Understanding the impact of calcination time of high-voltage spinel Li1+Ni0.5Mn1.5O4 on structure and electrochemical behavior

Betz, Johannes; Nowak, Laura; Brinkmann, Jan‐Paul; Bärmann, Peer; Diehl, Marcel; Winter, Martin; Placke, Tobias; Schmuch, Richard

doi:10.1016/j.electacta.2019.134901

Cited by 15 publications

(18 citation statements)

References 47 publications

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“…Typically, cathode materials that are in the 4 V potential range have surface areas near to 3 m 2 .g -1 [38]. The obtained lower electrochemical results, compared with other works [38][39][40][41], can be thus also explained by the higher particle surface area of the materials used in the present work (Table 3). With the increase of current rates, the plateau voltages between the charge and discharge increase and decrease, respectively, due to the increased cell polarization, as well the gradually blurry of the two plateaus [42].…”

Section: Electrochemical Studies Of the Cathodesmentioning

confidence: 59%

Improved electrochemical performance of LiMn1.5M0.5O4 (M=Ni, Co, Cu) based cathodes for lithium-ion batteries

Sharma

Ram

Ferdov

et al. 2021

Journal of Alloys and Compounds

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Section: Electrochemical Studies Of the Cathodesmentioning

confidence: 59%

Improved electrochemical performance of LiMn1.5M0.5O4 (M=Ni, Co, Cu) based cathodes for lithium-ion batteries

Sharma

Ram

Ferdov

et al. 2021

Journal of Alloys and Compounds

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“…The hierarchical structure of LNMO typically consists of interconnected primary particles (e.g., 100–600 nm in diameter), which can form larger secondary particles (e.g., 5–20 μm in diameter). − Representative SEM images for both the as-prepared LNMO particles (i.e., without a LiNbO 3 coating) and the LiNbO 3 -coated LNMO particles are shown in Figure . Both samples resembled similar octahedral-shaped particles with diameters ranging from ∼1 to 6 μm.…”

Section: Resultsmentioning

confidence: 99%

Enabling a High-Throughput Characterization of Microscale Interfaces within Coated Cathode Particles

Taylor

Nesvaderani²,

Ovens

et al. 2021

ACS Appl. Energy Mater.

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Lithium-ion batteries represent an emerging field. The development of battery materials could benefit from quick techniques that enable atomic-level diagnostics. High-performance cathodes, such as high-voltage spinel, often require coatings to protect against the destructive electrochemical environments at the particle–electrolyte interface. The preparations of these coatings are still in the early phases of development, and their analytical inspection by high-resolution scanning and transmission electron microscopy (HR-S/TEM) techniques presents a significant challenge due to the microscale dimensions of the cathode particles. In this work, a high-throughput ultramicrotome technique was assessed for the characterization of the particle–coating interface. The ultramicrotome technique enabled the rapid preparation of cross sections with a thickness of 126 ± 66 nm as determined by electron energy loss spectroscopy (EELS) measurements. Cathode particles composed of high-voltage spinel, LiNi0.5Mn1.5O4 (LNMO), coated with lithium niobate (LiNbO3) were synthesized, and cross sections were inspected using HR-S/TEM techniques. These ultrathin cross sections enabled the ability to obtain nanoscale information regarding the composition and crystallinity of the particle–coating interface over lateral areas of >1 μm. Accessible correlations between the electrochemical performance of the LiNbO3-coated LNMO particles and the HR-S/TEM results were enabled by the high-throughput method. Discharge capacity measurements were acquired over a series of 100 electrochemical cycles for both the LiNbO3 coated and the as-prepared LNMO particles. The limitations of the ultramicrotome technique are also discussed herein with respect to the coating morphology and the procedure for guidance toward technique optimization. The rapid preparation of ultrathin cross sections can assist the advancement of protective coatings on the surfaces of cathode particles for an efficient characterization of bulk–surface interfaces.

