Decoding the Superior Lithium‐Ion Storage Capabilities of Oligoaniline‐Derived Anodes

ABSTRACT The development of high‐performance anodes is critical for advancing lithium‐ion battery (LIB) technology, and oligoaniline‐based materials, such as tri‐aniline (T3) and tetra‐aniline (T4), have emerged as promising candidates due to their unique electrochemical properties. These materials offer multiple redox‐active sites, enabling efficient charge storage and reversible lithium‐ion intercalation, while their intrinsic conductivity facilitates rapid electron transport. T3 demonstrates better cycling stability and delivers the outstanding specific capacity of 964.14 mAh g −1 at 100 mA g −1 and 721.09 mAh g −1 at a high current density of 1 A g −1 , alongside a higher specific capacity compared to T4. The galvanostatic intermittent titration technique (GITT) reveals enhanced diffusion coefficients of 10 −11 cm 2 s −1 for T3 and 10 −12 cm 2 s −1 for T4. In situ electrochemical impedance spectroscopy (EIS) and distribution of relaxation times (DRT) analysis indicate a thinner solid‐electrolyte interphase (SEI) layer, reduced charge transfer resistance, and a lower Li + activation energy in T3, attributed to its higher electrical conductivity. These features collectively result in better transport properties, positioning T3 as a competitive anode material. To further support the experimental findings, density functional theory (DFT) calculations were conducted on both materials. This paper provides a comprehensive evaluation of T3 and T4, highlighting their potential to address key challenges in high‐performance LIBs.