Two-Dimensional Films Based on Graphene/Li4Ti5O12 and Carbon Nanotube/Li4Ti5O12 Nanocomposites as a Prospective Material for Lithium-Ion Batteries: Insight from Ab Initio Modeling

The combination of spinel Li4Ti5O12 (LTO) with carbon nanostructures, such as graphene (G) and carbon nanotubes (CNTs), provides all of the required properties for modern chemical power sources such as Li-ion batteries (LIBs) and supercapacitors (SCs). G/LTO and CNT/LTO composites demonstrate a superior reversible capacity, cycling stability, and good rate performances. In this paper, an ab initio attempt to estimate the electronic and capacitive properties of such composites was made for the first time. It was found that the interaction between LTO particles and CNTs was higher than that with graphene due to the larger amount of transfer charge. Increasing the graphene concentration raised the Fermi level and enhanced the conductive properties of G/LTO composites. For CNT/LTO samples, the radius of CNT did not affect the Fermi level. For both G/LTO and CNT/LTO composites, an increase in the carbon ratio resulted in a similar reduction in quantum capacitance (QC). It was observed that during the charge cycle in the real experiment, the non-Faradaic process prevailed during the charge cycle, while the Faradaic process prevailed during the discharge cycle. The obtained results confirm and explain the experimental data and improve the understanding of the processes occurring in G/LTO and CNT/LTO composites for their usages in LIBs and SCs.

Automated summary

Combining spinel Li4Ti5O12 (LTO) with carbon nanostructures such as graphene (G) and carbon nanotubes (CNTs) provides the required properties for Li-ion batteries (LIBs) and supercapacitors (SCs). G/LTO and CNT/LTO composites show excellent reversible capacity, cycling stability, and rate performances. This study presents an ab initio estimation of the electronic and capacitive properties of these composites for the first time, revealing the interaction between LTO particles and carbon nanostructures. The results improve the understanding of the processes occurring in G/LTO and CNT/LTO composites for their applications in LIBs and SCs.