Unraveling Mixed Hydrate Formation: Microscopic Insights into Early Stage Behavior

Hall, Kyle Wm.; Zhang, Zhengcai; Kusalik, Peter G.

doi:10.1021/acs.jpcb.6b11961

Cited by 18 publications

(43 citation statements)

References 34 publications

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“…Ordering in stages is also a well-documented feature of gas hydrate nucleation. For example, we have previously observed an amorphous phase that intermediates the solution and gas hydrate crystalline phases in our gas hydrate nucleation simulations [18,58,114], consistent with the observations in other MD simulations using different molecular models [17,18,33,35,55,[115][116][117][118][119]. The formation of an amorphous phase has also been reported in an experimental study of gas hydrates [120].…”

Section: Ordering In Stage and Funnel-shaped Energy Landscapesupporting

confidence: 91%

“…the 5 12 6 n -4 1 5 10 6 m cages where n = 0, 2, 3, 4 and m = 2, 3, 4), it is becoming increasingly clear that there is a plethora of transient cages from which more common and more stable cages arise as hydrate nucleation proceeds, again strongly indicating ordering in stages. For example, early on in the nucleation process, irregular and defective cages are prominent structural features, and appear in interfacial regions between the solution phase and the hydrate nucleus [119]. An ordering-in-stages perspective on gas hydrate nucleation is also supported by the fact that nascent ordering according to water-based molecular-level order parameters apparently precedes the appearance of cages, suggesting that lower level ordering (e.g.…”

Section: Ordering In Stage and Funnel-shaped Energy Landscapementioning

confidence: 99%

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Characterizing key features in the formation of ice and gas hydrate systems

Liang

Hall

Laaksonen

et al. 2019

Phil. Trans. R. Soc. A.

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Crystallization in liquids is critical to a range of important processes occurring in physics, chemistry and life sciences. In this article, we review our efforts towards understanding the crystallization mechanisms, where we focus on theoretical modelling and molecular simulations applied to ice and gas hydrate systems. We discuss the order parameters used to characterize molecular ordering processes and how different order parameters offer different perspectives of the underlying mechanisms of crystallization. With extensive simulations of water and gas hydrate systems, we have revealed unexpected defective structures and demonstrated their important roles in crystallization processes. Nucleation of gas hydrates can in most cases be characterized to take place in a two-step mechanism where the nucleation occurs via intermediate metastable precursors, which gradually reorganizes to a stable crystalline phase. We have examined the potential energy landscapes explored by systems during nucleation, and have shown that these landscapes are rugged and funnel-shaped. These insights provide a new framework for understanding nucleation phenomena that has not been addressed in classical nucleation theory. This article is part of the theme issue ‘The physics and chemistry of ice: scaffolding across scales, from the viability of life to the formation of planets’.

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Section: Ordering In Stage and Funnel-shaped Energy Landscapesupporting

confidence: 91%

Section: Ordering In Stage and Funnel-shaped Energy Landscapementioning

confidence: 99%

Characterizing key features in the formation of ice and gas hydrate systems

Liang

Hall

Laaksonen

et al. 2019

Phil. Trans. R. Soc. A.

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“…To confirm this, we carried out a hydrate cage identification procedure which has been widely used to determine various types of clathrate cages [64,[74][75][76]. The hydrate cage morphology is characterized based on the hydrogen-bonded networks and the structure of the rings they assemble [77].…”

Section: Thf Storage In the Growing Hydratementioning

confidence: 99%

Molecular mechanisms by which tetrahydrofuran affects CO2 hydrate Growth: Implications for carbon storage

Phan

Schlösser

Striolo

2021

Chemical Engineering Journal

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This is a PDF file of an article that has undergone enhancements after acceptance, such as the addition of a cover page and metadata, and formatting for readability, but it is not yet the definitive version of record. This version will undergo additional copyediting, typesetting and review before it is published in its final form, but we are providing this version to give early visibility of the article. Please note that, during the production process, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

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“…However, stirring the solution (37) which appears to be counterproductive to all of these key steps, can often promote clathrate formation. As another example, adding extra certain chemicals (e.g., H 2 S, CO 2 , THF) (23,(38)(39)(40) can lead to various effects on clathrate formation, while the underlying mechanisms are still largely unknown. Hence, an improved model on how to characterize the nucleation pathway is called for, not only to explain the experimental phenomena mentioned above, but also to offer theoretical guidance for the development of new ways to control the nucleation and growth of clathrate hydrates.…”

Section: Significancementioning

confidence: 99%

Unraveling nucleation pathway in methane clathrate formation

Zhong

Yan

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

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Methane clathrates are widespread on the ocean floor of the Earth. A better understanding of methane clathrate formation has important implications for natural-gas exploitation, storage, and transportation. A key step toward understanding clathrate formation is hydrate nucleation, which has been suggested to involve multiple evolution pathways. Herein, a unique nucleation/growth pathway for methane clathrate formation has been identified by analyzing the trajectories of large-scale molecular dynamics (MD) simulations. In particular, ternary water-ring aggregations (TWRAs) have been identified as fundamental structures for characterizing the nucleation pathway. Based on this nucleation pathway, the critical nucleus size and nucleation timescale can be quantitatively determined. Specifically, a methane hydration layer compression/shedding process is observed to be the critical step in (and driving) the nucleation/growth pathway, which is manifested through overlapping/compression of the surrounding hydration layers of the methane molecules, followed by detachment (shedding) of the hydration layer. As such, an effective way to control methane hydrate nucleation is to alter the hydration layer compression/shedding process during the course of nucleation.

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Unraveling Mixed Hydrate Formation: Microscopic Insights into Early Stage Behavior

Cited by 18 publications

References 34 publications

Characterizing key features in the formation of ice and gas hydrate systems

Characterizing key features in the formation of ice and gas hydrate systems

Molecular mechanisms by which tetrahydrofuran affects CO2 hydrate Growth: Implications for carbon storage

Unraveling nucleation pathway in methane clathrate formation

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