García Brais R, Algaba Jesús, Blas Felipe J, Pérez-Rodríguez Martín, Piñeiro Manuel M
Departamento de Física Aplicada, Universidade de Vigo, 36310 Vigo, Spain.
Laboratorio de Simulación Molecular y Química Computacional, CIQSO-Centro de Investigación en Química Sostenible and Departamento de Ciencias Integradas, Universidad de Huelva, 21006 Huelva, Spain.
Energy Fuels. 2025 May 14;39(21):9884-9892. doi: 10.1021/acs.energyfuels.5c01091. eCollection 2025 May 29.
Hydroquinone clathrates (HQ clathrates) are highly structured crystalline materials with promising application in carbon separation and sequestration, and also in hydrogen storage. In this study, molecular simulation techniques are employed to analyze the structure of β-HQ clathrates using local bond order parameters. The methodology is based on the definition by Steinhardt and Lechner-Dellago of the averaged bond order parameters, which allow a precise differentiation between solid and liquid phases. Using molecular dynamics simulations, we evaluate the role of guest molecules such as CO and CH in the stability and formation of clathrates. In this study, we determine and test an optimal combination of bond order parameters ( - ) capable of accurately characterizing phase transitions with a classification error of less than 0.001%. The proposed method is able to qualitatively and quantitatively discern the membership of each molecule to the different phases during the crystallization and dissociation processes, demonstrating its effectiveness in the study of the dynamics of HQ clathrate at different pressure and temperature conditions. The results of this work provide a solid and applicable theoretical framework intended to further provide insight into the nucleation process of this system, contributing to its understanding.
对苯二酚包合物（HQ包合物）是高度结构化的晶体材料，在碳分离与封存以及储氢方面有着广阔的应用前景。在本研究中，采用分子模拟技术，利用局部键序参数分析β - HQ包合物的结构。该方法基于Steinhardt以及Lechner - Dellago对平均键序参数的定义，这使得能够精确区分固相和液相。通过分子动力学模拟，我们评估了诸如CO和CH等客体分子在包合物稳定性和形成过程中的作用。在本研究中，我们确定并测试了键序参数（ - ）的最佳组合，其能够以小于0.001%的分类误差准确表征相变。所提出的方法能够定性和定量地辨别每个分子在结晶和解离过程中属于不同相的归属，证明了其在研究不同压力和温度条件下HQ包合物动力学方面的有效性。这项工作的结果提供了一个坚实且适用的理论框架，旨在进一步深入了解该系统的成核过程，有助于对其进行理解。
