Mendoza-Cortes Jose L, Goddard William A, Furukawa Hiroyasu, Yaghi Omar M
Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91106, United States.
Center for Reticular Chemistry, Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States.
J Phys Chem Lett. 2012 Sep 20;3(18):2671-5. doi: 10.1021/jz301000m. Epub 2012 Sep 10.
Physisorption in porous materials is a promising approach for meeting H2 storage requirements for the transportation industry, because it is both fully reversible and fast at mild conditions. However, most current candidates lead to H2 binding energies that are too weak (leading to volumetric capacity at 298 K of <10 g/L compared to the DOE 2015 Target of 40 g/L). Using accurate quantum mechanical (QM) methods, we studied the H2 binding energy to 48 compounds based on various metalated analogues of five common linkers for covalent organic frameworks (COFs). Considering the first transition row metals (Sc though Cu) plus Pd and Pt, we find that the new COF-301-PdCl2 reaches 60 g total H2/L at 100 bar, which is 1.5 times the DOE 2015 target of 40 g/L and close to the ultimate (2050) target of 70 g/L. The best current materials, MOF-200 and MOF-177, are predicted to store 7.6 g/L (0.54 wt % excess) and 9.6 g/L (0.87 wt % excess), respectively, at 298 K and 100 bar compared with 60 g/L (4.2 wt % excess) for COF-301-PdCl2.
多孔材料中的物理吸附是满足交通运输行业氢气存储要求的一种很有前景的方法，因为它在温和条件下既完全可逆又快速。然而，目前的大多数候选材料导致氢气结合能过弱（导致在298 K时的体积容量<10 g/L，而美国能源部2015年的目标是40 g/L）。我们使用精确的量子力学（QM）方法，基于共价有机框架（COF）的五种常见连接体的各种金属化类似物，研究了氢气与48种化合物的结合能。考虑到第一过渡系金属（从Sc到Cu）加上Pd和Pt，我们发现新型的COF-301-PdCl2在100 bar下的总氢气存储量达到60 g/L，是美国能源部2015年40 g/L目标的1.5倍，接近2050年70 g/L的最终目标。预计目前最好的材料MOF-200和MOF-177在298 K和100 bar下分别存储7.6 g/L（过量0.54 wt%）和9.6 g/L（过量0.87 wt%），而COF-301-PdCl2为60 g/L（过量4.2 wt%）。
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