Influence of non-stoichiometric solutions on the THF hydrate growth: chemical affinity modelling and visualization

Randeep Ravesh, Ayaj A Ansari, Sabyasachi Mohapatra, Pankaj Sharma, M K Das, P K Panigrahi
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Abstract

Tetrahydrofuran (THF) hydrate is a useful material for cold storage applications and an excellent substitute for simulating natural gas hydrates. THF also serves as a thermodynamic promoter for hydrate formation. The selection of suitable THF concentration in the aqueous solution remains a challenging task for the utilization of the THF hydrate. Present work focuses on the influence of non-stoichiometric solutions on THF hydrate growth. The THF hydrate was grown in polycrystalline form as a gross hydrate layer from the wall towards the center of a cylindrical reactor. Experiments were conducted at the three THF concentrations 19.06, 30, and 15 wt% at 276.15 K and atmospheric pressure. Transient imaging of the hydrate provided the hydrate thickness with time. Moreover, the chemical affinity model was used to analyze the hydrate formation kinetics. An increase in the concentration of the THF in bulk solution accelerated hydrate growth with time. We found that non-homogeneity in the THF hydrate front increased in the azimuthal direction if the concentration of THF in the THF-water solution deviated from stoichiometric concentration. A hypothesis was also proposed to explain the above observation. The non-homogeneity was qualitatively shown by binary images and mathematically quantified using the maximum to minimum hydrate thickness ratio. The chemical affinity model proved effective in describing hydrate growth kinetics.

Abstract Image

非化学计量溶液对 THF 水合物生长的影响:化学亲和性建模和可视化
四氢呋喃(THF)水合物是一种用于冷藏的有用材料,也是模拟天然气水合物的极佳替代品。THF 还是水合物形成的热力学促进剂。在水溶液中选择合适的 THF 浓度仍然是利用 THF 水合物的一项具有挑战性的任务。目前的研究重点是非化学计量溶液对 THF 水合物生长的影响。在圆柱形反应器中,THF 水合物以多晶体形式从壁面向中心生长,形成毛水合物层。实验是在 276.15 K 和大气压力下,以 19.06、30 和 15 wt% 三种 THF 浓度进行的。水合物的瞬态成像提供了随时间变化的水合物厚度。此外,还使用化学亲和力模型分析了水合物形成动力学。随着时间的推移,体积溶液中 THF 浓度的增加会加速水合物的增长。我们发现,如果 THF 水溶液中的 THF 浓度偏离了化学计量浓度,THF 水合物前沿的非均质性在方位角方向上会增加。还提出了一个假设来解释上述观察结果。非均质性通过二元图像定性显示,并使用最大与最小水合物厚度比进行数学量化。事实证明,化学亲和力模型可以有效地描述水合物的生长动力学。
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