2004
DOI: 10.1021/jp0310955
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In Situ Raman Spectroscopy Investigation of the Dissociation of Methane Hydrate at Temperatures Just below the Ice Point

Abstract: Dissociation kinetics of methane hydrates was investigated by using in situ Raman spectroscopy at temperatures just below the melting point of ice. Measurements of decomposition rates were performed using finely powdered hydrate samples with a diameter range of 100-250 µm. It was found that the dissociation rate of methane hydrate at 0.1 MPa is considerably faster than that at 0.25 and 0.5 MPa. A kinetic model using non steadystate approximation and a diffusion-controlled regime is presented for describing the… Show more

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Cited by 61 publications
(47 citation statements)
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“…When hydrate dissociates at temperatures below the freezing point of ice (<273.2 K) yet outside the hydrate region of stability, unexpectedly slow rate of hydrate dissociation is observed, which is a phenomenon termed as ''self-preservation'' or ''anomalous preservation'' in the literature [85][86][87]. The most popular explanation for the phenomenon is that the endothermic heat of dissociation causes the dissociated water to form ice, preventing further dissociation within the hydrate region.…”
Section: Self-preservation Phenomenamentioning
confidence: 99%
“…When hydrate dissociates at temperatures below the freezing point of ice (<273.2 K) yet outside the hydrate region of stability, unexpectedly slow rate of hydrate dissociation is observed, which is a phenomenon termed as ''self-preservation'' or ''anomalous preservation'' in the literature [85][86][87]. The most popular explanation for the phenomenon is that the endothermic heat of dissociation causes the dissociated water to form ice, preventing further dissociation within the hydrate region.…”
Section: Self-preservation Phenomenamentioning
confidence: 99%
“…Methane gas release from hydrate decomposition was also observed with high-resolution optical microscopy, which offered some information on 2-D gas/water rearrangements during hydrate decomposition [Katsuki et al, 2008]. In-situ Raman spectroscopy was found helpful in observing the decomposition of hydrates by providing time-resolved spectra for CH 4 molecules encaged in hydrate cavities during hydrate decomposition [Komai et al, 2004;Liu et al, 2008], but powerless in illustrating Geochemistry, Geophysics, Geosystems 10.1002/2016GC006521 detailed morphological characteristics of decomposing hydrates in pores. Cryo scanning electron microscopy (cryo-SEM) allows a more detailed access of surface properties down to the nanometer scale on recovered samples, which has been extremely useful for the observation of GHs and ice surfaces [Falenty et al, 2014;Kuhs et al, 2000].…”
Section: Introductionmentioning
confidence: 99%
“…Komai et al 37 performed a series of experiments to analyze the kinetics of MH dissociation via in situ Raman spectroscopy. Several methods have recently been used to monitor methane hydrate (MH) dissociation directly, such as magnetic resonance imaging (MRI), Raman spectroscopy, scanning electron microscopy (SEM), and X-ray computed tomography (CT).…”
Section: Introductionmentioning
confidence: 99%