title: A Covalent Organic Framework that Exceeds the DOE 2015 Volumetric Target for H2 Uptake at 298 K.
abstract: 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.
authors: 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.
authors: Jose L
authors: JL
authors: Mendoza-Cortes
authors: 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.
authors: William A
authors: WA
authors: Goddard
authors: 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.
authors: Hiroyasu
authors: H
authors: Furukawa
authors: 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.
authors: Omar M
authors: OM
authors: Yaghi
keywords: COF; Grand Canonical Monte Carlo; Hydrogen storage; MP2; force field; metalation; multiscale; quantum mechanics; sorption isotherm; transition metals