Issue 35, 2024

High-entropy configuration of O3-type layered transition-metal oxide cathode with high-voltage stability for sodium-ion batteries

Abstract

The O3-type cathode of NaNi0.4Fe0.2Mn0.4O2 stands out for its remarkable theoretical capacity, straightforward production process, affordability, and ecological compatibility for sodium-ion batteries. Nonetheless, the cycle stability of the cathode material is suboptimal. The slippage of the transition metal layers during the charging and discharging process leads to structural instability, and the elevated charging voltages (notably around 4.2 V) initiate the oxygen redox activities, leading to a sustained loss of oxygen ions and irreversible structural degradation. This work pioneers the utilization of a co-substitution strategy with titanium and antimony, fostering a high-entropy configuration of a new O3-type layered oxide cathode of NaNi0.35Fe0.2Mn0.3Ti0.1Sb0.05O2. It meticulously examines the potential effects of Ti4+ and Sb5+ substitution on the electrochemical performance of the cathode, including the role of the high-entropy configuration in modulating the phase transitions throughout the charging and discharging processes. Importantly, the designed cathode of NaNi0.35Fe0.2Mn0.3Ti0.1Sb0.05O2 showcased superior discharge-specific capacity (183.3 mA h g−1 at 0.1C in the voltage range of 1.9–4.1 V), improved cycle stability (with a capacity retention of 76.0% after 200 cycles at 1C), robust rate capability (76.3 mA h g−1 at 10C) and exceptional high-voltage resilience (213 mA h g−1 at 0.1C and capacity retention of 74.0% after 100 cycles at 1C in the voltage range of 1.7–4.3 V). This work articulates a strategic approach for the deliberate design of entropy-regulated cathode materials, aiming at the enhancement of the high voltage stability of cathode materials for sodium-ion batteries.

Graphical abstract: High-entropy configuration of O3-type layered transition-metal oxide cathode with high-voltage stability for sodium-ion batteries

Supplementary files

Article information

Article type
Paper
Submitted
24 Jun 2024
Accepted
28 Jul 2024
First published
31 Jul 2024

J. Mater. Chem. A, 2024,12, 23495-23505

High-entropy configuration of O3-type layered transition-metal oxide cathode with high-voltage stability for sodium-ion batteries

L. Liu, Y. Xin, Y. Wang, X. Ding, Q. Zhou, Z. Wang, W. Huang and H. Gao, J. Mater. Chem. A, 2024, 12, 23495 DOI: 10.1039/D4TA04371E

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