RESUMO
We report an effective approach of utilizing multiwalled carbon nanotubes (MWCNTs) as an active anode material in sodium ion batteries by expanding the interlayer distance in a few outer layers of multiwalled carbon nanotubes. The performance enhancement was investigated using a density functional tight binding (DFTB) molecular dynamics simulation. It is found that a sodium atom forms a stable bonding with the partially expanded MWCNT (PECNT) with the binding energy of -1.50 eV based on the density functional theory calculation with van der Waals correction, where a sodium atom is caged between the two carbon hexagons in the two consecutive MWCNTs. Wave function and charge density analyses show that this binding is physisorption in nature. This larger exothermic nature of binding energy favors the stable bonding between the PECNT and a sodium atom, and thereby, it helps to enhance the electrochemical performance. In the experimental works, partial opening of the MWCNT with the expanded interlayer has been designed by the well-known Hummer's method. It has been found that the introduction of functional groups causes a partial opening of the outer few layers of a MWCNT, with the inner core remaining undisturbed. The enhanced performance is due to an expanded interlayer of carbon nanotubes, which provide sufficient active sites for the sodium ions to adsorb as well as to intercalate into the carbon structure. The PECNT shows a high specific capacity of 510 mAh g-1 at a current density of 20 mA g-1, which is about 2.3 times the specific capacity obtained for a pristine MWCNT at the same current density. This specific capacity is higher when compared to other carbon-based materials. The PECNT also shows a satisfactory cyclic stability at a current density of 200 mA g-1 for 100 cycles. Based on our experimental and theoretical results, an alternative perspective for the storage of sodium ions in MWCNTs is proposed.