Truncated octahedral LiNi0.5Mn1.5O4 cathode material for ultralong-life lithium-ion battery: Positive (100) surfaces in high-voltage spinel system

Liu, Haidong; Kloepsch, Richard; Wang, Jun; Winter, Martin; Li, Jie

doi:10.1016/j.jpowsour.2015.09.066

Cited by 86 publications

(67 citation statements)

References 49 publications

(38 reference statements)

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“…This leads to higher-surface energy and more vulnerability for Mn dissolution on (100) planes43, but in the meantime, they are also expected to have more facile Li + transport pathways. The superior kinetics of (100) planes as compared with that of the (111) planes was experimentally confirmed on both spinel LiMn 2 O 4 and LMNO cathode materials194445. We believe that this kinetic advantage leads to preferential nucleation of the delithiated phase at the vertices where (100) facets are located.…”

Section: Resultsmentioning

confidence: 67%

Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

et al. 2017

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Understanding the reaction pathway and kinetics of solid-state phase transformation is critical in designing advanced electrode materials with better performance and stability. Despite the first-order phase transition with a large lattice mismatch between the involved phases, spinel LiMn1.5Ni0.5O4 is capable of fast rate even at large particle size, presenting an enigma yet to be understood. The present study uses advanced two-dimensional and three-dimensional nano-tomography on a series of well-formed LixMn1.5Ni0.5O4 (0≤x≤1) crystals to visualize the mesoscale phase distribution, as a function of Li content at the sub-particle level. Inhomogeneity along with the coexistence of Li-rich and Li-poor phases are broadly observed on partially delithiated crystals, providing direct evidence for a concurrent nucleation and growth process instead of a shrinking-core or a particle-by-particle process. Superior kinetics of (100) facets at the vertices of truncated octahedral particles promote preferential delithiation, whereas the observation of strain-induced cracking suggests mechanical degradation in the material.

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Section: Resultsmentioning

confidence: 67%

Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

et al. 2017

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Section: Approaches To Improve the Cycling Stability Of Lnmomentioning

confidence: 99%

Advances and Prospects of High‐Voltage Spinel Cathodes for Lithium‐Based Batteries

Manthiram

2021

Small Methods

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Insertion compounds have been dominating the cathodes in commercial lithium‐ion batteries. In contrast to layered oxides and polyanion compounds, the development of spinel‐structured cathodes is a little behind. Owing to a series of advantageous properties, such as high operating voltage (≈4.7 V), high capacity (≈135 mAh g−1), low environmental impact, and low fabrication cost, the high‐voltage spinel LiNi0.5Mn1.5O4 represents a high‐power cathode for advancing high‐energy‐density Li+‐ion batteries. However, the wide application and commercialization of this cathode are hampered by its poor cycling performance. Recent progress in both the fundamental understanding of the degradation mechanism and the exploration of strategies to enhance the cycling stability of high‐voltage spinel cathodes have drawn continuous attention toward this promising insertion cathode. In this review article, the structure–property correlations and the failure mode of high‐voltage spinel cathodes are first discussed. Then, the recent advances in mitigating the cycling stability issue of high‐voltage spinel cathodes are summarized, including the various approaches of structural design, doping, surface coating, and electrolyte modification. Finally, future perspectives and research directions are put forward, aiming at providing insightful information for the development of practical high‐voltage spinel cathodes.

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“…Several recent studies suggested that the crystalline orientations on the particle surfaces can have significant influences on the electrochemical properties. [19][20][21][22][23][24][25][26][27] In most experiments, different crystalline facets were found to coexist at the surfaces of LiMn 1.5 Ni 0.5 O 4 particles: [21][22][23][24][25][26][27] {111} and {100} surface facets were most frequently observed. Thermodynamically, {111} and {100} facets tend to coexist due to their similar (low) surface energies, while eliminating {100} facets appears to benefit rate capability and cycling stability.…”

Section: Introductionmentioning

confidence: 99%

Enhancing the Ion Transport in LiMn_1.5Ni_0.5O₄ by Altering the Particle Wulff Shape via Anisotropic Surface Segregation

Huang

Liu

Zhou

et al. 2017

ACS Appl. Mater. Interfaces

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Spontaneous and anisotropic surface segregation of W cations in LiMnNiO particles can alter the Wulff shape and improve surface stability, thereby significantly improving the electrochemical performance. An Auger electron nanoprobe was employed to identify the anisotropic surface segregation, whereby W cations prefer to segregate to {110} surface facets to decrease its relative surface energy according to Gibbs adsorption theory and subsequently increase its surface area according to Wulff theory. Consequently, the rate performance is improved (e.g., by ∼5-fold at a high rate of 25C) because the {110} facets have more open channels for fast lithium ion diffusion. Furthermore, X-ray photoelectron spectroscopy (XPS) depth profiling suggested that the surface segregation and partial reduction of W cation inhibit the formation of Mn on surfaces to improve cycling stability via enhancing the cathode electrolyte interphase (CEI) stability at high charging voltages. This is the first report of using anisotropic surface segregation to thermodynamically control the particle morphology as well as enhancing CEI stability as a facile, and potentially general, method to significantly improve the electrochemical performance of battery electrodes. Combining neutron diffraction, an Auger electron nanoprobe, XPS, and other characterizations, we depict the underlying mechanisms of improved ionic transport and CEI stability in high-voltage LiMnNiO spinel materials.

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Truncated octahedral LiNi0.5Mn1.5O4 cathode material for ultralong-life lithium-ion battery: Positive (100) surfaces in high-voltage spinel system

Cited by 86 publications

References 49 publications

Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

Advances and Prospects of High‐Voltage Spinel Cathodes for Lithium‐Based Batteries

Enhancing the Ion Transport in LiMn_1.5Ni_0.5O₄ by Altering the Particle Wulff Shape via Anisotropic Surface Segregation

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Truncated octahedral LiNi0.5Mn1.5O4 cathode material for ultralong-life lithium-ion battery: Positive (100) surfaces in high-voltage spinel system

Cited by 86 publications

References 49 publications

Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

Advances and Prospects of High‐Voltage Spinel Cathodes for Lithium‐Based Batteries

Enhancing the Ion Transport in LiMn1.5Ni0.5O4 by Altering the Particle Wulff Shape via Anisotropic Surface Segregation

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Enhancing the Ion Transport in LiMn_1.5Ni_0.5O₄ by Altering the Particle Wulff Shape via Anisotropic Surface Segregation