密度泛函理论
氢
金属有机骨架
氢气储存
化学
吸附
结合能
金属
钒
氢键
无机化学
分子
反离子
卤化物
计算化学
材料科学
化学物理
物理化学
离子
有机化学
原子物理学
物理
作者
Romit Chakraborty,Kurtis M. Carsch,David E. Jaramillo,Yuto Yabuuchi,Hiroyasu Furukawa,Jeffrey R. Long,Martin Head-Gordon
标识
DOI:10.26434/chemrxiv-2022-1q37t
摘要
Densifying hydrogen in a metal-organic framework (MOF) at moderate pressures can circumvent challenges associated with high-pressure compression. The highly tunable structural and chemical composition in MOFs affords vast possibilities to optimize binding interactions. At the heart of this search are the nanoscale characteristics of molecular adsorption at the binding site(s). Using density functional theory (DFT) to model binding interactions of hydrogen to the exposed metal site of cation-exchanged MFU-4l, we predict multiple hydrogen ligation of H2 at the first coordination sphere of V(II) in V(II)-exchanged MFU-4l. We find that the strength of this binding between the metal site and \ce{H2} molecules can be tuned by altering the halide counterion adjacent to the metal site and that the fluoride-containing node affords the most favourable interactions for high-density H2 storage. Using energy decomposition analysis, we delineate electronic contributions that enable multiple hydrogen ligation and demonstrate its benefits for hydrogen adsorption and release at modest pressures.
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