Heterogeneous NASICON‐Type Cathode With Reversible Multielectron Reaction for High‐Performance Sodium‐Ion Batteries

Author:

Zhu Lin1,Xiang Shuang1,Wang Miaomiao1,Sun Dan1,Huang Xiaobing2,Li Yixin1,Tang Yougen1,Peng Zhiguang1,Zhang Qi1,Wang Haiyan1ORCID

Affiliation:

1. Hunan Provincial Key Laboratory of Chemical Power Sources College of Chemistry and Chemical Engineering Central South University Changsha 410083 P. R. China

2. College of Chemistry and Materials Engineering Hunan University of Arts and Science Hunan 415000 P. R. China

Abstract

AbstractNa superionic conductor (NASICON)‐structured compounds demonstrate great application potential by their robust framework and compositional diversity. However, they are blamed for the mediocre energy density, and achieving both multielectron reaction and good cycling stability simultaneously is challenging. Herein, a novel heterogeneous Na4Fe3(PO4)2(P2O7)/Na2VTi(PO4)3 (NFPP/NVTP) material with stable multielectron reaction is constructed by spray drying technology. The mutual promotion effect of intergrowth structures effectively improves the purity and the crystallization of NFPP/NVTP during the fabrication process, which is beneficial to the high capacity and cycling stability. As a result, the optimized NFPP/NVTP demonstrates a high reversible capacity of 155.3 mAh g−1 at 20 mA g−1 and outstanding cycling stability with 82.9% capacity retention over 2500 cycles at 1 A g−1, which are much superior to those of NFPP and NVTP individually. Even in full cell configuration, the energy density remains high at ≈380 Wh kg−1 based on the cathode mass. The high capacity of NFPP/NVTP is also attributed to the successive reduction/oxidation mechanism involving the introduction of Ti3+ and interfacial charge redistribution effect between the heterogeneous phases, which greatly improve the electronic and ionic conductivity. Moreover, high reversible structural evolution during the multisodium storage process further guarantees excellent cycling stability.

Funder

National Natural Science Foundation of China

Publisher

Wiley

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