Computational design of tetrahedral silsesquioxane-based porous frameworks with diamond-like structure as hydrogen storage materials

XD Li and H Zhang and Y Miyamoto and YJ Tang and CY Wang, STRUCTURAL CHEMISTRY, 25, 177-185 (2014).

DOI: 10.1007/s11224-013-0267-4

A novel type of three-dimensional (3D) tetrahedral silsesquioxane-based porous frameworks (TSFs) with diamond-like structure was computationally designed using the density functional theory (DFT) and classical molecular mechanics (MM) calculations. The hydrogen adsorption and diffusion properties of these TSFs were evaluated by the methods of grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations. The results reveal that all designed materials possess extremely high porosity (87-93 %) and large H-2 accessible surface areas (5,268-6,544 m(2) g(-1)). Impressively, the GCMC simulation results demonstrate that at 77 K and 100 bar, TSF-2 has the highest gravimetric H-2 capacity of 29.80 wt%, while TSF-1 has the highest volumetric H-2 uptake of 65.32 g L-1. At the same time, the gravimetric H-2 uptake of TSF-2 can reach up to 4.28 wt% at the room temperature. The extraordinary performances of these TSF materials in hydrogen storage made them enter the rank of the top hydrogen storage materials so far.

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