Entropy Tuning Stabilizing P2‐Type Layered Cathodes for Sodium‐Ion Batteries

Liu, Jie; Huang, Weiyuan; Liu, Renbin; Lang, Jian; Li, Yuhao; Liu, Tongchao; Amine, Khalil; Li, Hongsen

doi:10.1002/adfm.202315437

Cited by 9 publications

(3 citation statements)

References 65 publications

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“…Among LTMOs, the gliding mainly triggers the transformation between P-type and O-type stacking, which brings typical phase transition including P2–O2, P2–OP4, O3–P3–O3′’, etc . For example, the P2-type Na 2/3 Ni 1/3 Mn 2/3 O 2 layered materials show a typical phase transition from P2 to O2 at a voltage of around 4.1 V . Such structural evolution has strong correlation with interlayered Na + content and distribution .…”

Section: Discussion Of Effects On Structurementioning

confidence: 92%

Cation Configuration and Structural Degradation of Layered Transition Metal Oxides in Sodium-Ion Batteries

Yang,

Wang,

Liu

et al. 2024

ACS Nano

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Given the pressing depletion of lithium resources, sodium-ion batteries (SIBs) stand out as a cost-effective alternative for energy storage solutions in the near future. Layered transition metal oxides (LTMOs) emerge as the leading cathode materials for SIBs due to their superior specific capacities and abundant raw materials. Nonetheless, achieving long-term stability in LTMOs for SIBs remains a challenge due to the inevitable structural degradation during charge− discharge cycles. The complexity and diversity of cation configurations/superstructures within the transition metal layers (TMO 2 ) further complicate the understanding for newcomers. Therefore, it is critical to summarize and discuss the factors leading to structural degradation and the available strategies for enhancing LTMOs' stability. In this review, the cationic configurations of TMO 2 layers are introduced from a crystallographic perspective. It then identifies and examines four key factors responsible for structural decay, alongside the impacts of various modification strategies. Finally, more effective and practical research approaches for investigating LTMOs have been proposed. The work aims to enhance the comprehension of the structural deterioration of LTMOs and facilitate a substantial improvement in their cycle life and energy density.

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Section: Discussion Of Effects On Structurementioning

confidence: 92%

Cation Configuration and Structural Degradation of Layered Transition Metal Oxides in Sodium-Ion Batteries

Yang,

Wang,

Liu

et al. 2024

ACS Nano

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“…The diffusion kinetics of Li + was further investigated through the GITT technique (Figure S10). Based on the following simplified equation, D Li + = 4 π τ true( m B V m M B S true) 2 true( normalΔ E s normalΔ E t true) 2 goodbreak0em1em⁣ ( τ ≪ L 2 D ) where τ, V m , S , Δ E s , Δ E t , and L represent the constant current pulse time, the molar volume, the contact area between electrodes and electrolytes, the steady-state voltage changes, the voltage changes during the constant current pulse, and the diffusion distance of lithium ions, respectively.…”

Section: Resultsmentioning

confidence: 99%

Regulating the Charge Distribution of Oxygen by High-Entropy Doping to Stabilize Single-Crystal Ni-Rich Cathode Materials

Gao,

Zhou,

Dai

et al. 2024

ACS Appl. Energy Mater.

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Single-crystal Ni-rich ternary cathode materials (811), with their comprehensive advantage of high energy density and low manufacturing cost, have been considered the most promising materials for Li-ion batteries. Due to strong O-p/TM-d covalent hybridization, the complete oxidation of Ni ions during electrochemical cycling is often accompanied by inevitable oxygen loss, resulting in an irreversible surface phase transition, accumulated lattice stress, and poor thermal stability. Considering the fact that introducing heteroatoms into traditional doping systems can alter the electron density distribution around coordinated oxygen, compositionally complex systems based on high-entropy doping may have a more significant effect on stabilizing lattice oxygen. Herein, the high-entropy doping strategy was applied to design and synthesize single-crystal NCM811 cathodes (HE811) through the molten salt method. Compared to 811, HE811 cathodes show an excellent initial Coulombic efficiency of 90.74% at 0.2C and deliver a higher capacity retention of 80.79% after 300 cycles at 1C between 2.8 and 4.3 V. Owing to high-entropy doping, the oxygen electron densities around multidopants are increased, inhibiting the excessive oxidation of lattice oxygen and improving the stability of TMO 6 coordination structures. This work could provide insights into the high-entropy doping effects in modulating oxygen charge distribution to design high-energydensity Ni-rich ternary cathode materials with long-term cycling.

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“…The Mg 2+ in the Na layer also stabilizes the overall structure, preventing the P2–O2/OP4 phase transition, and the sample shows a capacity retention rate of 82.5% after 120 cycles at 1 C rate. Li et al successfully prepared P2-[Na 0.67 Zn 0.05 ]Ni 0.22 Cu 0.06 Mn 0.66 Ti 0.01 O 2 by doping Zn 2+ into the Na layer . The introduction of Cu 2+ increases the covalent interaction between the TM–O, while Ti 4+ results in the formation of stronger Ti–O bond, stabilizing the lattice oxygen.…”

Section: Strategies For Inhibiting Phase Transitionmentioning

confidence: 99%

Perspective on Phase Transition in Layered Oxide Cathodes for Sodium-Ion Batteries: Mechanism, Influenced Factors, and Inhibition Strategies

Zhang,

2024

Energy Fuels

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Sodium-ion batteries (SIBs) have great potential for large-scale energy storage devices due to the high abundance, wide distribution, and nontoxicity of the resource. Among the various cathode materials, layered oxides are considered a strong contender in the future SIBs market due to their open two-dimensional sodium ion diffusion channels, high theoretical capacity, and ease of synthesis. Unfortunately, layered oxides face phase transition during cycling, accompanied by severe electrochemical performance degradation, which greatly limits the long cycling stability. Therefore, it is of great significance to fully understand the mechanism, the origin, the influenced factors, and the inhibition strategies of phase transitions to develop a good cathode material. This review focuses on the phase transition in layered oxide cathodes, pointing out the intrinsic causes and degradation mechanisms of phase transition. Moreover, we summarize the mainstream strategies to inhibit the phase transition, such as elemental doping, surface coating, and structural modification, as well as the novel strategy of introducing anionic redox. We hope that this review provides new comprehension in understanding the phase transition of layered oxides and in designing SIBs with superior performance.

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Entropy Tuning Stabilizing P2‐Type Layered Cathodes for Sodium‐Ion Batteries

Cited by 9 publications

References 65 publications

Cation Configuration and Structural Degradation of Layered Transition Metal Oxides in Sodium-Ion Batteries

Cation Configuration and Structural Degradation of Layered Transition Metal Oxides in Sodium-Ion Batteries

Regulating the Charge Distribution of Oxygen by High-Entropy Doping to Stabilize Single-Crystal Ni-Rich Cathode Materials

Perspective on Phase Transition in Layered Oxide Cathodes for Sodium-Ion Batteries: Mechanism, Influenced Factors, and Inhibition Strategies

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