Tsai Y.-JCHIN-LUNG KUO2022-03-222022-03-22202200134686https://www.scopus.com/inward/record.uri?eid=2-s2.0-85121262555&doi=10.1016%2fj.electacta.2021.139719&partnerID=40&md5=b47f40b48f1f75974f9f64016d1b9d45https://scholars.lib.ntu.edu.tw/handle/123456789/598349We performed first-principles calculations to investigate the effect of N-doping on the electronic structure property and the Li/Na storage behaviors of graphene nanomaterials. Our calculations first revealed that the N-doping treatment can effectively increase the number of C vacancy defects in graphene and the adsorption energy of a Li/Na atom on C vacancy can be largely enhanced by increasing the pyridinic-/pyrrolic-N atoms at the vacancy site. However, the reversible Li/Na capacity of the C vacancy defect was found to be largely reduced by increasing the doping level of N, which was primarily determined by the electronic structure property of the N-doped graphene structures and their strong electrostatic interactions with Li/Na. Our results clearly revealed that the enhanced Li/Na capacity by the N-doping on the graphene surface can be primarily attributed to the induced formation of a great number of C vacancy defects rather than the presence of the pyridinic-/pyrrolic-N on the basal plane. Our calculations also showed that the pyridinic-N doped graphene edges can possess a Li/Na capacity comparable to that of the N-doped C vacancy defects. Nevertheless, this excess Li/Na capacity was found to be largely reduced by the termination of the H atoms on these edge pyridinic-N groups. ? 2021 Elsevier LtdElectronic structure of the N-doped defective graphene structureFirst-principles calculationsLi and Na storage on grapheneN-doped graphene nanomaterialsAtomsCalculationsDoping (additives)GrapheneNanostructured materialsStructural propertiesElectronic.structureFirst principle calculationsLi and na storage on grapheneN-dopedN-doped graphene nanomaterialN-DopingPyridinicVacancy DefectsElectronic structureThe effect of N-doping on the electronic structure property and the li and Na storage capacity of graphene nanomaterials: A first-principles studyjournal article10.1016/j.electacta.2021.1397192-s2.0-85121262555