MgO/Y2O3复合包覆对LiNi0.9Mn0.1O2结构及性能的影响

doi:10.15541/jim20250430

无机材料学报 ›› 2026, Vol. 41 ›› Issue (9): 1220-1228.DOI: 10.15541/jim20250430

MgO/Y₂O₃复合包覆对LiNi_0.9Mn_0.1O₂结构及性能的影响

杨紫程¹(), 范广新¹^,²(), 袁振洛³, 刘宝忠³, 毛英杰¹

¹ 河南理工大学材料科学与工程学院, 焦作 454003
² 河南福鑫能源环保有限公司, 焦作 454191
³ 河南理工大学化学化工学院, 焦作 454003

收稿日期:2025-10-29 修回日期:2026-01-22 出版日期:2026-09-20 网络出版日期:2026-02-05
通讯作者: 范广新, 副教授. E-mail: fangx@hpu.edu.cn
作者简介:杨紫程(2000-), 男, 硕士研究生. E-mail: 3034991831@qq.com
基金资助:
国家自然科学基金联合基金重点项目(U22A20120);国家自然科学基金-青年科学基金项目(52401274)

Effect of MgO/Y₂O₃ Composite Coating on the Structure and Properties of LiNi_0.9Mn_0.1O₂

YANG Zicheng¹(), FAN Guangxin¹^,²(), YUAN Zhenluo³, LIU Baozhong³, MAO Yingjie¹

¹ School of Materials Science and Engineering, Henan Polytechnic University, Jiaozuo 454003, China
² Henan Fuxin Energy and Environmental Protection Co., Ltd., Jiaozuo 454191, China
³ College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo 454003, China

Received:2025-10-29 Revised:2026-01-22 Published:2026-09-20 Online:2026-02-05
Contact: FAN Guangxin, associate professor. E-mail:fangx@hpu.edu.cn
About author:YANG Zicheng (2000-), male, Master candidate. E-mail: 3034991831@qq.com
Supported by:
Joint Funds of the National Natural Science Foundation of China(U22A20120);Young Scientists Fund of the National Natural Science Foundation of China(52401274)

摘要/Abstract

摘要：

LiNi_0.9Mn_0.1O₂ (NM91)因高能量密度、良好的成本效益及环境友好性, 被认为是极具应用前景的锂离子电池正极材料之一, 然而, 较差的倍率性能和循环性能阻碍了其进一步发展。本研究以MgO和Y₂O₃为原料, 采用高温固相法对NM91分别进行MgO单包覆及MgO/Y₂O₃复合包覆, 制得样品NM91-M和NM91-MY, 并对改性效果及机理进行研究。结果表明, 包覆不改变材料晶型, 但会提高其表面粗糙度, 抑制材料在循环过程中晶格的收缩和膨胀, 减缓电解液侵蚀, 进而提升材料的综合性能。其中, 复合包覆因引入Y₂O₃, 在清除NM91表面残锂的同时生成快离子导体LiYO₂, 显著降低材料界面阻抗并提升离子扩散能力, 表现出最优的改性效果。复合包覆后, 材料在5C (1C=180 mA·g^-1)下的放电比容量由90.7 mAh·g^-1提高到129.7 mAh·g^-1; 1C下循环150周后的比容量保持率从73.3%提高到87.9%。即便在4.5 V高截止电压下循环100周(1C), NM91-MY仍保持85.8%的比容量保持率, 远高于NM91 (70.5%)。此外, 150周循环后材料的热分解温度从223.5 ℃提升至230.5 ℃。本研究表明, MgO/Y₂O₃复合包覆是提升NM91电化学性能与热稳定性的有效策略。

关键词: LiNi_0.9Mn_0.1O₂, MgO, Y₂O₃, 复合包覆改性, 电化学性能

Abstract:

