Deciphering the synergistic mechanism for thermal stability improvement in Ni-rich single-crystal cathode materials via LiNbO3 coating and Nb5+ surface doping
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PUBLIC SUMMARY
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Ni-rich cathodes' thermal stability improved by LiNbO3 coating and Nb5+ doping.
Nb@SC-NCM811 shows better electrochemical performance and higher thermal stability.
Enhanced stability due to oxygen vacancy formation and increased migration barrier.
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ABSTRACT
Ni-rich cathode materials are highly regarded for their potential in high-energy density lithium-ion batteries (LIBs). Nonetheless, their intrinsic thermal instability poses a significant risk of thermal runaway, which is a major obstacle to their commercial application. This study presents a novel approach to enhancing the thermal stability of Ni-rich cathode materials for LIBs through a synergistic modification strategy combining LiNbO3 coating and Nb5+ surface doping. By applying particle atomic layer deposition and high-temperature sintering, the modified cathode material Nb@SC-NCM811 shows better electrochemical performance. Thermal analysis reveals that Nb@SC-NCM811 has a higher thermal decomposition temperature, generates less heat, and releases less oxygen under thermal induction, indicating enhanced thermal stability. The microscopic mechanisms underlying the improvement of thermal stability are further revealed through aberration-corrected transmission electron microscopy and density functional theory calculations, which shows that the enhancement in thermal stability is due to the increased formation energy of oxygen vacancies and the raised energy barrier for interlayer migration of transition metal cations. This work provides insight into the Nb-modified mechanism of Ni-rich cathode materials and offers a promising avenue for designing safer, high-energy density LIBs. -
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Wei Z., Fang Z., Liang C., et al. (2025). Deciphering the synergistic mechanism for thermal stability improvement in Ni-rich single-crystal cathode materials via LiNbO3 coating and Nb5+ surface doping. The Innovation Energy 2:100083. https://doi.org/10.59717/j.xinn-energy.2025.100083
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Wei Z., Fang Z., Liang C., et al. (2025). Deciphering the synergistic mechanism for thermal stability improvement in Ni-rich single-crystal cathode materials via LiNbO3 coating and Nb5+ surface doping. The Innovation Energy 2:100083. https://doi.org/10.59717/j.xinn-energy.2025.100083
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Figure 1.
(A) Modification strategy of LiNbO3 coating and Nb5+ surface doping for the Pristine SC-NCM811. TEM images and HR-TEM images of Ni-rich cathode materials. (B & C) Pristine SC-NCM811. (D & E) LiNbO3@SC-NCM811. (F & G) Nb@SC-NCM811
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Figure 2.
(A) HAADF-STEM image of LiNbO3@SC-NCM811, atomic arrangement images and corresponding FFT patterns of (B & C) surface region, and (D & E) bulk region; (F) HAADF-STEM image of Nb@SC-NCM811 cathode particles, atomic arrangement images and corresponding FFT patterns of (G & H) surface region, and (I & J) bulk region.
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Figure 3.
Electrochemical performance of Pristine SC-NCM811 and Nb@SC-NCM811
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Figure 4.
(A) TG curves and (B) DSC curves of delithiated cathode materials. (C) Heat flow curves of the delithiated cathode-electrolyte mixed system by C80 micro-calorimeter. TG/MS results of delithiated cathode materials, (D) O2, (E) CO2 signals.
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Figure 5.
The dynamic heat flow curves of coin batteries during the charge-discharge cycle of
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Figure 6.
Low-magnification HAADF-STEM image of (A) Pristine SC-NCM811, (F) Nb@SC-NCM811 after thermal failure at 400 °C. Atomic arrangements in the (B & G) surface region and (C & H) bulk region, and corresponding FFT images in the (D & I) surface region and (E & J) bulk region. (A-E) Reproduced with permission.38 Copyright 2023, Elsevier.
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Figure 7.
O K-edge spectrum obtained by the EELS line scan results from the surface to the central region of
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Figure 8.
The projected density of states (PDOS) diagram for various elements in
