Cobalt-Free Layered LiNi_0.8Mn_0.15Al_0.05O₂/Graphene Aerogel Composite Electrode for Next-Generation Li-Ion Batteries

In this work, we introduce LiNi_0.8Mn_0.15Al_0.05O₂ (NMA), which is cobalt-free and has a high nickel content, and a conductive composite material to NMA by supporting it with a three-dimensional (3D) graphene aerogel (GA). With an easy freeze-drying approach, NMA nanoparticles are properly dispersed on graphene sheets, and GA creates a strong and conductive framework, significantly improving the structure and conductivity. The structure of the pure NMA and NMA/graphene aerogel (NMA/GA) composite was investigated by X-ray diffraction (XRD) and field emission scanning electron microscopy (FE-SEM). XRD and FE-SEM analyses clearly indicated that ultrapure NMA structures are homogeneously dispersed among the GAs. In addition, the composite structure was examined using transmission electron microscopy (TEM) to determine the dispersion mechanisms. The electrochemical cycling performance of the pure NMA and NMA/GA composite was evaluated by rate capacitance, cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). The synthesized NMA/GA was able to provide 89.81% specific capacity retention after the 500th cycle at C/2. The average charge/discharge rates of the obtained cathode show good electrochemical results and exhibit capacities of 190.2,186.3, 185.2, 176.2, 161.2,142.6, and 188.5 mAh g^-1 at C/20, C/10, C/5, C, 3C, 5C, and C/20, respectively. EIS data showed an improvement in the impedance of the composite containing GA. According to the results of the electrochemical tests, NMA nanoparticles formed a conductive network with its porous structure thanks to GA, formed a protective layer on the surface, prevented the side reactions between the cathode and the electrolyte, decreased the impedance of the cathode, and increased the redox kinetics. In addition, the changes in the structure were investigated in the NMA/GA composite cathode by XRD, FE-SEM, and Raman analyses at the end of the 50th, 250th, and 500th cycles. In summary, the NMA/GA cathode is expected to play an important role in lithium-ion batteries (LIBs) by taking advantage of its easy synthesis and excellent cycle stability.