4.7 Article

High resolution MRI studies of CO2 hydrate formation and dissociation near the gas-water interface

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 425, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.131426

Keywords

CO2 hydrate; Hydrate film; Gas-water interface; Dissociation rate; MRI

Funding

  1. National Science Foundation of China [51676025, 52076030, 52020105007]
  2. National Key Research and Development Plan of China [2017YFC0307300]
  3. Innovation Foundation of Science and Technology of Dalian [2019J11CY012]
  4. Fundamental Research Funds for Central Universities [DUT19TD29, DUT21ZD103]

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Gas hydrates are considered promising for gas storage, energy transportation, and seawater desalination. Using MRI, researchers were able to non-invasively image the formation of opaque hydrates from CO2 and water in a cylindrical vessel at low temperature and high pressure. They observed dense hydrate layers forming consistently at the gas-water interface, porous hydrate layers above it, and complex dendritic formations in the water phase below.
Gas hydrates are widely considered as promising candidates for gas storage, energy transportation and seawater desalination. Critical to such applications is a detailed 3D understanding of hydrate formation. To this end, we employ magnetic resonance imaging (MRI) to non-invasively image the gradual formation of opaque hydrate from CO2 and water in a cylindrical vessel at 1 degrees C and as a function of pressure between 2.0 and 3.5 MPa. A 200 mu m thick dense hydrate layer is consistently observed to form at the gas-water interface accompanied by a similar to 1.4 mm thick porous hydrate layer above it and frequently complex dendritic hydrate formation in the water phase below it. Dissociation is observed to occur preferentially via the thick hydrate layer with the initial hydrate film retained largely intact for an extended period of time. The sequential images of hydrate dissociation inside the water phase are most consistent with a vertical heat and mass transfer controlled hydrate dissociation process. The observed difference between the hydrates formed above and inside the water phase is of mechanistic value in understanding these complex interfacial phase transitions.

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