钠离子电池正极材料中离子迁移与电子转移的协同优化

doi:10.1016/j.actphy.2025.100206

摘要/Abstract

摘要：

钠离子电池(SIBs)凭借钠资源丰富、成本低廉及环境友好等优势，在大规模储能系统中展现出巨大应用潜力。正极材料的离子迁移与电子转移速率是决定电池倍率性能、循环寿命及容量保持率的关键因素，二者的协同提升对突破性能瓶颈至关重要。本文以钠离子电池三大主流正极材料——层状过渡金属氧化物(LTMOs)、聚阴离子化合物(PACs)和普鲁士蓝类似物(PBAs)为研究对象，系统梳理了不同材料体系中离子迁移通道与电子转移路径的结构基础，深入解析了二者的协同调控机制。结合最新研究成果，从元素优化、结构设计与复合改性三个维度，阐释了协同提升离子通道通畅性与电子通路连续性的具体路径与作用机理，提炼出高性能SIBs正极材料的普适性设计策略，为进一步开发兼具高容量、高倍率性能与稳定的SIBs正极材料提供了有益参考。

关键词: 正极材料, 协同调控, 元素优化, 结构设计, 复合改性

Abstract:

Sodium-ion batteries (SIBs) have demonstrated enormous application potential in large-scale energy storage systems due to their abundant sodium resources, low cost, and environmental friendliness. The ion migration rate and electron transfer efficiency of cathode materials are key factors determining the rate performance, cycle life, and capacity retention rate of batteries, and synergistic improvement of both is essential to overcoming performance bottlenecks. This paper takes the three mainstream cathode materials of sodium-ion batteries as its research objects, including layered transition metal oxides (LTMOs), polyanionic compounds (PACs), and Prussian blue analogues (PBAs). It systematically reviews the structural basis of ion migration channels and electron transfer pathways in different material systems and thoroughly analyzes their synergistic regulatory mechanisms. Combining the latest research findings, this paper explains, from three dimensions of elemental optimization, structural design, and composite modification, the specific pathways and mechanisms for synergistically enhancing the efficiency of ion channels and the continuity of electronic pathways. It distills universal strategies for designing high-performance SIBs cathode materials, providing a valuable reference for further developing SIBs cathode materials that combine high capacity, exceptional rate performance, and robust stability.

Key words: Cathode materials, Synergistic regulation, Elemental optimization, Structural design, Composite modification

王双, 傅小奇, 姚山山. 钠离子电池正极材料中离子迁移与电子转移的协同优化[J]. 物理化学学报, 2026, 42(5), 100206. doi: 10.1016/j.actphy.2025.100206

Shuang Wang, Xiaoqi Fu, Shanshan Yao. Synergistic optimization of ion migration and electron transfer in sodium-ion battery cathode materials[J]. Acta Phys. -Chim. Sin. 2026, 42(5), 100206. doi: 10.1016/j.actphy.2025.100206

