4.6 Article

Enhancing Hydrogen Cluster Storage in Clathrate Hydrates via Defect-Mediated Lattice Engineering

期刊

JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 3, 页码 1767-1773

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c10508

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资金

  1. National Research Foundation of Korea (NRF) - Korea government (MSIT) [2020R1A2C2008619]
  2. NRF - MSIT [NRF-2016M2B2A4911795]
  3. POSTECH
  4. National Research Foundation of Korea [2020R1A2C2008619] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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By irradiating the lattice of clathrate hydrates with protons, it is possible to enhance the interactions between the host water frameworks and guest molecules, leading to improved occupation of guest molecules. Experimental results show that proton irradiation can create artificial defects on host water molecules, resulting in better accommodation of guest molecules, while the roles of secondary guest molecules in lattice elongation of THF hydrates were also examined.
Can we create even more plenty of room at the bottom of the confined nanospaces in clathrate hydrates by tuning the complex interactions between the host water frameworks and guest molecules? Because the lattice of the clathrate hydrate is stabilized by van der Waals forces between the host and guest, irradiating the lattice of the clathrate hydrate with energetic particles is anticipated to introduce artificial defects on the host water molecules, resulting in creating a better occupation of guest molecules. Here, we explored the effects of proton irradiation on the intermolecular hydrogen and intramolecular polar covalent bonds in the host frameworks of THF hydrates. The distinct roles of the secondary guest molecules in the lattice elongation of the proton irradiated THF hydrates were examined experimentally. Conclusively, multiple occupations of H-2 in small cages was observed at moderate pressure and temperature conditions following H-2 reloading of the lattice elongated THF hydrate.

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