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Diffusivity and solubility of methane in ice Ih

机译：甲烷在冰上的扩散和溶解度

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Diffusivity and solubility of gas molecules in crystalline water ice are fundamental parameters to understand physicochemical processes in various environments in space, icy bodies, planets, and the Earth. For instance, diffusion and solubility of methane in ice Ih could constrain the methane flux from sub-surface Martian ice, and could be used to discuss diffusive elemental fractionation of gases trapped in polar ice cores that could disturb the reconstruction of the Earth's paleoatmosphere. The diffusion coefficient and the solubility of methane in ice Ih, however, have not yet been directly determined. In this study, we performed diffusive degassing experiments of helium and methane from ice Ih at 251-259 K to measure both the diffusion coefficient and solubility of methane in ice Ih. We first determined the diffusion coefficient and solubility of helium in ice Ih, and could successfully reproduce those reported in previous studies. We then determined the diffusion coefficient of methane in ice Ih, and the obtained diffusion coefficient of methane at 257 K was (5.2 +/- 1.4) x 10(-11) m(2) s(-1). This is well consistent with that estimated by a molecular-dynamics simulation, where methane molecules do not diffuse through interstitial sites but by breaking hydrogen bonds between H2O molecules. The methane solubility in ice Ih was estimated to be (7.2 +/- 1.1) x 10(-7 )mol mol(H2O)(-1) MPa-1 at 257 K, which is smaller than those of He and Ne and could be due to a larger van der Waals radius of methane than those of light noble gases.
机译：气体分子在结晶水中的扩散和溶解度是了解太空，冰冷的身体，行星和地球的各种环境中的物理化学过程的基本参数。例如，甲烷在冰Ih中的扩散和溶解度可以限制来自子表面火星冰的甲烷通量，并且可用于讨论被困在极地冰芯中的气体的扩散元素分级，这可能会扰乱地球古卫星的重建。然而，甲烷在冰I中的扩散系数和溶解度尚未直接确定。在这项研究中，我们在251-259k中从冰Ih进行氦和甲烷的扩散脱气实验，以测量甲烷在冰I中的扩散系数和溶解度。我们首先确定了冰Ih中氦的扩散系数和溶解度，并且可以成功再现先前研究报告的那些。然后，我们确定冰Ih中的甲烷的扩散系数，并且在257 k下获得的甲烷的扩散系数是（5.2 +/- 1.4）×10（-11）m（2）s（-1）。这与分子动力学模拟的估计良好，其中甲烷分子不会通过间质部位扩散，而是通过在H 2 O分子之间破坏氢键。冰Ih中的甲烷溶解度估计为（7.2 +/- 1.1）×10（-7）摩尔摩（H 2 O）（ - 1）MPa-1，在257 k处，比他和NE的那些由于甲烷的较大范德·甲烷半径而不是轻质惰性气体。

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