Physisorption in porous materials is a promising route to meet molecular hydrogen (H2) storage and delivery requirements for transportation because it is both fast and fully reversible at mild conditions. However, most current candidates have binding enthalpies to H2 that are too small, which lead to volumetric capacity at 298 K of less than 10 g/L compared to the system target of 40 g/L. Using accurate quantum mechanical (QM) methods, we determine the H2 binding enthalpy of 48 compounds (5 linkers and 11 different transition metals) used for porous covalent organic frameworks (COF) which we metalated with different transition metals (TM), including first row TM (Sc though Cu) and precious TM (Pd and Pt). We showed that first row TM give similar and sometimes superior van der Waals interactions with H2 than precious TMs. Based on these results, we constructed 26 new COFs based on these linkers and we determine the uptake using force fields (FF) based on QM and grand canonical Monte Carlo simulations. We determined new COFs that reach the DOE 2017 target of 40 g/L. This work highlights the designing principles for the optimal interaction enthalpy in the next generation of H2 storage materials.

Design principles to exceed the DOE 2017 standards for delivery and storage of H<sub>2</sub> at room temperature using nitrogen bases covalent organic frameworks

248th National Meeting (2014)

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Design principles to exceed the DOE 2017 standards for delivery and storage of H2 at room temperature using nitrogen bases covalent organic frameworks

Design principles to exceed the DOE 2017 standards for delivery and storage of H₂ at room temperature using nitrogen bases covalent organic frameworks