Reversible hydrogenation of nitriles to amines has been proposed as a method of hydrogen storage. Several research groups have demonstrated that acceptorless dehydrogenation of amines can be performed. Furthermore, the reactions were performed with homogeneous catalysts at moderate temperatures of only about 110 °C. This is highly beneficial in terms of efficiency. However, all reported works have been performed in nitrogen atmospheres. The research question to be evaluated in this study is whether it is possible to carry out the reaction at moderate conditions without any inert gas. Reaction thermodynamics, including the calculation of the reaction equilibria with the superimposed phase equilibria, has been analyzed to answer this question. The main conclusion in this regard is that the thermodynamic driving force for dehydrogenation of amines at 110 °C is too low to reach reasonable conversions. The addition of nitrogen dilutes hydrogen, decreasing its partial pressure. This way, near‐vacuum conditions are simulated regarding hydrogen. This shifts equilibrium toward the products. However, a technical hydrogen storage process requires the release of pure hydrogen. A possibility to enable hydrogen release at moderate temperatures and provide pure hydrogen could be the application of electrochemical compression. This technic selectively withdraws hydrogen, making high conversions thermodynamically feasible.