Two-Dimensional Lattice-Gas model for methane clathrate Hydrates: Comparative analysis with experiments and Three-Dimensional simulations

IF 5.3 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Liquids Pub Date : 2025-05-09 DOI:10.1016/j.molliq.2025.127669

Julián Juan , María E. Pronsato , Antonio J. Ramirez-Pastor , Pablo Longone

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引用次数: 0

Abstract

Methane clathrate hydrates, particularly those with an sI structure, are significant due to their potential as energy resources and their impact on gas pipelines. In this study, a two-dimensional (2D) lattice-gas model is employed to investigate the main thermodynamic properties of methane clathrate hydrates. The proposed framework is validated through comparison with experimental data and more advanced three-dimensional (3D) simulations. Adsorption isotherms, dissociation enthalpy and phase stability of the sI structure are evaluated using Monte Carlo (MC) simulations in the grand canonical ensemble. The 2D adsorption isotherms demonstrate a strong alignment with both experimental data and 3D simulations, thereby highlighting the 2D model’s ability to accurately represent both rigid and flexible sI structures. The dissociation enthalpy calculated using the proposed approach (76.4 kJ/mol) ~~excellently~~ matches the experimental value (78 kJ/mol), thus confirming the model’s validity. Furthermore, the phase diagram calculated using the Clausius-Clapeyron equation shows very good agreement with experimental data between 260 and 290 K, with deviations observed above this temperature. These findings highlight the efficacy and robustness of the 2D model in studying methane clathrate hydrates and suggest its potential applicability for investigating other guest species and hydrate structures.

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甲烷笼形水合物的二维晶格-气体模型：与实验和三维模拟的比较分析

甲烷包合物水合物，特别是具有sI结构的水合物，由于其作为能源的潜力和对天然气管道的影响而具有重要意义。本文采用二维晶格-气体模型研究了甲烷包合物水合物的主要热力学性质。通过与实验数据和更先进的三维（3D）模拟的比较，验证了所提出的框架。利用蒙特卡罗（MC）模拟计算了sI结构在大正则系综中的吸附等温线、解离焓和相稳定性。二维吸附等温线显示出与实验数据和三维模拟的强烈一致性，从而突出了二维模型准确表征刚性和柔性sI结构的能力。利用该方法计算的解离焓（76.4 kJ/mol）与实验值（78 kJ/mol）吻合良好，证实了模型的有效性。此外，用克劳修斯-克拉珀龙方程计算的相图与260 ~ 290 K之间的实验数据非常吻合，在此温度以上观察到偏差。这些发现突出了二维模型在研究甲烷包合物水合物方面的有效性和稳健性，并表明其在研究其他客体物种和水合物结构方面的潜在适用性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Molecular Liquids 化学-物理：原子、分子和化学物理

CiteScore

10.30

自引率

16.70%

发文量

2597

审稿时长

78 days

期刊介绍： The journal includes papers in the following areas: – Simple organic liquids and mixtures – Ionic liquids – Surfactant solutions (including micelles and vesicles) and liquid interfaces – Colloidal solutions and nanoparticles – Thermotropic and lyotropic liquid crystals – Ferrofluids – Water, aqueous solutions and other hydrogen-bonded liquids – Lubricants, polymer solutions and melts – Molten metals and salts – Phase transitions and critical phenomena in liquids and confined fluids – Self assembly in complex liquids.– Biomolecules in solution The emphasis is on the molecular (or microscopic) understanding of particular liquids or liquid systems, especially concerning structure, dynamics and intermolecular forces. The experimental techniques used may include: – Conventional spectroscopy (mid-IR and far-IR, Raman, NMR, etc.) – Non-linear optics and time resolved spectroscopy (psec, fsec, asec, ISRS, etc.) – Light scattering (Rayleigh, Brillouin, PCS, etc.) – Dielectric relaxation – X-ray and neutron scattering and diffraction. Experimental studies, computer simulations (MD or MC) and analytical theory will be considered for publication; papers just reporting experimental results that do not contribute to the understanding of the fundamentals of molecular and ionic liquids will not be accepted. Only papers of a non-routine nature and advancing the field will be considered for publication.