This research uses theoretical techniques to investigate the interaction of hydrogen with light metal nanostructures and assemblies to identify materials suitable for high capacity hydrogen storage. Using Density Functional Theory methods, we calculate the structures and stabilities of novel light metal clusters and assemblies. We also theoretically simulate the physical and chemical interaction of hydrogen with these novel assemblies, identifying transition states and calculating reaction energetics.

Reaction barriers and enthalpies were determined for dissociative adsorption of H₂ onto both neutral and singly charged clusters Al₁₂X (X = Mg, Al, Si). Quite low barriers are observed for addition of H₂ to Al₁₃⁺ and Al₁₂Mg, however, dissociation of H₂ between closely spaced Al₁₂Mg clusters proceeds spontaneously. We analyse the trends in barriers and enthalpies in terms of the progression from 38 valence electrons in Al₁₂Mg, through to 40 valence electrons in Al₁₂Si, using electron deformation densities and orbital analysis.