Title: Mixed Polyanionic NaFe$_{1.6}$V$_{0.4}$(PO$_{4}$)(SO$_{4}$)$_{2}$@CNT Cathode for Sodium-ion Batteries: Electrochemical Diffusion Kinetics and Distribution of Relaxation Time Analysis at Different Temperatures

Abstract: We report the electrochemical sodium-ion kiinetics and distribution of relaxation time (DRT) analysis of a newly designed mixed polyanionic NaFe$_{1.6}$V$_{0.4}$(PO$_{4}$)(SO$_{4}$)$_{2}$@CNT composite as a cathode. The specific capacity of 104 mAhg$^{-1}$ is observed at 0.1~C with the average working voltage of $\sim$3~V. Intriguingly, a remarkable rate capability and reversibility are demonstrated up to very high current rate of 25~C. The long cycling test up to 10~C shows high capacity retention even after 2000 cycles. The detailed analysis of galvanostatic intermittent titration technique (GITT) and cyclic voltammetry (CV) data reveal the diffusion coefficient of 10$^{-8}$--10$^{-11}$ cm$^{2}$s$^{-1}$. We find excellent stability in the thermal testing between 25--55$^\circ$C temperatures and 80\% capacity retention up to 100 cycles at 5~C. Further, we analyse the individual electrochemical processes in the time domain using the novel DRT technique at different temperatures. The {\it ex-situ} investigation shows the stable and reversible structure, morphology and electronic states of the long cycled cathode material. More importantly, we demonstrate relatively high specific energy of $\approx$155 Wh kg$^{-1}$ (considering the total active material loading of both the electrodes) at 0.2~C for full cell battery having excellent rate capability up to 10~C and long cyclic stability at 1~C.