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Research Article

Unraveling nucleation pathway in methane clathrate formation

Liwen Li, Jie Zhong, Youguo Yan, Jun Zhang, Jiafang Xu, Joseph S. Francisco, and Xiao Cheng Zeng
PNAS October 6, 2020 117 (40) 24701-24708; first published September 21, 2020; https://doi.org/10.1073/pnas.2011755117
Liwen Li
aSchool of Materials Science and Engineering, China University of Petroleum (East China), 266580 Qingdao, China;
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Jie Zhong
bDepartment of Earth and Environmental Science, University of Pennsylvania, Philadelphia, PA 19104-6316;
cDepartment of Chemistry, University of Pennsylvania, Philadelphia, PA 19104-6316;
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Youguo Yan
aSchool of Materials Science and Engineering, China University of Petroleum (East China), 266580 Qingdao, China;
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Jun Zhang
aSchool of Materials Science and Engineering, China University of Petroleum (East China), 266580 Qingdao, China;
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  • For correspondence: zhangjun.upc@gmail.com xjiafang@upc.edu.cn frjoseph@sas.upenn.edu xzeng1@unl.edu
Jiafang Xu
dSchool of Petroleum Engineering, China University of Petroleum (East China), 266580 Qingdao, China;
eKey Laboratory of Unconventional Oil & Gas Development, China University of Petroleum (East China), Ministry of Education, 266580 Qingdao, China;
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  • For correspondence: zhangjun.upc@gmail.com xjiafang@upc.edu.cn frjoseph@sas.upenn.edu xzeng1@unl.edu
Joseph S. Francisco
bDepartment of Earth and Environmental Science, University of Pennsylvania, Philadelphia, PA 19104-6316;
cDepartment of Chemistry, University of Pennsylvania, Philadelphia, PA 19104-6316;
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  • For correspondence: zhangjun.upc@gmail.com xjiafang@upc.edu.cn frjoseph@sas.upenn.edu xzeng1@unl.edu
Xiao Cheng Zeng
fDepartment of Chemistry, University of Nebraska–Lincoln, Lincoln, NE 68588;
gDepartment of Chemical & Biomolecular Engineering, University of Nebraska–Lincoln, Lincoln, NE 68588
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  • For correspondence: zhangjun.upc@gmail.com xjiafang@upc.edu.cn frjoseph@sas.upenn.edu xzeng1@unl.edu
  1. Contributed by Joseph S. Francisco, August 21, 2020 (sent for review June 11, 2020; reviewed by Jianwen Jiang and Sotiris S. Xantheas)

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Significance

Understanding the clathrate formation mechanism has important implications on natural gas exploitation, storage, and transportation. A key toward clathrate formation is the hydrate nucleation, which involves complex interplay between water and guest molecules at nanoscale and multiple kinetic stages. Herein, by tracing the kinetic evolution of multiple ternary water-ring aggregations based on trajectories of large-scale molecular dynamics simulations, we identified a generic nucleation pathway to clathrate formation. This observed nucleation pathway is driven by numerous compression/shedding processes among the methane hydration layers, and it can explain the widely accepted “blob” model of clathrate nucleation. The molecular insight into the nucleation pathway allows us to quantitatively assess the nucleation timescales as well as the critical nucleus sizes in the clathrate formation.

Abstract

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.

  • methane
  • nucleation
  • clathrate
  • aggregations

Footnotes

  • ↵1L.L. and J. Zhong contributed equally to this work.

  • ↵2To whom correspondence may be addressed. Email: zhangjun.upc{at}gmail.com, xjiafang{at}upc.edu.cn, frjoseph{at}sas.upenn.edu, or xzeng1{at}unl.edu.
  • Author contributions: L.L., J. Zhong, Y.Y., J. Zhang, J.X., J.S.F., and X.C.Z. designed research; J. Zhong, Y.Y., J. Zhang, and X.C.Z. performed research; L.L., J. Zhong, Y.Y., J. Zhang, J.X., J.S.F., and X.C.Z. analyzed data; and L.L., J. Zhong, Y.Y., J. Zhang, J.X., J.S.F., and X.C.Z. wrote the paper.

  • Reviewers: J.J., National University of Singapore; and S.S.X., Pacific Northwest National Laboratory.

  • The authors declare no competing interest.

  • This article contains supporting information online at https://www.pnas.org/lookup/suppl/doi:10.1073/pnas.2011755117/-/DCSupplemental.

Data Availability.

All study data are included in the article and SI Appendix.

Published under the PNAS license.

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Unraveling nucleation pathway in methane clathrate formation
Liwen Li, Jie Zhong, Youguo Yan, Jun Zhang, Jiafang Xu, Joseph S. Francisco, Xiao Cheng Zeng
Proceedings of the National Academy of Sciences Oct 2020, 117 (40) 24701-24708; DOI: 10.1073/pnas.2011755117

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Unraveling nucleation pathway in methane clathrate formation
Liwen Li, Jie Zhong, Youguo Yan, Jun Zhang, Jiafang Xu, Joseph S. Francisco, Xiao Cheng Zeng
Proceedings of the National Academy of Sciences Oct 2020, 117 (40) 24701-24708; DOI: 10.1073/pnas.2011755117
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