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Water Wettability Coupled with Film Growth on Realistic Cyclopentane Hydrate Surfaces
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    Water Wettability Coupled with Film Growth on Realistic Cyclopentane Hydrate Surfaces
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    Langmuir

    Cite this: Langmuir 2021, 37, 42, 12447–12456
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    https://doi.org/10.1021/acs.langmuir.1c02136
    Published October 13, 2021
    Copyright © 2021 American Chemical Society

    Abstract

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    Although the wettability of hydrate surfaces and hydrate film growth are key to understanding hydrate agglomeration and pipeline plugging, a quantitative understanding of the coupled behavior between both phenomena is lacking. In situ measurements of wettability coupled with film growth were performed for cyclopentane hydrate surfaces in cyclopentane at atmospheric pressure and temperatures between 1.5–6.8 °C. Results were obtained as a function of annealing (conversion) time and subcooling. Hydrate surface wettability decreased as annealing time increased, while hydrate film growth rate was unaffected by annealing time at any subcooling. The results are interpreted as a manifestation of the hydrate surface porosity, which depends on annealing time and controls water spreading on the hydrate surface. The wettability generally decreased as the subcooling increased because higher subcooling yields rougher hydrate surfaces, making it harder for water to spread. However, this effect is balanced by hydrate growth rates, which increase with subcooling. Also affecting the results, surface heating from heat release (from exothermic crystallization) allows excess surface water to promote spreading. The hydrate film growth rate on water droplets increased with subcooling, as expected from a higher driving force. At any subcooling, the instantaneous hydrate growth rate decreased over time, likely from heat transfer limitations. A new phenomenon was observed, where the angle at the three-phase point increases from the initial contact angle upon hydrate film growth, named the crystallization angle. This is attributed to the water droplet trying to spread while the thin film is weak enough to be redirected. Once the hydrate film grows and forms a “wall” around the droplet, it cannot be moved, and further growth yields a crater on the droplet surface, attributed to water penetrating the hydrate surface pore structures. This fundamental behavior has many flow assurance implications since it affects the interactions between the agglomerating hydrate particles and water droplets.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.langmuir.1c02136.

    • Additional contact angle images from experiments performed on cyclopentane hydrate in a cyclopentane/n-dodecane mixture (PDF)

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    Cited By

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    This article is cited by 10 publications.

    1. Muhammad A. Kamel, Aleksei S. Lobasov, Surya Narayan, Konstantin S. Pervunin, Christos N. Markides. Hydrate Growth over a Sessile Drop of Water in Cyclopentane. Crystal Growth & Design 2023, 23 (6) , 4273-4284. https://doi.org/10.1021/acs.cgd.3c00087
    2. Miguel Pineda, Anh Phan, Carolyn Ann Koh, Alberto Striolo, Michail Stamatakis. Stochastic Cellular Automata Modeling of CO2 Hydrate Growth and Morphology. Crystal Growth & Design 2023, 23 (6) , 4222-4239. https://doi.org/10.1021/acs.cgd.3c00045
    3. Saphir Venet, Patrick Bouriat, Subahong Yusufujiang, Catherine Monge-Daugé, Daniel Broseta, Ross Brown. Crystal Dewetting at the Water–Guest Interface in Macropores Sidesteps the Hydrate Mass-Transfer Bottleneck. Crystal Growth & Design 2023, 23 (5) , 3144-3153. https://doi.org/10.1021/acs.cgd.2c01313
    4. Alberto Striolo, Shanshan Huang. Upcoming Transformations in Integrated Energy/Chemicals Sectors: Some Challenges and Several Opportunities. The Journal of Physical Chemistry C 2022, 126 (51) , 21527-21541. https://doi.org/10.1021/acs.jpcc.2c05192
    5. Min Li, Zhenhe Jian, Aliakbar Hassanpouryouzband, Lunxiang Zhang. Understanding Hysteresis and Gas Trapping in Dissociating Hydrate-Bearing Sediments Using Pore Network Modeling and Three-Dimensional Imaging. Energy & Fuels 2022, 36 (18) , 10572-10582. https://doi.org/10.1021/acs.energyfuels.2c01306
    6. Rui Ma, Senbo Xiao, Yuanhao Chang, Yuequn Fu, Jianying He, Zhiliang Zhang. An interfacial gas-enrichment strategy for mitigating hydrate adhesion and blockage. Chemical Engineering Journal 2023, 453 , 139918. https://doi.org/10.1016/j.cej.2022.139918
    7. Joshua E. Worley, Jose G. Delgado-Linares, Carolyn A. Koh. Dual functionality of ultralow levels of a model kinetic hydrate inhibitor on hydrate particle morphology and interparticle force. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2022, 652 , 129825. https://doi.org/10.1016/j.colsurfa.2022.129825
    8. Saeid Sinehbaghizadeh, Agus Saptoro, Amir H. Mohammadi. CO2 hydrate properties and applications: A state of the art. Progress in Energy and Combustion Science 2022, 93 , 101026. https://doi.org/10.1016/j.pecs.2022.101026
    9. Marshall A. Pickarts, Sriram Ravichandran, Nur Aminatulmimi Ismail, Hannah M. Stoner, Jose Delgado-Linares, E. Dendy Sloan, Carolyn A. Koh. Perspective on the oil-dominated gas hydrate plugging conceptual picture as applied to transient Shut-In/Restart. Fuel 2022, 324 , 124606. https://doi.org/10.1016/j.fuel.2022.124606
    10. Anh Phan, Hannah M. Stoner, Michail Stamatakis, Carolyn A. Koh, Alberto Striolo. Surface morphology effects on clathrate hydrate wettability. Journal of Colloid and Interface Science 2022, 611 , 421-431. https://doi.org/10.1016/j.jcis.2021.12.083

    Langmuir

    Cite this: Langmuir 2021, 37, 42, 12447–12456
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.langmuir.1c02136
    Published October 13, 2021
    Copyright © 2021 American Chemical Society

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