Hydrogen absorption in intermetallic compounds from first principles

Intermetallic compounds such as {A₂B₇} alloys are promising candidates for mobile hydrogen storage applications due to their high and reversible hydrogen absorption capacity. We compute the absorption isotherm of {Nd₃MgNi₁₄} from first-principles using a multiscale modeling approach. Absorption sites are identified through a systematic geometrical analysis, and are characterized with Density Functional Theory (DFT) calculations. The absorption site properties are used in room-temperature Grand Canonical Monte Carlo simulations to predict hydrogen uptake as a function of pressure, leading to a full absorption isotherm in good agreement with experimental data. We show that both hybrid exchange-correlation functionals and zero-point energy corrections are necessary to obtain accurate absorption properties. The analysis of the fully hydrogenated structure with DFT shows considerable volume expansion, which stabilizes the structure at large hydrogen content.