Reversible hydrogen-storage at reduced temperatures in the intermetallic compound Mg6(Ni,Pd)

A rapidly-solidified Mg–Ni–Pd alloy is shown to exhibit reversible hydrogen-storage of 5 mass % H at a temperature of 473 K, nearly 100 K below temperatures typically required for Mg-based alloys, with an equilibrium absorption plateau near 1 atm H2 pressure. Additionally, a single plateau is observed in the pressure–composition isotherm where MgH2 and Mg2NiH4 form and decompose simultaneously during the absorption/desorption process. The increase in absorption plateau pressure to 100 kPa suggests a decrease in the free energy by as much as 15 kJ/mol resulting from either a decrease in enthalpy or an increase in entropy of reaction between the hydride and metallic phases. The improved thermodynamics are discussed in terms of the formation of a new equilibrium metallic phase, Mg6(Ni,Pd). The phase alters the thermodynamics of the hydriding reaction, allowing both MgH2 and Mg2NiH4 to form cooperatively in a single reaction. This method for reducing the free energy of the hydriding reaction is promising, and may prove useful in a variety of other metal-hydride hydrogen-storage systems.

► An Mg–Ni–Pd alloy exhibits reversible hydriding at 473 K and 1 bar H2 pressure.
► The formation of Mg6(Ni,Pd) creates new pathways for the hydriding reaction.
► Both MgH2 and Mg2NiH4 form simultaneously from Mg6(Ni,Pd).
► The enthalpy of reaction of hydride formation is reduced by up to 20%.