LiNi_0.9Mn_0.1O₂ (NM91) is one of the most promising cathode materials for lithium-ion batteries owing to its high energy density, favorable cost-effectiveness, and environmental friendliness. However, its practical application is hindered by poor rate performance and cycling performance. In this study, MgO and Y₂O₃ were used as raw materials, and single MgO and MgO/Y₂O₃ composite were coated on NM91 via a high-temperature solid-state method, yielding the corresponding samples designated as NM91-M and NM91-MY. Effects of these coatings and their underlying mechanisms were systematically investigated. Research results indicate that surface coatings do not change the crystal form of NM91, but both can make the material's surface rougher, inhibit the lattice shrinkage and expansion of the material during the cycling process, and mitigate the erosion of electrolytes on the electrode surface, leading to overall performance enhancement. The composite coating, owing to the introduction of Y₂O₃, removes surface residual lithium while generating the fast ion conductor LiYO₂ thus drastically reducing the material’s interfacial impedance, enhancing its ionic diffusion capability, and showing the best modification effect. After composite coating, the discharge specific capacity of the material at 5C (1C=180 mA·g^-1) increased from 90.7 mAh·g^-1 to 129.7 mAh·g^-1. After 150 cycles at 1C, the specific capacity retention rate of the material increased from 73.3% to 87.9%. Even at a high cut-off voltage of 4.5 V, after 100 cycles (1C), the composite-coated material still maintained a specific capacity retention rate of 85.8%, which was much higher than that of NM91 (70.5%). In addition, the thermal decomposition temperature of the material after 150 cycles increased from 223.5 ℃ to 230.5 ℃. This study demonstrates that MgO/Y₂O₃ composite coating is an effective strategy to improve the electrochemical performance and thermal stability of NM91 materials.

Key words: LiNi_0.9Mn_0.1O₂, MgO, Y₂O₃, composite coating modification, electrochemical performance

中图分类号:

O646

杨紫程, 范广新, 袁振洛, 刘宝忠, 毛英杰. MgO/Y₂O₃复合包覆对LiNi_0.9Mn_0.1O₂结构及性能的影响[J]. 无机材料学报, 2026, 41(9): 1220-1228.

YANG Zicheng, FAN Guangxin, YUAN Zhenluo, LIU Baozhong, MAO Yingjie. Effect of MgO/Y₂O₃ Composite Coating on the Structure and Properties of LiNi_0.9Mn_0.1O₂[J]. Journal of Inorganic Materials, 2026, 41(9): 1220-1228.

图/表 17

图1 NM91、NM91-M和NM91-MY的XRD谱图(a)和NM91-MY的XRD Rietveld精修图(b)

Fig. 1 XRD patterns of NM91, NM91-M and NM91-MY (a), and Rietveld XRD refinement of NM91-MY (b)

表1 NM91、NM91-M和NM91-MY的晶体结构参数

Table 1 Crystal structure parameters for NM91, NM91-M and NM91-MY

Material	a=b/Å	c/Å	V/Å³	I₍₀₀₃₎/I₍₁₀₄₎
NM91	2.87962	14.21669	102.1	2.088
NM91-M	2.87947	14.21753	102.1	2.296
NM91-MY	2.87779	14.20794	101.9	2.638

图2 NM91 (a, b)、NM91-M (c)和NM91-MY (d, e)的SEM照片; NM91-M (f)和NM91-MY (g)的EDS元素分布图

Fig. 2 SEM images of NM91 (a, b), NM91-M (c) and NM91-MY (d, e); EDS elemental distribution mappings of NM91-M (f) and NM91-MY (g)

图3 MgO、Y2O3和Li2CO3烧结产物的XRD谱图

Fig. 3 XRD patterns of MgO, Y2O3 and Li2CO3 sintered product

图4 NM91、NM91-M和NM91-MY在2.7~4.3 V下的初始充放电曲线(a)、倍率性能(b)和循环性能(c)

Fig. 4 Initial charge/discharge curves (a), rate performance (b) and cycling performance (c) of NM91, NM91-M and NM91-MY within the voltage range of 2.7-4.3 V Colorful figures are available on website

图5 NM91、NM91-M和NM91-MY在2.7~4.5 V下的倍率性能(a)和循环性能(b)

