Stability and electronic structure of carbon capsules with superior gas storage properties: A theoretical study

Highlights: • Stability and electronic structure of various carbon capsules are studied. • Effects of capsule's sizes on electronic and optical properties are explored. • Changes in cohesive and formation energy and electronic gap are discussed. • Capsule's gas storage propensity is addressed using DFT and ab initio MD. • Capsule's optical absorptions are discussed with and without stored gas molecules. - Abstract: Structures, electronic and optical properties of carbon nanocapsules of varying sizes (length and diameter) are studied using first-principles density functional theory. Based on calculated cohesive energy, formation energy, electronic gap and extent of orbital delocalization, we examine structural stability and changes in low-energy physics of these carbon capsules. We find that both cohesive and formation energy decrease with increase in capsule's sizes, indicating their greater structural rigidity and favorable formation feasibility. The electronic gap also decreases with increase in capsule's sizes due to the larger electronic delocalization. The simulated optical absorption spectra show lowering of low-energy peak positions with increase in the capsule's dimensions, consistent with the reduction in electronic gap. Additionally, we also provide an estimate of gas storage capacity for the larger carbon capsule (C460) considered. We find 7.69 wt.% and 28.08 wt.% storage propensity for hydrogen and carbon dioxide gases, respectively, which clearly suggests their potential use as light storage materials