Chng Jia Yuan, Sholl David S
School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States.
Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States.
ACS Appl Mater Interfaces. 2023 Aug 9;15(31):37828-37836. doi: 10.1021/acsami.3c07158. Epub 2023 Jul 26.
We present a transferable force field (FF) for simulating the bulk properties of linear and cyclic siloxanes and the adsorption of these species in metal-organic frameworks (MOFs). Unlike previous FFs for siloxanes, our FF accurately reproduces the vapor-liquid equilibria of each species in the bulk phase. The quality of our FF combined with the Universal Force Field using standard Lorentz-Berthelot combining rules for MOF atoms was assessed in a wide range of MOFs without open metal sites, showing good agreement with dispersion-corrected density functional theory calculations. Predictions with this FF show good agreement with the limited experimental data for siloxane adsorption in MOFs that is available. As an example of using the FF to predict adsorption properties in MOFs, we present simulations examining entropy effects in binary linear and cyclic siloxane mixture coadsorption in the large-pore MOF with structure code FOTNIN.
我们提出了一种可转移的力场（FF），用于模拟线性和环状硅氧烷的本体性质以及这些物质在金属有机框架（MOF）中的吸附。与先前用于硅氧烷的力场不同，我们的力场能准确再现各物质在本体相中的气液平衡。我们使用针对MOF原子的标准洛伦兹 - 贝塞洛特组合规则，将我们的力场与通用力场相结合，在广泛的无开放金属位点的MOF中进行了评估，结果表明与色散校正密度泛函理论计算结果吻合良好。使用该力场的预测结果与现有的关于MOF中硅氧烷吸附的有限实验数据吻合良好。作为使用该力场预测MOF吸附性质的一个例子，我们展示了在具有结构代码FOTNIN的大孔MOF中，对二元线性和环状硅氧烷混合物共吸附中的熵效应进行模拟研究。
