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The results of studies on the hydrogen accumulation, storage and release systems differing in the type of hydrogen interaction with the material (medium) used for hydrogen storage are analyzed. Published data on the use of polycyclic hydrocarbons as the basis for hydrogen storage in a chemically bound state are summarized. Substrate-structure-dependent differences between the mechanisms of heterogeneous catalytic hydrogenation reactions of mono- and polycyclic aromatic hydrocarbons with hydrogen storage capacity > 7 mass% and dehydrogenation of corresponding polycyclic naphthenes are discussed. The bibliography includes 188 references.