高熵P2/O3双相正极的协同设计助力高性能钠离子电池

引用本文: 赵珊, 刘旭, 郭昊天, 柳宗琳, 王鹏飞, 舒杰, 伊廷锋. 高熵P2/O3双相正极的协同设计助力高性能钠离子电池[J]. 物理化学学报, 2026, 42(1): 100129. doi: 10.1016/j.actphy.2025.100129 shu

Citation: Shan Zhao, Xu Liu, Haotian Guo, Zonglin Liu, Pengfei Wang, Jie Shu, Tingfeng Yi. Synergistic design of high-entropy P2/O3 biphasic cathodes for high-performance sodium-ion batteries[J]. Acta Physico-Chimica Sinica, 2026, 42(1): 100129. doi: 10.1016/j.actphy.2025.100129 shu

高熵P2/O3双相正极的协同设计助力高性能钠离子电池

赵珊 ^1, ,
刘旭 ^1, ,
郭昊天 ^1, ,
柳宗琳 ^{1,
,} ,
王鹏飞 ^1, ,
舒杰 ^2, ,
伊廷锋 ^{1,3,
,}

1.
东北大学材料科学与工程学院, 辽宁沈阳 110819;
2.
宁波大学材料科学与化学工程学院, 浙江宁波 315211;
3.
东北大学秦皇岛分校资源与材料学院, 河北省电介质与电解质功能材料重点实验室, 河北秦皇岛 066004

通讯作者: 柳宗琳，Emails:liuzonglin_yoo@163.com; 伊廷锋，Emails:tfyihit@163.com

基金项目:
国家自然科学基金(52374301)；河北省自然科学基金(E2024501010)；石家庄市基础研究计划项目(241790667A)；中央高校基本科研业务费专项基金(N2423013)；河北省自然科学基金(B2024501004)；东北大学秦皇岛分校河北省电介质与电解质功能材料重点实验室绩效补助经费(22567627H)；2025年河北省研究生创新能力培养项目(CXZZSS2025163)资助

摘要: P2型层状过渡金属氧化物(P2-Na_xTMO₂)因其优异的循环稳定性和倍率性能，成为钠离子电池正极材料的有力候选者。然而，其在高电压下的不可逆相变和固有低理论容量问题，阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计来克服这些挑战。通过在P2相高熵基体中引入O3相，构建新型P2/O3双相高熵层状氧化物Na_0.70Ni_0.25Mn_0.35Co_0.15Fe_0.05Ti_0.20O₂ (简称Na_0.70NMCFT)。其中，高熵设计通过构型熵稳定效应有效抑制P2相的不可逆相变，而O3相则通过协同作用弥补容量不足并提升循环稳定性。此外，双相组分之间的相互作用进一步促进P2-O3与P2-P3相变的高度可逆性。Na_0.70NMCFT在1C倍率下的初始放电容量为102.08 mAh g⁻¹，200次循环后容量保持率达88.15%，表明具有优异的循环稳定性。更重要的是，即使在10C的高倍率下，Na_0.70NMCFT仍能提供85.67 mAh g⁻¹的初始放电比容量，并在1000次循环后容量保持率达70%。本工作证实双相高熵设计在提升钠离子电池正极性能中的关键作用，为开发先进钠离子电池正极材料提供了新思路。

关键词:

English

Synergistic design of high-entropy P2/O3 biphasic cathodes for high-performance sodium-ion batteries

Shan Zhao ^1, ,
Xu Liu ^1, ,
Haotian Guo ^1, ,
Zonglin Liu ^{1,
,} ,
Pengfei Wang ^1, ,
Jie Shu ^2, ,
Tingfeng Yi ^{1,3,
,}

1.
School of Materials Science and Engineering, Northeastern University, Shenyang 110819, Liaoning Province, China;
2.
School of Materials Science and Chemical Engineering, Ningbo University, Ningbo 315211, Zhejiang Province, China;
3.
Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province, School of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao 066004, Hebei Province, China