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100206

https://www.whxb.pku.edu.cn/CN/Y2026/V42/I5/100206

图/表 24

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表1

表2

Cathode	Anode	Cycle performance (cycle/rentention)	Voltage (V)	Capacity (mAh g⁻¹)	Na⁺ diffusion Coefficient		Conductivity		Elyctrolyte		Ref.
Na_3.08Fe_2.44(P₂O_6.98)₂F_0.04	half-cell: Na	50C, 20000, 86.3%; 1C, 300, 94.3%	1.8–4.2	54.4–116.4_C	10⁻¹⁰–10⁻⁹ cm² s⁻¹		Band gap dropped from 4.43 eV to 3.19 eV		1 mol L⁻¹ NaPF₆ in PC + 2 vol% FEC		72
Na_3.08Fe_2.44(P₂O_6.98)₂F_0.04	full-cell: HC	–	–	88.3_C	10⁻¹⁰–10⁻⁹ cm² s⁻¹		Band gap dropped from 4.43 eV to 3.19 eV		1 mol L⁻¹ NaPF₆ in PC + 2 vol% FEC		72
P2-Na_2/3Ni_1/3Mn_2/3O₂	half-cell: Na	–	2.0–4.3	69.1– 89.9_C	10⁻¹⁰ cm² s⁻¹		–		1 mol L⁻¹ NaPF₆ in PC + 2 vol% FEC		84
P2/O3-Na_0.80Li_0.13Ni_0.20Fe_0.10Mn_0.57O₂	half-cell: Na	1C, 100, 88.60%	2.0–4.5	152.4–172.02_C	10⁻¹² cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC : PC = 1 : 2 + 5 vol% FEC		85
layered-tunnel intergrowth Na_0.6MnO₂ (LT-NaMO)	half-cell: Na	5C, 300, 70.5%	2.0–4.0	98.7–179.4_C	Fast Kinetics		enhanced		1 mol L⁻¹ NaClO₄ in PC + 5 vol% FEC		86
layered-tunnel intergrowth Na_0.6MnO₂ (LT-NaMO)	full-cell: HC	1C, 100, 85.0%	1.9–3.9	162.3_C	Fast Kinetics		enhanced		1 mol L⁻¹ NaClO₄ in PC + 5 vol% FEC		86
P2-Na_0.7Mg_0.05 [Mn_0.6Ni_0.2Mg_0.15]O₂	half-cell: Na	1C, 1000, 79%	1.5–4.2	130_C	enhanced		enhanced		1 mol L⁻¹ NaClO₄ in EC : PC (1 : 1)		45
P2-Na_0.7Mg_0.05 [Mn_0.6Ni_0.2Mg_0.15]O₂	full-cell: HC	0.2C, 50, 85%	2.0–4.0	63_C	enhanced		enhanced		1 mol L⁻¹ NaClO₄ in EC : PC (1 : 1)		45
P'2-Na_0.653Ni_0.081Mn_0.799Ti_0.120O₂	full-cell: HC	250 mA g⁻¹, 500, 87.2%	1.8–4.3	185_C	10⁻¹¹–10⁻¹⁰ cm² s⁻¹		enhanced		–		41
NaNi_0.3Cu_0.1Fe_0.2Mn_0.3Ti_0.1O₂ (NCFMT)	half-cell: Na	1C, 500, 85%; 45 ℃, 1C, 500, 80%	2.0–4.0	141.5_C	twice that of NCFMS		Better than NCFMS		1 mol L⁻¹ NaClO₄ in PC/EC/DMC (1 : 1 : 1) + 2 vol% FEC		42
NaNi_0.3Cu_0.1Fe_0.2Mn_0.3Ti_0.1O₂ (NCFMT)	full-cell: HC	1C, 682, 80%; 4.15 V, 1C–2C, 67.2%	0.5–4.0; 0.5–4.15	–	twice that of NCFMS		Better than NCFMS		1 mol L⁻¹ NaClO₄ in PC/EC/DMC (1 : 1 : 1) + 2 vol% FEC		42
[Na_0.89Li_0.05Cu_0.11Ni_0.11Fe_0.3 Mn_0.43O_1.97F_0.03] (LCNFM)	half-cell: Na full-cell: HC	1C, 300, 80% 1C, 200, 81.6%	1.5–4.0 1.0–4.0	138.6_C 134.5_C	10⁻¹⁰–10⁻⁹ cm² s⁻¹		Better than CNFM		–		31
NaNi_0.2Fe_0.2Mn_0.35Cu_0.05Zn_0.1Sn_0.1O₂	full-cell: HC	3.0C, 500, 87%; 1.0C, 300, 80%	0.5–4.0	64–122_C	10⁻¹¹–10⁻¹⁰ cm² s⁻¹		Narrow band gap 0.14 eV		1 mol L⁻¹ NaClO₄ in EC/PC/DMC (4.5 : 4.5 : 0.1) + 3 wt% FEC		78