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“…Recently, some studies have demonstrated substantially improved reversibility of consecutive Ni For a fair comparison, the values of LCO were calculated based on the operation with a 4.6 V charge cut-off. [18] and Mn redox reactions in LNMO cathodes, realized by tuning the nickel-manganese ordering through additional annealing [39] and adapting the secondary particle morphology. [40,41] Despite the improvements, a comprehensive explanation of the inconsistent cycling performance and origin of the deterioration of LNMO upon wide-voltage cycling remain elusive.…”

Section: Introductionmentioning

confidence: 99%

Regulating Dynamic Electrochemical Interface of LiNi_0.5Mn_1.5O₄ Spinel Cathode for Realizing Simultaneous Mn and Ni Redox in Rechargeable Lithium Batteries

Lim

Shin

Chae

et al. 2022

Advanced Energy Materials

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The exploding electric‐vehicle market requires cost‐effective high‐energy materials for rechargeable lithium batteries. The manganese‐rich spinel oxide LiNi0.5Mn1.5O4 (LNMO) can store a capacity greater than 200 mAh g−1 based on the multi‐cation (Ni2+/Ni4+ and Mn3+/Mn4+) redox centers. However, its practical capacity is limited to Ni2+/Ni4+ redox (135 mAh g−1) due to the poor reversibility of Mn3+/Mn4+ redox. This instability is generally attributed to the Jahn–Teller distortion of Mn3+ and its disproportionation, which leads to severe Mn dissolution. Herein, for the first time, the excellent reversibility of Mn3+/Mn4+ redox within 2.3–4.3 V is demonstrated, requiring revisiting the previous theory. LNMO loses capacity only within a wide voltage range of 2.3–4.9 V. It is revealed that a dynamic evolution of the electrochemical interface, for example, potential‐driven rocksalt phase formation and decomposition, repeatedly occurs during cycling. The interfacial evolution induces electrolyte degradation and surface passivation, impeding the charge‐transfer reactions. It is further demonstrated that stabilizing the interface by electrolyte modification extends the cycle life of LNMO while using the multi‐cation redox, enabling 71.5% capacity retention of LNMO after 500 cycles. The unveiled dynamic oxide interface will propose a new guideline for developing Mn‐rich cathodes by realizing the reversible Mn redox.

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Understanding the impact of calcination time of high-voltage spinel Li1+Ni0.5Mn1.5O4 on structure and electrochemical behavior

Cited by 15 publications

References 47 publications

Improved electrochemical performance of LiMn1.5M0.5O4 (M=Ni, Co, Cu) based cathodes for lithium-ion batteries

Improved electrochemical performance of LiMn1.5M0.5O4 (M=Ni, Co, Cu) based cathodes for lithium-ion batteries

Enabling a High-Throughput Characterization of Microscale Interfaces within Coated Cathode Particles

Regulating Dynamic Electrochemical Interface of LiNi_0.5Mn_1.5O₄ Spinel Cathode for Realizing Simultaneous Mn and Ni Redox in Rechargeable Lithium Batteries

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Understanding the impact of calcination time of high-voltage spinel Li1+Ni0.5Mn1.5O4 on structure and electrochemical behavior

Cited by 15 publications

References 47 publications

Improved electrochemical performance of LiMn1.5M0.5O4 (M=Ni, Co, Cu) based cathodes for lithium-ion batteries

Improved electrochemical performance of LiMn1.5M0.5O4 (M=Ni, Co, Cu) based cathodes for lithium-ion batteries

Enabling a High-Throughput Characterization of Microscale Interfaces within Coated Cathode Particles

Regulating Dynamic Electrochemical Interface of LiNi0.5Mn1.5O4 Spinel Cathode for Realizing Simultaneous Mn and Ni Redox in Rechargeable Lithium Batteries

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Product

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Regulating Dynamic Electrochemical Interface of LiNi_0.5Mn_1.5O₄ Spinel Cathode for Realizing Simultaneous Mn and Ni Redox in Rechargeable Lithium Batteries