High-Entropy O3-Phase Cathodes with Enhanced Diffusion Kinetics and Lattice Stability for High-Power Na-Ion Batteries

O3-phase layered oxide cathodes have been considered as the most promising candidates for high-energy Na-ion batteries (SIBs) due to their high reversible specific capacity, yet the detrimental OP2 phase transition with severe c-axis contraction at high operating voltages hampers its power performance. Herein, we design and synthesize a novel high-entropy O3-phase cathodes, Na1.0(Ni0.4Fe0.2Mn0.4)0.83Zn0.06Cu0.01Ti0.08Ca0.02O2, with a configurational entropy of 1.53R. This high-entropy design significantly broadens the Na-ion diffusion channels and effectively mitigates c-axis contraction by stabilizing the lattice structure and suppressing phase transitions, thereby facilitating rapid Na-ion transport throughout the charge/discharge process. Consequently, the as-obtained cathode delivers a high specific capacity of 161.8 mAh g–1 at 0.1 C within 2.0–4.2 V and maintains a capacity of 122.1 mAh g–1 even at 5 C with a twofold improvement. In addition, 80.1% of initial capacity is retained after 100 cycles at 1 C, markedly higher than that of the counterpart (40.0%). These results highlight the critical role of high-entropy design in stabilizing the O3-phase cathodes for high-power SIBs.

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Publication Details

Journal
Industrial & Engineering Chemistry Research
Published
2025-09-03
DOI
https://doi.org/10.1021/acs.iecr.5c02686
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
0.00

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article

High-Entropy O3-Phase Cathodes with Enhanced Diffusion Kinetics and Lattice Stability for High-Power Na-Ion Batteries

Qilin Cheng, Muslum Demi̇r, Chenke Zhang, Hao Jiang et al.
Industrial & Engineering Chemistry Research
Advancements in Battery Materials
article

High-Entropy O3-Phase Cathodes with Enhanced Diffusion Kinetics and Lattice Stability for High-Power Na-Ion Batteries

Qilin Cheng, Muslum Demi̇r, Chenke Zhang, Hao Jiang, Ling Chen, Haifeng Yu
article en

Abstract

O3-phase layered oxide cathodes have been considered as the most promising candidates for high-energy Na-ion batteries (SIBs) due to their high reversible specific capacity, yet the detrimental OP2 phase transition with severe c-axis contraction at high operating voltages hampers its power performance. Herein, we design and synthesize a novel high-entropy O3-phase cathodes, Na1.0(Ni0.4Fe0.2Mn0.4)0.83Zn0.06Cu0.01Ti0.08Ca0.02O2, with a configurational entropy of 1.53R. This high-entropy design significantly broadens the Na-ion diffusion channels and effectively mitigates c-axis contraction by stabilizing the lattice structure and suppressing phase transitions, thereby facilitating rapid Na-ion transport throughout the charge/discharge process. Consequently, the as-obtained cathode delivers a high specific capacity of 161.8 mAh g–1 at 0.1 C within 2.0–4.2 V and maintains a capacity of 122.1 mAh g–1 even at 5 C with a twofold improvement. In addition, 80.1% of initial capacity is retained after 100 cycles at 1 C, markedly higher than that of the counterpart (40.0%). These results highlight the critical role of high-entropy design in stabilizing the O3-phase cathodes for high-power SIBs.

Industrial & Engineering Chemistry ResearchVol. 64(37)
East China University of Science and Technology (CN), Nanomaterials Research (United States) (US), Boğaziçi University (TR)
National Natural Science Foundation of China, Fundamental Research Funds for the Central Universities
Openalex Percentile: Top 78%
Advancements in Battery Materials
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