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基于密度泛函理论以及ADF/SCM软件,利用GGA-D-PBE-D3(Perdew-Burke-Ernzerhof)/TZP基组对包含重烷烃分子的sH型水合物的稳定性进行了研究。基于量子化学原理,分别对sH型水合物中的小、中、大笼进行了结构优化计算,进而计算了笼子的结合能(binding energy)。计算结果表明,重烷烃分子在CH_4分子作为辅助气体分子时可以形成稳定的sH型水合物,其中CH_4占据小笼和中笼,重烷烃分子占据大笼。研究发现,大笼的结合能处于由2条平行线构成的狭窄区域内。计算结果与现有的试验结果有很好的一致性。
Based on the density functional theory (DFT) and the ADF / SCM software, the stability of sH-containing hydrate containing heavy alkanes was studied by using the GDE-D-PBE-D3 / PerkinElmer- Based on the principle of quantum chemistry, the structural optimization of small, medium and large cages in sH hydrate were calculated respectively, and then the binding energy of cages was calculated. The calculation results show that the heavy alkane molecules can form stable sH hydrates when CH_4 molecules act as auxiliary gas molecules, of which CH_4 occupies small cages and middle cages, and heavy alkanes occupy large cages. The study found that large cage binding can be in the narrow area formed by two parallel lines. The calculated results are in good agreement with the existing test results.