高熵策略驱动下的钠离子电池层状氧化物正极材料改性研究：进展、机理与展望

doi:10.11949/0438-1157.20250511

摘要/Abstract

摘要：

近年来，钠离子电池（SIB）因其成本优势和对锂离子电池的替代作用而受到了越来越多的关注。层状氧化物正极作为最有潜力的钠电正极材料，具有理论比容量高、合成工艺简单等优势，但也存在着不可逆相变、结构退化以及电压衰减等缺陷，这些因素阻碍了SIB的商业化发展与大规模应用。高熵策略是一种结合了多元素掺杂、体相结构设计等多种手段的综合改性策略，可以有效提高电极材料的能量密度、长循环稳定性以及离子传输动力学等性能指标。总结了近年来高熵策略在钠离子电池层状氧化物材料改性研究领域的前沿成果，探讨了高熵效应与层状氧化物材料电化学性能之间的内在联系与作用机理，并展望了高熵策略未来的发展方向，为未来高性能钠离子电池层状正极材料的设计与合成提供新的见解。

关键词: 钠离子电池, 层状氧化物, 熵, 相变, 电化学

Abstract:

In recent years, sodium-ion batteries (SIB) have received more and more attention due to its cost advantage and potential as an alternative to lithium-ion batteries (LIB). Layered oxide cathodes, as the most promising sodium-ion cathode materials, offer advantages such as high theoretical specific capacity and simple synthesis processes. However, they also suffer from drawbacks such as irreversible phase transitions, structural degradation, and voltage decay, which hinder the commercial development and large-scale application of SIBs. The high-entropy strategy is a comprehensive modification strategy that combines multiple methods, including multi-element doping and bulk structure design, to effectively improve electrode material performance indicators such as energy density, long-term cycle stability, and ion transport kinetics. This review systematically summarizes recent achievement in high-entropy strategies for modification of layered oxide cathode materials for SIB. The intrinsic correlation and modification mechanism between high-entropy effect and improved electrochemical performance are analyzed. Furthermore, future directions for high-entropy strategy are prospected, providing new insight for the design and synthesis of high-performance layered cathode material for future sodium-ion batteries.

Key words: sodium-ion battery, layered oxide materials, entropy, phase change, electrochemistry

中图分类号:

TM 912

童逸凡, 张宁霜, 蔡星鹏, 李成煜, 李世友. 高熵策略驱动下的钠离子电池层状氧化物正极材料改性研究：进展、机理与展望[J]. 化工学报, 2025, 76(12): 6218-6235.

Yifan TONG, Ningshuang ZHANG, Xingpeng CAI, Chengyu LI, Shiyou LI. Research on modification of layered oxide cathode materials for sodium-ion battery driven by high-entropy strategy: progress, mechanism, and future[J]. CIESC Journal, 2025, 76(12): 6218-6235.

图/表 12

表1 主流钠离子电池正极材料优缺点总结

Table 1 Summary of advantages and disadvantages of mainstream SIB cathode materials

材料	优势	劣势
聚阴离子型材料^[9]	结构稳定性强、工作电压高	电子电导率低，能量密度低，合成成本高昂
普鲁士蓝材料^[10]	合成工艺简单、快速充放电能力强	循环寿命较短、工作温度范围较窄
过渡金属氧化物材料^[11]	合成工艺简单、可逆比容量高、储钠能力强	充放电过程中易发生不可逆相变、空气稳定性差

表2 钠离子电池中的高熵层状正极材料总结

Table 2 Summary of layered cathodes with high-entropy configurations in SIBs

正极材料	放电比容量/(mAh·g^-1)	电压范围/V	循环稳定性	倍率性能/(mAh·g^-1)	文献
Na_0.83Li_0.1Ni_0.25Co_0.2Mn_0.15Ti_0.15Sn_0.15O_2-_δ	109.4	2.0~4.2	87.2%/200次循环/2.0C	83.3 /10C	[35]
NaCu_0.1Ni_0.25Co_0.15Mn_0.35Li_0.05Ti_0.05Sn_0.05O₂	144.5	2.2~4.4	90.1%/100次循环/1.0C	76.7/5.0C	[36]
NaNi_0.3Cu_0.1Fe_0.2Mn_0.3Ti_0.1O₂	141.5	2.0~4.0	85%/500次循环/1.0C	120/5.0C	[37]
NaNi_0.2Fe_0.2Mn_0.35Cu_0.05Zn_0.1Sn_0.1O₂	128	2.0~4.0	87%/500次循环/3.0C	64.3/2.0C	[38]
Na_2/3Li_1/6Fe_1/6Co_1/6Ni_1/6Mn_1/3O₂	171.2	2.0~4.5	90%/30次/0.3C	78.2/10C	[39]
[Na_0.67Zn_0.05]Ni_0.22Cu_0.06Mn_0.66Ti_0.01O₂	146.1	2.0~4.3	92.7%/100次循环/1.0C	91.54/10C	[40]
Na_0.67Mn_0.6Cu_0.08Ni_0.09Fe_0.18Ti_0.05O₂	150.3	2.0~4.5	100%/500次循环/10C	62.5/10C	[41]
Na[FeCoNiTi]_1/6Mn_1/4Zn_1/12O₂	127.3	2.0~4.1	88%/1000次循环/1.0C	30.7/10C	[42]
Na_0.9Ni_0.2Fe_0.2Co_0.2Mn_0.2Ti_0.15Cu_0.05O₂	117.8	2.2~4.1	70.7%/1000次循环/1.0C	98.6/10C	[43]
Na(Fe_0.2Co_0.15Cu_0.05Ni_0.2Mn_0.2Ti_0.2)B_0.02O₂	120.5	2.0~4.1	95%/100次循环/1.0C	103.3/2.0C	[44]
Na_0.95Li_0.06Ni_0.25Cu_0.05Fe_0.15Mn_0.49O₂	141.2	2.0~4.2	83.2/500次循环/8.0C	83.5/20C	[45]
Na_0.89Li_0.05Cu_0.11Ni_0.11Fe_0.3Mn_0.43O_1.97F_0.03	145	1.5~4.0	80%/300次循环/1.0C	109/10C	[46]
Na_0.85Li_0.05Ni_0.25Cu_0.025Mg_0.025Fe_0.05Al_0.05Mn_0.5Ti_0.05O₂	122	2.0~4.3	89%/1000次循环/10C	81.8/10C	[47]
Na_0.85Li_0.05Ni_0.3Fe_0.1Mn_0.5Ti_0.05O₂	182.2	1.5~4.3	94.3/10次循环/10C	68.4/10C	[48]

