Dept. of Applied Sciences, Haldia Institute of Technology, Haldia 721657, India Dept. of Chemical Engineering, Haldia Institute of Technology, Haldia 721657, India Dept. of Chemistry, Faculty of Science, Tokyo University of Science, Tokyo 1628601, Japan. * Corresponding Email: (MKG) kantimrinal88@gmail.com; (GR) grm.chem@gmail.com This article deals with the different types of the hydrogen storage process, its thermochemistry, adsorption process, and binding energy, in the light of the computational approach using the conceptual density functional theory (CDFT). This article expresses the view that lithium iodide (LiI) is a viable template for hydrogen storage at low temperatures. The density functional theory (DFT) has been used to investigate the structure and chemical reactivity of the resulting templates. The adsorption process is found to be quasi-sorption in nature. The molecular hydrogen interacts with building blocks (with Li centre) through electrovalent interaction and a single LiI molecule is capable of absorbing 10 H2 with a high gravimetric wt% value (13.07 wt%) which is found to be a promising system as per standard. The changes in Gibbs free energy indicate that hydrogen adsorption can occur spontaneously at cryogenic temperatures.