4.6 Article

Effect of Ammonia on Methane Hydrate Stability under High-Pressure and High-Temperature Conditions

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JOURNAL OF PHYSICAL CHEMISTRY A
卷 124, 期 51, 页码 10890-10896

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AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.0c09652

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  1. Photon Factory, High Energy Accelerator Research Organization [2018G524, 2020G544, 2018G569]
  2. JSPS Kakenhi programs [19J01467, 19K14815]
  3. Joint Usage/Research Center PRIUS, Ehime University, Japan [2019A18 and 2020A07]

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High-pressure experiments were conducted to investigate the stability and phase transition of methane hydrate (MH) in the water-methane-ammonia system at room-to-high temperatures employing Raman spectroscopy and synchrotron X-ray powder diffraction, in combination with an externally heated diamond anvil cell. The results revealed that, at room temperature, MH undergoes phase transitions from MH-I to MH-II at similar to 1.0 GPa and from MH-II to MH-III at similar to 2.0 GPa. These transition behaviors are consistent with those in the water-methane system, which indicates that ammonia has a negligible effect on a series of phase transitions of MH. Contrarily, a sequential in situ Raman spectroscopy revealed that ammonia affects the stability of MH-III under high pressure and high temperature: the dissociation temperature of MH-III was more than 10 K lower in the water-methane-ammonia system than in the water-methane system. These findings aid in improving the internal structural models of icy bodies and estimating the origin of their atmospheric methane.

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