The storage of H2 in a safe and compact form represents a significant current challenge,[1] and there is wide-ranging interest in materials that can store and release H2 with fast kinetics and high reversibility over multiple cycles.[2] Porous coordination frameworks have become competitors to other porous materials, such as zeolites [3] and carbon materials (for example, activated carbon or nanotubes),[4] with recent studies confirming that these ...