Gas Hydrate Dynamics with Parameter-Free Clathrate Phase Description: Validation for Hydrate Formation and Dissociation.

IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry A Pub Date : 2024-09-19 Epub Date: 2024-09-04 DOI:10.1021/acs.jpca.4c03130
Shubhangi Sharma, Harshal J Dongre, Amiya K Jana
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Abstract

One of the major challenges involved in clathrate hydrate science that has remained for more than six decades lies in highly parametric clathrate phase estimation. In this contribution, a recently developed parameter-free hydrate phase statistical equilibrium model is employed for the first time to formulate the formation and dissociation dynamics of clathrates and predict their experimental observation at diverse geological conditions. This rigorous thermokinetic model takes into account various practical issues, notably hydrate formation in nanometer-sized pores (confirmed through seismic survey studies), irregularity in porous particle shape and pore size, renewal of the particle surface over which hydrate majorly forms and decays, and nth-order phase transformation. The model parameters are identified by formulating the genetic algorithm-based optimization strategy. Finally, this multicomponent hydrate model is tested by predicting the formation and decomposition data having pure water as well as saltwater with and without porous media. The proposed formulation secures a promising performance with a lower absolute average relative deviation for a wide variety of data sets over the latest hydrate models.

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气体水合物动力学与无参数凝块相描述:验证水合物的形成和解离。
凝块水合物科学的主要挑战之一是高度参数化的凝块相估算,这一挑战已持续了六十多年。在本论文中,首次采用了最近开发的无参数水合物相统计平衡模型,来阐述凝块的形成和解离动力学,并预测在不同地质条件下的实验观测结果。这一严格的热动力学模型考虑了各种实际问题,特别是纳米级孔隙中的水合物形成(通过地震勘测研究证实)、多孔颗粒形状和孔隙大小的不规则性、水合物主要形成和衰减的颗粒表面的更新以及 n 次相变。通过制定基于遗传算法的优化策略,确定了模型参数。最后,通过预测有多孔介质和无多孔介质的纯水和盐水的形成和分解数据,对该多组分水合物模型进行了测试。与最新的水合物模型相比,所提出的模型在各种数据集上的绝对平均相对偏差较小,性能良好。
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来源期刊
The Journal of Physical Chemistry A
The Journal of Physical Chemistry A 化学-物理:原子、分子和化学物理
CiteScore
5.20
自引率
10.30%
发文量
922
审稿时长
1.3 months
期刊介绍: The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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