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Direct transition mechanism for molecular diffusion in gas hydrates

机译:天然气水合物分子扩散的直接转变机制

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摘要

Several mechanisms for transport of gases inside hydrates have been proposed in the literature. Previous results have pointed out the apparent impossibility of some guests passing directly through faces connecting adjacent cages without destroying the water structure. Alternative diffusion mechanisms were proposed, such the participation of an additional guest (help-gas) or a water-hopping displacement of defects in the lattice. In this work, we use dual cage explicit atomic systems, where the position of some external atoms are fixed, to demonstrate theoretically that direct transitions are feasible through hexagonal and pentagonal faces in type I hydrate, for both carbon dioxide and methane, without compromising the overall structure integrity. Our DFT calculations show that even in the case that some bonds break during the transition, all of them are recovered, because the face distortion is absorbed locally by the hydrogen bond network. This result opens the door to improve the description of transport mechanisms of guest molecules by means of direct inter-cage transitions.
机译:在文献中提出了在水合物内部运输气体的几种机制。以前的结果指出,一些客人直接通过连接相邻笼子的面孔而不会破坏水结构的表观不可能。提出了替代的扩散机制,使额外的客人(帮助 - 气)的参与或晶格中的缺陷的跳水位移。在这项工作中,我们使用双笼式显式原子系统,其中一些外部原子的位置是固定的,从理论上证明直接过渡通过I型水合物中的六角形和五角形面部可行,用于二氧化碳和甲烷,而不会损害整体结构完整性。我们的DFT计算表明,即使在过渡期间的某些粘合断裂的情况下,也被恢复,因为面部失真被氢键网络局部吸收。该结果打开门,以通过直接的笼式转换来改善客体分子的传输机制的描述。

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