First-Principles Study of Hydrogen Storage of Sc-Modified Semiconductor Covalent Organic Framework-1

[Image: see text] At present, the development of new carbon-based nanoporous materials with semiconductor properties and high hydrogen storage capacity has become a research hotspot in the field of hydrogen storage and hydrogen supply. Here, we pioneered the study of the hydrogen storage capacity of a scandium (Sc) atom-modified semiconductor covalent organic framework-1 (COF-1) layer. It was found that the hydrogen storage capacity of the COF-1 structure was significantly enhanced after the modification of the Sc atom. We found that each Sc atom of the modified COF-1 structure can stably adsorb up to four H(2) molecules, and the average adsorption energy of the four hydrogen molecules is −0.284 eV/H(2). Six Sc atoms are stably adsorbed most bilaterally on the cell of the COF-1 unit, which can adsorb 24 H(2) molecules in total. In addition, we have further studied the adsorption and desorption behaviors of H(2) molecules on the 6Sc-COF-1 surface at 300 and 400 K, respectively. It can be found that each Sc atom of the COF-1 unit cell can stably adsorb three H(2) molecules with a hydrogen storage performance of 5.23 wt % at 300 K, which is higher than those of lithium-modified phosphorene (4.4 wt %) and lithium-substituted BHNH sheets (3.16 wt %). At 400 K, all of the adsorbed H(2) molecules are released. This confirms the excellent reversibility of 6Sc-COF-1 in hydrogen storage performance. This research has great significance in the application of fuel cells, surpassing traditional hydrogen storage materials.