Effect of MgO/Y2O3 Composite Coating on the Structure and Properties of LiNi0.9Mn0.1O2

doi:10.15541/jim20250430

Abstract

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

CLC Number:

O646

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.

Figures/Tables 17

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

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

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)

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

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

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

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

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

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

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

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

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

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%

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

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

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

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

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