Accumulating electrical energy in decentralized electrical grids is a demanding task. Preliminary work exists on the charging and discharging of liquid organic hydrogen carriers (LOHCs). These carriers allow the storage of hydrogen by reversible hydrogenation of an aromatic compound. A challenge is that the chemical process has to be conducted within the power-generating infrastructure, and therefore, continuous and fully automated implementation is mandatory. In this work, the fundamentals of controlling and automating LOHC-based energy-storage systems are presented. For this purpose, the identification of the controlled variable is performed before its influence on the reaction dynamics is determined. This results in a fully automated hydrogenation process, whereby the conductibility of the reaction, the performance, and the necessity of applying pressure pulsations to get a stable operation mode are shown. Derived from these results, the investigations help to establish LOHCs as feasible hydrogen carriers, which will be a decisive step to mid- and long-term energy-storage systems suitable to a modern smart-grid infrastructure.