Attachment of Li(+) ion on graphene surface to realize Li(+)-ion conductor is a real challenge because of the weak interaction between the ions and the functional groups of graphene oxide; although, a large number of theoretical results are already available in the literature. To overcome this problem, graphene oxide is functionalized by 1-aza-15-crown-5, the cage-like structure containing four oxygens that can bind Li(+) ion through electrostatic interaction. Li(+) migration on graphene surface has been investigated using ac relaxation mechanism. Perfect Debye-type relaxation behavior with β (relaxation exponent) value ≈1 resulting from single ion is observed. The activation energy of Li(+) migration arising due to cation-π interaction is found to be 0.37 eV, which agrees well with recently reported theoretical value. It is believed that this study will help to design isolated ion conductors for Li(+)-ion battery.
The increasing demand of sodium ion batteries (SIBs) remarkably accelerates the study of solid-state sodium ion conductors due to their potential application as solid-state electrolytes in SIBs. In the present work, the sodium ion is attached to reduced graphene oxide (rGO) to realize a sodium ion conductor. Tuning the activation energy of migration for Na+ and Li+ ions on rGO surface is investigated by varying the concentration of both ions. The lowest values of activation energies for Na+ and Li+ conduction are found to be 0.28 eV and 0.37 eV, respectively. It is seen that the activation energy of migration of the Na+ ion is smaller than that of the Li+ ion. The lower positive charge density of Na+ compared to Li+ causes this lowering of activation energy in Na+ due to the comparatively weak cation–π interaction between the Na+ ion and the carbon hexagon. From the relaxation study, the relaxation exponent (β) value of the Na+ ion is found to be smaller than that of the Li+ ion. This deviation from Debye-type relaxation behavior of the Na+ ion also agrees well with the decreasing value of activation energy as mentioned above. We hope that this study will aid the design of ion conductors for solid-state SIBs.
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