This study is focused on the development of liquid organic hydrogen carriers (LOHC) based on N-heterocyclic compounds. These LOHC-substrates are attractive for their lower hydrogen extraction temperature compared to cycloalkanes, which is caused by the low enthalpy of the dehydrogenation reaction of the N-heterocyclic compounds. The low hydrogen extraction temperature, as well as the low volatility of the heterocycles, provide high purity hydrogen from the reaction. Under similar reaction conditions, the comparison of the efficacy of three promising heterocycles (1-methyl-octahydroindole (8HMI), tetradecahydrophenazine and decahydroquinoline) was carried out in the presence of palladium-containing catalysts. As a result, the advantages of using catalysts supported by alumina, and the high perspectivity of the 8MHI application as a LOHC-substrate, were shown. The dehydrogenation of 8HMI in the presence of 1 wt.% Pd/Al₂O₃ allowed for reaching a 100% yield in hydrogen under the conditions of the standard catalytic test (1 h, 240 °C). In order to study the high reactivity of 8HMI, thermodynamic dehydrogenation reaction profiles were computationally evaluated, which showed that 8HMI was the most energetically preferred in the field of hydrogen storage from the studied heterocyclic compounds.