图1 Na+脱嵌过程中的高熵改性材料结构演化（1 Å =0.1 nm）[35]

Fig.1 Entropy-optimized structural evolution during Na+ extraction/insertion[35]

图2 高熵改性稳定晶格氧示意图[36]

Fig.2 Schematic diagram of stabilizing lattice oxygen through high-entropy modification[36]

图3 HE和NFM正极材料的结构演化和DFT计算[38]

Fig.3 The structural evolution and density functional theory (DFT) calculations of HE and NFM cathode materials[38]

图4 (a)本研究提出的高熵和超晶格稳定的O3型正极的充放电行为示意图，其中低电压区的O3-P3相变被促进，高电压区的P3-O3相变被抑制；(b)NaLFCNM与之前报道的O3/P3型正极之间的电化学性能对比，其中所有正极都已经历超过50次充放电循环[39]

Fig.4 (a) Schematic illustration of charge/discharge behaviors for high-entropy and superlattice-stabilized O3-type cathodes proposed in this work,where the O3-P3 phase transition at the low-voltage region is facilitated and the P3-O3 phase transition at the high-voltage region is suppressed; (b) Electrochemical performance comparison between NaLFCNM and previously reported O3/P3-type cathodes, in which all cathodes havebeen cycled for more than 50 cycles[39]

图5 (a)经过高熵掺杂改性的NZNCMTO材料结构；(b)NZNCMTO和NNMO中Ni—O和Mn—O键的COHP值的对比；(b)熵调谐的NZNCMTO的COHP结果；(d)~(g)Na+在NNMO和熵调谐的NZNCMTO中通过Ni/Mn、Ti和Cu的迁移路径和迁移能垒示意图；(h)NNMO和(i)初始状态的NZNCMTO的总态密度（DOS）[40]

Fig.5 (a) The optimized structures of entropy-tuned NZNCMTO; (b) Comparison of COHP values of Ni—O and Mn—O bonds in NZNCMTO and NNMO; (c) COHP results of entropy-tuned NZNCMTO; (d)—(g) Schematic diagram of the migration paths and migration energy barrier of sodium ions through Ni/Mn, Ti, and Cu in NNMO and entropy-tuned NZNCMTO; (h) Total density of states (DOS) of NNMO and (i) entropy-tuned NZNCMTO of the initial state[40]

图6 MCNFT的电荷补偿机制[41]

Fig.6 Charge compensation mechanism of MCNFT[41]

图7 FCNTMZ1/12//HC的动力学性能和全电池性能[42]

Fig.7 The kinetic performance and full cell of FCNTMZ1/12//HC[42]

图8 高熵和低熵钠离子层状氧化物的结构对比[43]

Fig.8 Structural comparison between high-entropy and low-entropy sodium layered oxides[43]

图9 Na0.95LNCFM材料结构设计示意图[45]

Fig.9 Structure characterization of Na0.95LNCFM materials[45]

图10 氧化还原机理和晶体结构的演化过程：(a)~(d)不同充放电状态下的Cu、Ni、Fe和Mn的归一化K边XANES谱；(e)~(g)CNFM、LCNFM和LCNFMF的电压曲线和对应的原位XRD演化过程；(h)通过拟合原位XRD数据得到的3个样品的a/c晶格参数变化过程；(i)LCNFM和LCNFMF在充电过程结束时的晶体结构演化示意图[46]

Fig.10 Redox mechanism and crystal structural evolution: (a)—(d) Normalized Cu, Ni, Fe, and Mn K-edge XANES spectra at different charge- discharge states; (e)—(g) Voltage profile and corresponding in situ XRD evolution of CNFM, LCNFM, and LCNFMF; (h) The a/c-lattice parameters change in the three samples obtained by fitting the in situ XRD data; (i) Schematic illustration of the crystal structural evolution at the end of charging of LCNFM and LCNFMF[46]

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