Structural and electronic properties of Li-adsorbed single and bilayer porphyrin sheets as an electrode material for energy storage devices – a DFT analysis

In this study, we adopt density functional theory (DFT) to investigate the structural and electronic properties of monolayer and bilayer 2-D porphyrin sheets (PS) of covalent organic frameworks (COFs) upon interaction with Li atoms as an electrode material for Li-ion batteries. Based on their mechanical properties, our systems exhibit remarkable stability. The adsorption of Li at various sites in the monolayer, including over and between the bilayers of PS, is investigated. Our results indicate that Li at site S3 has the highest adsorption energy, and Li is energetically preferred to intercalate within the bilayer rather than monolayers due to its high adsorption energies. Notably, the charge transfer remains consistent for both systems. The density of state distribution, charge density difference plots, spin density and the band structure results show that the PS has high electrical conductivity. Additionally, the reaction potential was carried out, and the negative reaction potential results demonstrate that the system undergoes a reduction reaction. The resultant theoretical capacity and the open circuit voltage highlight that the PS materials of COFs are an important step for use in the next generation high-performance lithium-ion batteries.