的位置。我们还将回顾一些早期的经典分子模拟研究，这些研究有助于我们对MOF中的气体吸附机理进行工作理解。最后，我们证明了在MOF中模拟进行经典极化对于精确建模这些材料（尤其是那些包含开放金属位点的材料）中的吸附物可能是必要的。通常，分子模拟可以通过帮助合理化MOF-吸附物相互作用和气体吸附机理，为实验研究提供很大的补充。