Corresponding author: Zonglin Liu, ; Tingfeng Yi,

Received Date: 27 May 2025
Revised Date: 29 June 2025
Available Online: 08 July 2025

Abstract: P2-type layered transition metal oxides (P2-Na_xTMO₂) have emerged as promising cathodes for sodium-ion batteries (SIBs) owing to their superior cycling stability and excellent rate capability. However, their practical application is significantly hindered by two major challenges. Firstly, irreversible phase transitions occur during high-voltage operation, which disrupt the structural integrity and deteriorate electrochemical performance. Secondly, their inherently low theoretical specific capacity fails to meet modern energy demands. To tackle these challenges, this study proposes a novel synergistic strategy that integrates high-entropy engineering with a biphasic P2/O3 structural design. An innovative cathode material, Na_0.70Ni_0.25Mn_0.35Co_0.15Fe_0.05Ti_0.20O₂ (denoted as Na_0.70NMCFT), was successfully synthesized via a high-temperature solid-state reaction. This material design critically incorporates five distinct transition metal cations into the transition metal (TM) layer, constructing a stabilized high-entropy configuration. Careful optimization of both the five TM elements and the sodium content was essential to precisely regulate the synthesis and formation of the desired integrated P2/O3 biphasic structure within this high-entropy host. Comprehensive structural characterization unequivocally confirms the successful construction of this tailored architecture. X-ray diffraction (XRD) and transmission electron microscopy (TEM) collectively confirm the successful construction of the P2/O3 biphasic architecture. The high-entropy engineering stabilizes the P2 phase through configurational entropy, effectively suppressing irreversible phase transitions and Na⁺/vacancy ordering during cycling, as evidenced by smoother charge/discharge profiles and ex-situ XRD analysis under high potentials. Meanwhile, the introduced O3 phase compensates for capacity shortages and improves cycling stability, working in tandem with the P2 phase. Critically, the interaction between the two phases enables a highly reversible transition between P2/O3-P2/P3, further enhancing the overall performance. Under the combined action of the high-entropy and biphasic strategies, Na_0.70NMCFT exhibits optimal electrochemical performance. It delivers an initial discharge capacity of 102.08 mAh g⁻¹ at 1C, retaining 88.15% after 200 cycles, demonstrating exceptional cycling stability. Moreover, even at 10C, Na_0.70NMCFT still has an initial discharge specific capacity of 85.67 mAh g⁻¹ and a capacity retention of up to 70% after 1,000 cycles. Kinetic analyses further reveal that Na_0.70NMCFT possesses the lowest charge transfer resistance and the highest sodium-ion diffusion coefficient among the materials studied. In conclusion, this work demonstrates that the rational design of biphasic high-entropy cathodes can synergistically achieve superior rate capability, cycling stability, and maintain high theoretical capacity. It not only overcomes the key bottlenecks of P2-type oxides but also paves the way for the development of advanced SIB cathodes, establishing a new paradigm for the engineering of high-performance cathode materials in the field of sodium-ion batteries.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

高熵P2/O3双相正极的协同设计助力高性能钠离子电池

通讯作者: 柳宗琳，Emails:liuzonglin_yoo@163.com; 伊廷锋，Emails:tfyihit@163.com

English

Synergistic design of high-entropy P2/O3 biphasic cathodes for high-performance sodium-ion batteries

Corresponding author: Zonglin Liu, ; Tingfeng Yi,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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中国化学会秘书处

高熵P2/O3双相正极的协同设计助力高性能钠离子电池

通讯作者: 柳宗琳，Emails:liuzonglin_yoo@163.com; 伊廷锋，Emails:tfyihit@163.com

English

Synergistic design of high-entropy P2/O3 biphasic cathodes for high-performance sodium-ion batteries

Corresponding author: Zonglin Liu, ; Tingfeng Yi,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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