Heijmans Koen, Tranca Ionut C, Smeulders David M J, Vlugt Thijs J H, Gaastra-Nedea Silvia V
Department of Mechanical Engineering, Eindhoven University of Technology, Groene Loper 15, 5600MB Eindhoven, The Netherlands.
Process & Energy Department, Delft University of Technology, Leeghwaterstraat 39, 2628CB Delft, The Netherlands.
J Chem Theory Comput. 2021 Jan 12;17(1):322-329. doi: 10.1021/acs.jctc.0c00876. Epub 2020 Dec 22.
Absorption and reactive properties of fluids in porous media are key to the design and improvement of numerous energy related applications. Molecular simulations of these systems require accurate force fields that capture the involved chemical reactions and have the ability to describe the vapor-liquid equilibrium (VLE). Two new reactive force fields (ReaxFF) for CO and HO are developed, which are capable of not only modeling bond breaking and formation in reactive environments but also predicting their VLEs at saturation conditions. These new force fields include extra terms (ReaxFF-lg) to improve the long-range interactions between the molecules. For validation, we have developed a new Gibbs ensemble Monte Carlo (GEMC-ReaxFF) approach to predict the VLE. Computed VLE data show good agreement with National Institute of Standards and Technology reference data as well as existing nonreactive force fields. This validation proves the applicability of the GEMC-ReaxFF method to test new reactive force fields, and simultaneously it proves the applicability to extend newly developed ReaxFF force fields to other more complex reactive systems.
多孔介质中流体的吸收和反应特性是众多能源相关应用设计和改进的关键。对这些系统进行分子模拟需要精确的力场，以捕捉所涉及的化学反应，并具备描述气液平衡（VLE）的能力。开发了两种用于CO和HO的新型反应力场（ReaxFF），它们不仅能够模拟反应环境中的键断裂和形成，还能预测饱和条件下的气液平衡。这些新的力场包括额外的项（ReaxFF-lg），以改善分子间的长程相互作用。为了进行验证，我们开发了一种新的吉布斯系综蒙特卡罗（GEMC-ReaxFF）方法来预测气液平衡。计算得到的气液平衡数据与美国国家标准与技术研究院的参考数据以及现有的非反应性力场显示出良好的一致性。该验证证明了GEMC-ReaxFF方法在测试新反应力场方面的适用性，同时也证明了将新开发的ReaxFF力场扩展到其他更复杂反应系统的适用性。
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