Na_0.78Ni_0.31Mn_0.67Nb_0.02O₂ (P2-NaMNNb)	half-cell: Na	−40 ℃, 368 mA g⁻¹, 1800, 76%; 25 ℃, 9.2 A g⁻¹, 65%	2.4–4.15	66–97_C	10⁻⁹–10⁻⁶ cm² s⁻¹		Band gap dropped from 0.500 eV to 0.332 eV		1 mol L⁻¹ NaPF₆ in diglyme		44
Na_0.78Ni_0.31Mn_0.67Nb_0.02O₂ (P2-NaMNNb)	full-cell: HC	25 ℃, 920 mA g⁻¹, 300, 84%; −40 ℃, 92 mA g⁻¹, 100, 89%	2.3–4.14	20–60_C	10⁻⁹–10⁻⁶ cm² s⁻¹		Band gap dropped from 0.500 eV to 0.332 eV		1 mol L⁻¹ NaPF₆ in diglyme		44
Na_3.5V_1.5Fe_0.5(PO₄)₃–V₂O₃ (NVFP–VO)	half-cell: Na	100C, 100, 000, 72.6%	2.0–4.1	82–130_C	10⁻⁸ cm² s⁻¹		Band gap about 1.18 eV		1 mol L⁻¹ NaClO₄ in PC + 5 vol% FEC		61
Na_3.5V_1.5Fe_0.5(PO₄)₃–V₂O₃ (NVFP–VO)	full-cell: HC	1C, 500, 77.38%	1.7–4.1	–	10⁻⁸ cm² s⁻¹		Band gap about 1.18 eV		1 mol L⁻¹ NaClO₄ in PC + 5 vol% FEC		61
Na₃V_1.8Mn_0.2(PO₄)₃/C (NVMP/C)	half-cell: Na	1C, 100, 90%	2.0–4.0	107_C		10⁻¹¹ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC : PC (1 : 1)	80
Na₃V₂(PO₄)₃ (NVP-E700)	half-cell: Na	0.2C, 200, 99.6%; 10 C, 82.8%	2.0–4.5	83–180_C		10⁻¹¹ cm² s⁻¹		enhanced		–	47
Na_2.5Fe₂(SO₄)_2.5(PO₄)_0.5 (NFSP-0.5)	half-cell: Na	10C, 10000, 88.8%	2.0–4.5	80–112_C		10⁻¹¹ cm² s⁻¹		Band gap dropped from 3.63 eV to 3.35 eV		–	50
Na_2.5Fe₂(SO₄)_2.5(PO₄)_0.5 (NFSP-0.5)	full-cell: HC	1C, 1000, 85.9%	–	–		10⁻¹¹ cm² s⁻¹		Band gap dropped from 3.63 eV to 3.35 eV		–	50
Na₃V_1.44Fe_0.5Mo_0.06(PO₄)₃ (NVFP-Mo (0.06))	half-cell: Na	30C, 2500, 92%; 0.2C, 50, 97.7%	2.2–4.2	123.4c		10⁻¹⁰–10⁻⁸ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in PC + 5 vol% FEC	51
Na₃Cr_0.5V_1.5(PO₄)₃/rGO (VC/C-G)	half-cell: Na	0.2C, 100, 80.4%	1.5–4.5	95–176_C		10⁻¹¹–10⁻⁸ cm² s⁻¹		enhanced		–	57
Na_3.4Fe_2.4(PO₄)_1.4P₂O₇/C (1.4-NFPP/C)	half-cell: Na	10C, 1000, 97.7%; 1C, 300, 100%	1.7–4.1	112.2c		10⁻¹¹ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC : PC (1 : 1) + 5 vol% FEC	60
Na_3.4Fe_2.4(PO₄)_1.4P₂O₇/C (1.4-NFPP/C)	full-cell: HC	1C, 1000, 87.7%	1.7–4.1	106.3c		10⁻¹¹ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC : PC (1 : 1) + 5 vol% FEC	60
Na₃Fe₂(PO₄)P₂O₇/rGO (NFPP/rGO)	half-cell: Na	20C, 8000, 72.4%; 10C, 2000, 88.0%	1.5–4.0	42–106_C		10⁻¹⁰ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC/DEC (1 : 1)	64
Na₃Fe₂(PO₄)P₂O₇/rGO (NFPP/rGO)	full-cell: HC	100 mA g⁻¹, 500, 85.2%	–	86.2_C		10⁻¹⁰ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC/DEC (1 : 1)	64
Na₄VMn_0.75Mg_0.25(PO₄)₃ (Mg-NVMP)	half-cell: Na	78 mAh g⁻¹, 100, 96%	3.8–2.75	80_C		10⁻⁴ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC/PC/DMC (4.5 : 4.5 : 0.1) + 3 wt% FEC	59
