AbstractThe Mg–Si–H system is economically favorable as a hydrogen storage medium for renewable energy systems while moving toward sustainable energy production. Hydrogen desorption from MgH2 in the presence of Si is achievable, forming magnesium silicide (Mg2Si). However, absorbing hydrogen into Mg2Si remains problematic due to severe kinetic limitations. The objective of this study is to reduce these kinetic limitations by synthesizing Mg2Si nanoparticles to limit the migration distance for magnesium atoms from the Mg2Si matrix to produce MgH2 and Si, thus improving the reversibility of the Mg–Si–H system. Mg2Si nanoparticles were synthesized using a reduction reaction undertaken by solid–liquid mechanochemical ball milling. Particle size was controlled by adding a reaction buffer (lithium chloride) to the starting reagents to restrict particle growth during milling. The reaction buffer was removed from the nanoparticles using tetrahydrofuran and small-angle X-ray scattering revealed an average Mg2Si particle size of ∼10 nm, the smallest Mg2Si nanoparticles synthesized to date. High-pressure hydrogen measurements were undertaken above thermodynamic equilibrium at a range of temperatures to attempt hydrogen absorption into the Mg2Si nanoparticles. X-ray diffraction results indicate that partial hydrogen absorption took place. Under these absorption conditions bulk Mg2Si cannot absorb hydrogen, demonstrating the kinetic benefit of nanoscopic Mg2Si.