In recent years, high-entropy alloys have been proposed as potential hydrogen storage materials. Despite a number of experimental efforts, there is a lack of theoretical understanding regarding the hydrogen absorption behavior of high-entropy alloys. In this work, the hydrogen storage properties of a new TiZrHfScMo high-entropy alloy are investigated. This material is synthesized successfully, and its structure is characterized as body-centered cubic. Based on density functional theory, the lattice constant, formation enthalpy, binding energy, and electronic properties of hydrogenated TiZrHfScMo are all calculated. The calculations reveal that the process of hydrogenation is an exothermic process, and the bonding between the hydrogen and metal elements are of covalent character. In the hydrogenated TiZrHfScMo, the Ti and Sc atoms lose electrons and Mo atoms gain electrons. As the H content increases, the <Ti⁻H> bonding is weakened, and the <Hf⁻H> and <Mo⁻H> bonding are strengthened. Our calculations demonstrate that the TiZrHfScMo high-entropy alloy is a promising hydrogen storage material, and different alloy elements play different roles in the hydrogen absorption process.
Keywords: DFT; high-entropy alloys; hydrogenation; overlap population; projected density of state.