Research progress on high specific-capacity lithium-rich single crystal materials

doi:10.19799/j.cnki.2095-4239.2025.0289

Abstract

Abstract:

Due to their high specific capacity and low cost, lithium-rich oxide materials have been regarded as next-generation cathodes to overcome the bottleneck of energy density in lithium-ion batteries. However, traditional polycrystalline agglomerated lithium-rich materials suffer from intrinsic defects such as particle pulverization and irreversible lattice oxygen release caused by structural reconstruction during long-term cycling, leading to continuous deterioration of the electrode-electrolyte interface and capacity fading. The single-crystal approach has been demonstrated as an effective strategy to mitigate these degradation mechanisms by eliminating grain boundary stress. This paper reviews the unique advantages of lithium-rich single-crystal materials with high nickel content in terms of structural and electrochemical properties. It systematically compares the differences between lithium-rich single-crystal and polycrystalline materials across key performance metrics, including initial Coulombic efficiency, structural stability, morphological evolution after cycling, and gas generation behavior induced by interfacial side reactions. Furthermore, it elaborates on the influence of critical parameters in mainstream synthesis processes, such as high-temperature solid-state methods, molten salt-assisted approaches, and hydrothermal/solvothermal methods, on crystal morphology. Modification strategies and research advancements in lithium-rich single-crystal materials are comprehensively summarized, demonstrating that optimization approaches, including elemental doping, surface coating, and structural engineering, can significantly enhance both structural stability and electrochemical performance. Finally, future development directions for lithium-rich single-crystal materials are discussed, providing theoretical foundations and technical support for the development and application of high energy density lithium-ion batteries.

Key words: Li-rich materials, single-crystal, polycrystalline crystal, synthesis method, modification

CLC Number:

TM 911

Jingjing LI, Danfeng JIANG, Jiaxin LI, Jie YAN, Changjie SHEN. Research progress on high specific-capacity lithium-rich single crystal materials[J]. Energy Storage Science and Technology, 2025, 14(8): 3122-3137.

Figures/Tables 10

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References 68

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材料组成	合成方法	煅烧工艺	形貌	电压范围/V	容量/(mAh/g)	循环保持率/%	文献
Li_1.2Mn_0.54Ni_0.13Co_0.13O₂	高温固相法	800*12	片状	2.0~4.8	254.5	71.9(1000)	[22]
Li_1.2Mn_0.54Ni_0.13Co_0.13O₂	高温固相法	4506+90010	不规则	2.0~4.8	291.4	89.8(100)	[26]
Li_1.1Na_0.1Ni_0.13Co_0.13Mn_0.54O₂	高温固相法	4505+85012	不规则	2.0~4.8	278.5	87(100)	[27]
Li_1.2Mn_0.54Ni_0.13Co_0.13O₂	高温固相法	5002+80012	不规则	2.0~4.8	270	89(400)	[28]
Li_1.2Mn_0.54Ni_0.13Co_0.13O₂	高温固相法	4505+90012	不规则	2.0~4.8	290.4	100(100)	[29]
Li_1.2Ni_0.13Co_0.13Mn_0.54O₂	高温固相法	4505+92514	不规则	2.0~4.8	290.3	81.9(100)	[30]
Li_1.2Mn_0.56Ni_0.12Co_0.12O₂	溶剂热法	4506+90012	片状	2.0~4.8	306.9	—	[31]
0.5Li₂MnO₃·0.5LiMn_0.4Ni_0.3Co_0.3O₂	溶剂热法	4506+90012	片状	2.0~4.8	300.1	93.5(50)	[32]
L_i1.2Mn_0.56Co_0.12Ni_0.12O₂	溶剂热法	900*12	纳米棒	2.0~4.8	264.6	91(100)	[33]
Li_1.2Ni_0.13Co_0.13Mn_0.54O₂	高温固相法	5505+90010+500*5	不规则	2.0~4.8	286.3	89(100)	[9]
Li_1.2Ni_0.13Co_0.13Mn_0.54O₂	高温固相法	5005+85015	片状	2.0~4.8	296	83.2(160)	[34]
Li_1.2Mn_0.48Ni_0.16Co_0.16O₂	高温固相法	9402+76010	不规则	2.0~4.8	259	84.9(100)	[24]
Li_1.2Mn_0.533Ni_0.267O₂	熔融盐辅助法	5005+90020	细长状	2.0~4.8	240	84.06(200)	[8]
Li_1.2Mn_0.56Ni_0.16Co_0.08O₂	熔融盐辅助法	900*15	多边形	2.0~4.7	263.1	82.7(200)	[35]
Li_1.2Ni_0.2Mn_0.6O₂	熔融盐辅助法	900*10	不规则	2.0~4.8	258	97.3(250)	[36]
0.5Li₂MnO₃· 0.5LiMn_1/3Ni_1/3Co_1/3O₂	熔融盐辅助法	900*12	不规则	2.0~4.8	268	82(100)	[37]
Li_1.2Mn_0.533N_i0.267O₂	熔融盐辅助法	5005+90020	不规则	2.0~4.8	210.8	84.06(200)	[8]
Li_1.2Ni_0.13Mn_0.54Co_0.13O₂	熔融盐辅助法	850*8	不规则	2.5~4.6	277	—	[38]
Li[Li_0.2Ni_0.2Mn_0.6]O₂	高温固相法	900*12	片状	2.0~4.8	253	85(200)	[7]

合成方法	优点	缺点
高温固相法	工艺简单易操作、成本低、易于商业化	反应温度高、能耗大、材料形貌和粒度分布不易控制、易混入杂质
熔融盐辅助法	合成温度低、材料形貌可控、产物纯度高、易于商业化	熔融盐选择复杂、操作要求较高
水热/溶剂热法	反应活性高、材料形貌可控	设备要求高、操作复杂、成本较高

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