Abstract
We performed first-principle molecular dynamics (FPMD) calculations to test the total attraction force on a physisorbed molecule at a given temperature and ambient pressure and applied it to the hydrogen storage on the 2D material MoP2. We considered a pristine material and one with 12.5% of Mo vacancies. By optimization, we calculated a gravimetric capacity for pristine MoP2 of 5.72%, with an adsorption energy of -0.13 eV/molecule. We found 6.02% and -0.14 eV/molecule for the defective surface. Next, we applied our approach to determine if the molecular hydrogen physisorption obtained by simple energy optimization exists for a given temperature and ambient pressure. We used this approach to determine the number of molecules adsorbed on the surface at a given temperature. Thus, we conducted a FPMD calculation at temperature T(1), using optimization as the initial system configuration. Subsequently, we performed a second FPMD calculation at a temperature T(2) (with T(2) << T(1)), using the steady configuration of the first FPMD calculation as the initial configuration. We identified as adsorbed molecules at temperature T(1,) only those forced back toward the surface at temperature T(2) due to kinetic energy loss at the lower temperature. The defective surface gave the best gravimetric capacity, ranging from 5.27% at 300 K to 6.02% at 77 K. The latter met the requirement from the US-DOE, indicating the potential practical application of our research in hydrogen storage.