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| sH型CO2水合物的稳定性分析 |
| Stability analysis of CO2 sH hydrate |
| 投稿时间：2016-09-08 |
| DOI：10.13259/j.cnki.eri.2019.02.007 |
| 中文关键词: 密度泛函理论 sH型水合物 CO2 分子动力学模拟 稳定性 |
| 英文关键词:density function theory sH hydrate CO2 molecular dynamics (MD) simulation stability |
| 基金项目: |
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| 中文摘要: |
| 基于密度泛函理论并利用ADF/ME软件，在GGA-PBE（Perdew-Burke-Ernzerhof）/TZP基组下对sH型水合物进行了第一性原理计算。在等温等容（NVT）系综下，利用分子动力学（MD）模拟方法得到了sH型水合物的初始结构。基于量子化学原理，对sH型水合物的大笼、中笼、小笼进行了几何结构优化，根据计算得到的单点能量得到了笼子的总能量。对比计算了包含不同客体分子的笼子的稳定能和范德华相互作用能，计算结果表明：在sH型水合物中，CO2既不能置换大笼中的环庚烷，也不能置换小笼、中笼中的甲烷。但是，每个大笼可以通过包含2个CO2分子的形式形成sH型水合物。 |
| 英文摘要: |
| Based on density functional theory and ADF/ME software, the first-principle calculations were performed on the sH hydrate at GGA-PBE (Perdew-Burke-Ernzerhof)/TZP level. Under the constant temperature and constant volume NVT system, molecular dynamics (MD) simulation was carried out to obtain the equilibrium molecular structures of the sH hydrate cages. Based on the principles of quantum chemistry, the geometry optimizations of the small, medium and large cages of sH hydrate were carried out. The total energies of the cages were obtained according to the single point energy. Comparisons of the stabilization and Van de Walls interaction energies of the cages with different guest molecules were conducted. The calculation results showed that CO2 couldn't replace cycloheptane molecules in the large cages and CH4 molecules in the small and medium cages of sH hydrate. However, CO2 might form sH hydrate by occupying the large cages with two CO2 molecules per cage. |
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