Key Takeaways & Executive Findings
- •• • The low-nickel cathode Li(Li0.05Ni0.57Mn0.31Co0.07)O2 (Ni<60%) achieves high discharge capacity and cycling stability comparable to Ni-rich cathodes (N80/N90), reducing nickel content by over 20% and mitigating supply chain risks. • • mRIXS analysis reveals a persistent spectral feature at 4.5 V, indicating highly reversible lattice oxygen redox that remains largely unchanged after 100 cycles, directly contributing to capacity retention. • • The radially integrated structure comprises three phases: an outermost rock-salt phase with lithium-percolation channels, an intermediate Li/Mn-rich phase with delocalized superlattice ordering, and an inner Ni-rich layered phase, enabling synergistic '1+1+1>3' performance. • • In-situ high-energy X-ray diffraction demonstrates minimized lattice variations and suppressed Ni oxidation state changes during cycling, addressing bulk structural degradation and interfacial side reactions.
Abstract
Nickel-rich layered cathodes (Ni≥80%) offer high discharge capacity for lithium-ion batteries but face sustainability and structural stability challenges. This study presents a radially multiphase integrated low-nickel (Ni<60%) cathode material, Li(Li0.05Ni0.57Mn0.31Co0.07)O2 (LNC), which achieves high capacity and long-term cycling stability by leveraging highly reversible anionic redox chemistry. The cathode comprises three distinct radial phases: an outermost epitaxial rock-salt phase with lithium-percolation channels, an intermediate lithium-rich manganese-rich phase with delocalized superlattice ordering, and an inner nickel-rich layered phase. The rock-salt phase suppresses interfacial side reactions and structural degradation, while the superlattice enhances lattice oxygen redox reversibility, as evidenced by resonant inelastic X-ray scattering (mRIXS) showing persistent spectral features at 4.5 V even after 100 cycles. The inner nickel-rich phase provides high discharge capacity via nickel-ion redox. This synergistic integration minimizes lattice variations and nickel oxidation state changes during cycling, as demonstrated by in-situ high-energy X-ray diffraction. Compared to commercial N60, N70, N80, and N90 cathodes, LNC delivers superior discharge capacity, cycling stability, and rate performance while reducing nickel dependence, offering a sustainable pathway for high-energy-density batteries.
1. Introduction
Commercial high-energy-density lithium-ion batteries rely heavily on nickel-rich layered cathodes (Ni≥80%) to achieve high discharge capacity. However, the escalating use of nickel raises critical concerns about resource sustainability and environmental impact from mining. Moreover, at high voltages, Ni4+ ions induce fragile Ni–O bonds and trigger structural degradation, including lattice oxygen release and phase transitions to spinel/rock-salt, alongside persistent interfacial side reactions. These mechanisms accelerate capacity fading and thermal instability, compromising cycle life and safety. Consequently, the industry faces a dual challenge: maintaining high specific capacity while suppressing structural degradation, and reducing nickel dependence to align with sustainable development goals.
This study introduces a radially multiphase integrated low-nickel cathode, Li(Li0.05Ni0.57Mn0.31Co0.07)O2 (LNC), which addresses these bottlenecks by employing highly reversible anionic redox as a capacity compensation mechanism. This approach lowers the oxidation state of nickel ions, mitigating bulk structural degradation. The cathode's unique radial architecture—comprising an outer rock-salt phase with lithium-percolation channels, an intermediate Li/Mn-rich phase with delocalized superlattice ordering, and an inner Ni-rich layered phase—enables efficient lithium diffusion, suppresses interfacial side reactions, and enhances lattice oxygen redox reversibility. As a result, LNC achieves comprehensive improvements in discharge capacity, cycling stability, and rate performance while significantly reducing nickel content, offering a viable path toward sustainable high-energy-density batteries.
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Jiaxuan Zuo, Xifei Li (2026). Radial multiphase integration boosting capacity and stability for low-nickel cathodes. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3955-0
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Frequently Asked Questions
What specific mechanisms enable the low-nickel cathode to achieve high capacity without relying on high Ni content?
The cathode leverages highly reversible anionic (oxygen) redox as a capacity compensation mechanism. The intermediate Li/Mn-rich phase with delocalized superlattice ordering enhances the reversibility of lattice oxygen redox, as evidenced by mRIXS showing persistent spectral features at 4.5 V even after 100 cycles. This reduces the oxidation state of Ni ions, mitigating structural degradation while contributing additional capacity.
How does the radial multiphase structure suppress interfacial side reactions and structural degradation during cycling?
The outermost epitaxial rock-salt phase with lithium-percolation diffusion channels acts as a chemically stable barrier, preventing direct contact between the electrolyte and highly oxidized Ni4+ or reactive oxygen species. This suppresses interfacial side reactions and structural degradation. Additionally, the inner Ni-rich layered phase provides high capacity via Ni redox, while the overall structure minimizes lattice variations and Ni oxidation state changes, as confirmed by in-situ high-energy X-ray diffraction.
What are the quantitative improvements in discharge capacity, cycling stability, and rate performance compared to commercial N60/N70/N80/N90 cathodes?
The abstract indicates that the multiphase integration cathode achieves 'comprehensive improvements' in discharge capacity, cycling stability, and rate performance compared to commercial N60, N70, N80, and N90 cathodes, but specific numerical values are not provided in the given text. However, the low-nickel composition (Ni<60%) suggests that it can match or exceed the performance of higher-nickel cathodes while using less nickel, as demonstrated by the mRIXS data showing stable oxygen redox after 100 cycles.
What are the scalability and manufacturing challenges for this radially multiphase cathode, and how might they be addressed?
The synthesis of such a radially structured cathode with three distinct phases requires precise control over precursor preparation and calcination conditions. Scalability may be challenging due to the need for uniform phase distribution and epitaxial growth. However, the use of low-nickel content reduces raw material costs and supply chain risks. Further research is needed to optimize synthesis parameters for industrial-scale production, but the potential for cost reduction and sustainability makes it an attractive candidate for commercialization.
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