Ultra-high hydrogen storage capacity of holey graphyne

Holey graphyne (HGY), a novel two-dementional 2D single-crystalline carbon allotrope, was recently synthesized by Castro-Stephens coupling reaction. The naturally existing uniform periodic holes in the 2D carbon-carbon network demonstrate its promising potential in the energy storage. Herein, we conducted density functional theory (DFT) calculation to predict the hydrogen storage capacity of HGY sheet. It is found the Li-decorated single-layer HGY can serve as a promising candidate for hydrogen storage. Our DFT calculations demonstrate that Li atoms can bind strongly to the HGY sheet without the formation of Li clusters, and each Li atom can anchor four H2 molecules with the average adsorption energy about 0.22 eV/H2. The largest hydrogen storage capacity of the doped HGY sheet can reach as high as 12.8 wt%, largely surpassing the target of the U. S. DOE (9 wt%), showing the Li/HGY complex is an ideal hydrogen storage material at ambient conditions. In addition, we investigate the polarization mechanism of the storage media and find that the polarization is originated from both the electric field induced by the ionic Li decorated on the HGY and the weak polarized hydrogen molecules dominated the H2 adsorption process.