Exploring the Interaction between Lithium Ion and Defective Graphene Surface Using Dispersion Corrected DFT Studies

To analyze the lithium ion interaction with realistic graphene surfaces, we carried out dispersion corrected DFT-D3 studies on graphene with common point defects and chemisorbed oxygen containing functional groups along with defect free graphene surface. Our study reveals that, the interaction between lithium ion (Li+) and graphene is mainly through the delocalized π electron of pure graphene layer. However, the oxygen containing functional groups pose high adsorption energy for lithium ion due to the Li-O ionic bond formation. Similarly, the point defect groups interact with lithium ion through possible carbon dangling bonds and/or cation-π type interactions. Overall these defect sites render a preferential site for lithium ions compared with pure graphene layer. Based on these findings, the role of graphene surface defects in lithium battery performance were discussed.