Fig. 5 Rate performance (a) and cycling performance (b) of NM91, NM91-M and NM91-MY within the voltage range of 2.7-4.5 V Colorful figures are available on website

图6 NM91 (a)、NM91-M (b)、NM91-MY (c)前三周的CV曲线

Fig. 6 CV curves of NM91 (a), NM91-M (b) and NM91-MY (c) in the first three cycles Colorful figures are available on website

图7 NM91、NM91-M、NM91-MY的EIS谱图及等效电路图(a)和Z′-ω-1/2拟合直线(b)

Fig. 7 EIS spectra and equivalent circuit diagram (a) and Z'-ω-1/2 fitting lines (b) of NM91、NM91-M and NM91-MY

表2 NM91、NM91-M和NM91-MY的EIS拟合结果及Li+扩散系数

Table 2 Fitting results of EIS and diffusion coefficients of Li+ for NM91, NM91-M and NM91-MY

Material	R_s/Ω	R_ct/Ω	D_Li+/(×10^-13, cm²·s^-1)
NM91	21.73	318.9	2.59
NM91-M	13.71	255.1	3.97
NM91-MY	7.32	64.9	11.32

图8 NM91、NM91-M和NM91-MY在2.7~4.3 V下150周循环前后的XRD谱图(a)和局部放大图(b)

Fig. 8 XRD patterns (a) and magnified areas (b) of NM91, NM91-M and NM91-MY before and after 150 cycles within the voltage range of 2.7-4.3 V

图9 NM91 (a, b)、NM91-M (c)、NM91-MY (d)电极在2.7~ 4.5 V下循环100周后的SEM照片

Fig. 9 SEM images of NM91 (a, b), NM91-M (c) and NM91- MY (d) after 100 cycles within the voltage range of 2.7-4.5 V

图10 NM91、NM91-M和NM91-MY在2.7~4.3 V下循环150周后的DSC曲线

Fig. 10 DSC curves of NM91, NM91-M and NM91-MY after 150 cycles within the voltage range of 2.7-4.3 V

表S1 NM91、NM91-M和NM91-MY的电化学性能

Table S1 Electrochemical performance of NM91, NM91-M and NM91-MY

Material	Voltage/V	Discharge specific capacity/(mAh·g^-1)						Specific capacity retention@1C
Material	Voltage/V	0.2C	0.5C	1C	2C	5C	0.2C	100 cycles	150 cycles
NM91	4.3	192.7	173.3	151.2	140.0	90.7	181.0	77.5%	73.3%
NM91-M		189.2	171.7	151.8	140.6	98.4	180.3	87.6%	84.6%
NM91-MY		196.6	176.6	159.7	153.7	129.7	183.5	91.0%	87.9%
NM91	4.5	197.5	178.7	160.0	143.2	113.6	169.6	70.5%
NM91-M		200.6	184.6	174.2	162.1	138.1	183.4	78.6%
NM91-MY		218.5	202.7	189.0	175.8	146.1	198.8	85.8%

图S1 包覆样品的合成示意图

Fig. S1 Schematic diagram of synthesis process for the coated samples

图S2 NM91 (a)和NM91-M (b)的XRD Rietveld精修图

Fig. S2 XRD rietveld refinements for NM91 (a) and NM91-M (b)

图S3 Y2O3与正极材料表面残锂反应示意图

Fig. S3 Reaction diagram of Y2O3 and residual lithium on the surface of cathode material

图S4 NM91 (a)、NM91-M (b)和NM91-MY (c)在2.7~4.3 V、1C (1C=180 mA•g-1)下第1、50、100、150周的充放电曲线

Fig. S4 Charging/discharging curves at the 1st, 50th, 100th and 150th cycles of NM91 (a), NM91-M (b) and NM91-MY (c) within the voltage range of 2.7-4.3 V at 1C (1C=180 mA•g-1)

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MgO/Y₂O₃复合包覆对LiNi_0.9Mn_0.1O₂结构及性能的影响

Effect of MgO/Y₂O₃ Composite Coating on the Structure and Properties of LiNi_0.9Mn_0.1O₂

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