Na_3.75VMn_0.75Al_0.25(PO₄)₃ (Al-NVMP)	half-cell: Na	92 mAh g⁻¹, 100, 96%	3.8–2.75	80–89_C		10⁻⁴ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC/PC/DMC (4.5 : 4.5 : 0.1) + 3 wt% FEC	59
Na₄Fe₃(PO₄)₂P₂O₇ (NFPP-Si₀.₀₅)	half-cell: Na	50C, 5000, 84.2%	1.5–4.0	61–119_C		10⁻¹¹–10⁻⁹ cm² s⁻¹		enhanced		1 mol L⁻¹ NaClO₄ in EC/DEC (1 : 1) + 5% FEC	87
Na_1.97Fe[Fe(CN)₆]_0.986 (Fe-HCF-5)	half-cell: Na	1C, 100, 80.6%	2.0–4.2	112–152_C		enhanced		enhanced		–	70
Na_1.97Fe[Fe(CN)₆]_0.986 (Fe-HCF-5)	full-cell: HC	0.1C, 50, 83.24%	2.0–3.6	89.0_C		enhanced		enhanced		–	70
Na_1.68Fe_0.92Cu_0.08[Fe(CN)₆]_0.86· 1.43H₂O (Cu-FeHCF)	half-cell: Na	100 mA g⁻¹, 100, 83.6%; 2 A g⁻¹, 500, 76.5%	2.0–4.2	82–127_C		10⁻¹⁰ cm² s⁻¹		enhanced		–	75
K_0.95Ag_3.05Fe(CN)₆@CNTs (AgHCF@CNTs)	half-cell: Na	500 mA g⁻¹, 500, 74%	1.1–4.1	152c		10⁻¹⁴–10⁻¹⁰ cm² s⁻¹		enhanced		–	69
a core–shell structure of cobalt hexacyanoferrate (CoFeHCF)	half-cell: Na	100 mA g⁻¹, 300, 89%	2.0–4.2	94–160_C		enhanced		–		1 mol L⁻¹ NaClO₄ in PC	93
high sodium content PBAs (HSPB)	half-cell: Na	50 mA g⁻¹, 200, 65.7%	2.0–4.2	136.9_C		–		–		1 mol L⁻¹ NaClO₄ in EC : DEC (1 : 1) + 5 wt% FEC	34
high sodium content PBAs (HSPB)	full-cell: HC	1C, 1000, 80%	2.0–3.6	–		–		–		1 mol L⁻¹ NaClO₄ in EC : DEC (1 : 1) + 5 wt% FEC	34
K_0.24(VO)_0.58[Fe(CN)₆]·2.59H₂O (FeVO-PBA)	half-cell: Na	–	1.6–4.0	56.1– 48.9_C		10⁻¹²–10⁻⁸ cm² s⁻¹		Exhibit metallic properties		ether-based electrolyte	89
K_0.24(VO)_0.58[Fe(CN)₆]·2.59H₂O (FeVO-PBA)	full-cell: HC	1C, 100, 85.0%	1.9–3.9	138.0–162.3_C		10⁻¹²–10⁻⁸ cm² s⁻¹		Exhibit metallic properties		ether-based electrolyte	89
PB-PA3	half-cell: Na	1C, 200, 94%; 10C, 2500, 79%; 20C, 4000, 79%	2.0–4.2	94.8–143.9_C		10⁻¹⁴–10⁻¹³ cm² s⁻¹		–		–	66
PB-PA3	full-cell: HC	1C, 300, 85%; 5C, 1000, 84%	2.0–3.8	108–133_C		10⁻¹⁴–10⁻¹³ cm² s⁻¹		–		–	66
Na_1.7Ni_0.04Fe_0.48Mn_0.48[Fe(CN)₆]_0.92 (NFM-PB-1)	half-cell: Na	100 mA g⁻¹, 1000, 85.19%	2.0–4.2	102.7–131.0_C		10⁻¹¹ cm² s⁻¹		–		–	65
Na_1.7Ni_0.04Fe_0.48Mn_0.48[Fe(CN)₆]_0.92 (NFM-PB-1)	full-cell: HC	100 mA g⁻¹, 250, 79.35%	–	88.9_C		10⁻¹¹ cm² s⁻¹		–		–	65
Na_0.28K_1.55Fe[Fe(CN)₆]·1.53H₂O (NKPB-3)	half-cell: Na	150 mA g⁻¹, 300, 83.5%	2.0–4.2			10⁻¹²–10⁻⁸ cm² s⁻¹		–			66

表2

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图18

图19

图20

图21

图22

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	Construct a conductive network	Reduce the band gap	Reduce the particle size
LTMOs	★★	★★★	★
PACs	★★★	★★	★★
PBAs	★★	★	★★★

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