Abstract: The current disclosure is directed to a hydrogen-storage system that employs catalytic dehydrogenation of low-molecular-weight amines in a hydrogen reactor. The hydrogen-storage system comprises aliphatic amines and di-amines as organic carriers that store hydrogen covalently, a hydrogen reactor that releases and separates hydrogen gas from the carrier, and metal or metal-oxide catalysts that promote a dehydrogenation reaction to release hydrogen. In certain implementations, a metal or metal-oxide catalyst may be carried on high-surface-area support materials, such as gamma-alumina and metal-organic-framework materials, to enhance catalytic properties. The hydrogen reactor may be a packed-bed reactor, a monolith reactor, or a flow-through hydrogen-membrane reactor.