Binding energy of gas molecule with two pyrazine molecules as organic linker in meal-organic framework : its theoretical evaluation and understanding of determining factors
Binding energy of gas molecule with two pyrazine molecules as organic linker in meal-organic framework : its theoretical evaluation and understanding of determining factors
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气体分子与两个吡嗪分子作为有机连接体的金属-有机骨架的结合能：其理论评估和对决定因素的理解
DOI：
10.1007/s00214-011-1025-6
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发表时间：
2011
期刊：
影响因子：
--
通讯作者：
S.Sakaki
中科院分区：
文献类型：
--
作者：
M.Deshmukh;S.Sakaki
研究了H2、CH 4、C2 H4、C2 H6、CO2和CS2等气体分子夹在两个吡嗪分子之间的相互作用.本文采用MP2.5/aug-cc-pVTZ方法，因为该方法计算的结合能与CCSD（T）/aug-cc-pVDZ方法计算的结合能几乎相同，并考虑了MP2.5对aug-cc-pVTZ基组的扩展效应。气体分子的结合能按H2<CH 4 < CO2<C2 H4 ≈ C2 H6 < CS2的顺序增加。对相互作用能的能量分解分析表明，静电项在Hartree-Fock能级上对相互作用能的贡献最大。然而，色散相互作用提供了主要贡献的总结合能在相关水平。我们新发现了气体分子极化率的z分量与色散能之间的线性关系，其中z轴取为垂直于两个Pz环。这些结果有助于理解和预测气体分子与有机连接基团的结合能。
We explored the interactions of gas molecules such as H2, CH4, C2H4, C2H6, CO2, and CS2sandwiched by two pyrazine (Pz) molecules, which were employed as a model of organic linker in the Hofmann-type metal–organic framework (MOF). The MP2.5/aug-cc-pVTZ method was employed here, because this method presents almost the same binding energy as that calculated by the CCSD(T)/aug-cc-pVDZ with MP2.5-evaluated basis set extension effects to aug-cc-pVTZ basis set. The binding energy of the gas molecule increases in the order H2< CH4< CO2< C2H4≈ C2H6< CS2. The energy decomposition analysis of the interaction energy indicates that the electrostatic term presents the largest contribution to the interaction energy at the Hartree–Fock level. However, the dispersion interaction provides dominant contribution to the total binding energy at correlated level. We newly found a linear correlation between thez-component of polarizability of gas molecules and dispersion energy, where thez-axis was taken to be perpendicular to two Pz rings. These results are useful for understanding and predicting the binding energy of the gas molecule with the organic linkers of MOF.