Ultrafast Preparation of High‐Entropy NASICON Cathode Enables Stabilized Multielectron Redox and Wide‐Temperature (−50–60 °C) Workability in Sodium‐Ion Batteries
Abstract
Abstract Avoiding severe structural distortion, irreversible phase transition, and realizing the stabilized multielectron redox are vital for promoting the development of high‐performance NASICON‐type cathode materials for sodium‐ion batteries (SIBs). Herein, a high‐entropy Na 3.45 V 0.4 Fe 0.4 Ti 0.4 Mn 0.45 Cr 0.35 (PO 4 ) 3 (HE‐Na 3.45 TMP) cathode material is prepared by ultrafast high‐temperature shock, which inhibits the possibility of phase separation and achieves reversible and stable multielectron transfer of 2.4/2.8 e − at voltage range of 2.0–4.45/1.5–4.45 V versus Na + /Na (the capacity of 137.2/162.0 mAh g −1 ). The galvanostatic charge/discharge and in‐situ X‐ray diffraction tests indicate the sequential redox reactions and approximate solid solution phase transition behavior of HE‐Na 3.45 TMP. Density functional theory calculations analyze the migration pathways and energy barriers, further confirming the superior reaction kinetics of HE‐Na 3.45 TMP. Accordingly, the HE‐Na 3.45 TMP exhibits outstanding wide temperature applicability and can operate stably in the temperature range of −50–60 °C, accompanied by a capacity retention of 92.8% after 400 cycles at −40 °C and a capacity of 73.7 mAh g −1 even at −50 °C. The assembled hard carbon//HE‐Na 3.45 TMP full‐cell offers an energy density of ≈301 Wh kg −1 based on total cathode and anode active mass, verifying the application feasibility of HE‐Na 3.45 TMP. This work provides an innovative and ultrafast pathway to rationally fabricate high‐performance cathodes for SIBs.
Article Details
Authors (13)
Miao Du
State Key Laboratory of Integrated Optoelectronics and MOE Key Laboratory for UV Light-Emitting Materials and Technology, Department of Physics
Kai Li
Ning Yu
Department of Chemistry
Ze‐Lin Hao
State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory for UV Light‐Emitting Materials and Technology, Department of Physics Northeast Normal University Changchun China
Jin‐Zhi Guo
State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory for UV Light‐Emitting Materials and Technology, Department of Physics Northeast Normal University Changchun China
Hao‐Jie Liang
MOE Key Laboratory for UV Light‐Emitting Materials and Technology Department of Physics Northeast Normal University Changchun 130024 P. R. China
Zhen‐Yi Gu
MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China
Xiao‐Hua Zhang
State Key Laboratory of Metastable Materials Science and Technology and Key Laboratory for Microstructural Material Physics of Hebei Province, School of Science Yanshan University Qinhuangdao China
Kai‐Yang Zhang
MOE Key Laboratory for UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin 130024 P.R. China
Yan Liu
Jia‐Lin Yang
State Key Laboratory of Integrated Optoelectronics MOE Key Laboratory for UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin China
Yi‐Tong Liu
Department of Chemistry Northeast Normal University Changchun 130024 P. R. China
Xing‐Long Wu
MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China