A density functional theory study of hydrogen adsorption in MOF-5
A density functional theory study of hydrogen adsorption in MOF-5
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DOI：
10.1021/jp051202q
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发表时间：
2005-09-29
影响因子：
3.3
通讯作者：
Ceder, G
中科院分区：
文献类型：
--
作者：
Mueller, T;Ceder, G
采用密度泛函理论的广义梯度近似下的从头算分子动力学和基态弛豫方法研究了分子氢与分子式为Zn_4 O（O_2C-C_6 H_4-CO_2）的金属有机骨架之间的相互作用。五个对称的独特的吸附位点被确定，计算表明，与氢的相互作用最强的网站位于附近的Zn 4 O团簇。20个总的吸附位点被发现周围的每个Zn 4 O簇，但其中16个被填充后，在其余四个网站的相互作用能下降福尔斯关闭显着。氢在孔壁上的吸附在孔中心为氢产生吸引势阱。计算了骨架对有机连接体的物理结构和电子结构的影响，提出了骨架与氢之间的相互作用可以被修改的方法。
Ab initio molecular dynamics in the generalized gradient approximation to density functional theory and ground-state relaxations are used to study the interaction between molecular hydrogen and the metal-organic framework with formula unit Zn4O(O2C-C6H4-CO2)(3). Five symmetrically unique adsorption sites are identified, and calculations indicate that the sites with the strongest interaction with hydrogen are located near the Zn4O clusters. Twenty total adsorption sites are found around each Zn4O cluster, but after 16 of these are populated, the interaction energy at the remaining four sites falls off significantly. The adsorption of hydrogen on the pore walls creates an attractive potential well for hydrogen in the center of the pore. The effect of the framework on the physical structure and electronic structure of the organic linker is calculated, suggesting ways by which the interaction between the framework and hydrogen could be modified.