Dataset Information

Optimized Morphology and Tuning the Mn³⁺ Content of LiNi_0.5Mn_1.5O₄ Cathode Material for Li-Ion Batteries.

ABSTRACT: The advantages of cobalt-free, high specific capacity, high operating voltage, low cost, and environmental friendliness of spinel LiNi_0.5Mn_1.5O₄ (LNMO) material make it one of the most promising cathode materials for next-generation lithium-ion batteries. The disproportionation reaction of Mn³⁺ leads to Jahn-Teller distortion, which is the key issue in reducing the crystal structure stability and limiting the electrochemical stability of the material. In this work, single-crystal LNMO was synthesized successfully by the sol-gel method. The morphology and the Mn³⁺ content of the as-prepared LNMO were tuned by altering the synthesis temperature. The results demonstrated that the LNMO_110 material exhibited the most uniform particle distribution as well as the presence of the lowest concentration of Mn³⁺, which was beneficial to ion diffusion and electronic conductivity. As a result, this LNMO cathode material had an optimized electrochemical rate performance of 105.6 mAh g^-1 at 1 C and cycling stability of 116.8 mAh g^-1 at 0.1 C after 100 cycles.

SUBMITTER: Lin Y

PROVIDER: S-EPMC10142292 | biostudies-literature | 2023 Apr

REPOSITORIES: biostudies-literature

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Publications

Optimized Morphology and Tuning the Mn3+ Content of LiNi0.5Mn1.5O4 Cathode Material for Li-Ion Batteries.

Lin Yan Y Välikangas Juho J Sliz Rafal R Molaiyan Palanivel P Hu Tao T Lassi Ulla U

Materials (Basel, Switzerland) 20230415 8

The advantages of cobalt-free, high specific capacity, high operating voltage, low cost, and environmental friendliness of spinel LiNi0.5Mn1.5O4 (LNMO) material make it one of the most promising cathode materials for next-generation lithium-ion batteries. The disproportionation reaction of Mn3+ leads to Jahn-Teller distortion, which is the key issue in reducing the crystal structure stability and limiting the electrochemical stability of the material. ...[more]

PMID: 37109953

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Project description:The high-voltage LiNi0.5Mn1.5O4 (LNMO) spinel cathode material offers high energy density storage capabilities without the use of costly Co that is prevalent in other Li-ion battery chemistries (e.g., LiNixMnyCozO2 (NMC)). Unfortunately, LNMO-containing batteries suffer from poor cycling performance because of the intrinsically coupled processes of electrolyte oxidation and transition metal dissolution that occurs at high voltage. In this work, we use operando electron paramagnetic resonance (EPR) and nuclear magnetic resonance (NMR) spectroscopies to demonstrate that transition metal dissolution in LNMO is tightly coupled to HF formation (and thus, electrolyte oxidation reactions as detected with operando and in situ solution NMR), indicative of an acid-driven disproportionation reaction that occurs during delithiation (i.e., battery charging). Leveraging the temporal resolution (s-min) of magnetic resonance, we find that the LNMO particles accelerate the rate of LiPF6 decomposition and subsequent Mn2+ dissolution, possibly due to the acidic nature of terminal Mn-OH groups. X-ray photoemission electron microscopy (XPEEM) provides surface-sensitive and localized X-ray absorption spectroscopy (XAS) measurements, in addition to X-ray photoelectron spectroscopy (XPS), that indicate disproportionation is enabled by surface reconstruction upon charging, which leads to surface Mn3+ sites on the LNMO particle surface that can disproportionate into Mn2+(dissolved) and Mn4+(s). During discharge of the battery, we observe high quantities of metal fluorides (in particular, MnF2) in the cathode electrolyte interphase (CEI) on LNMO as well as the conductive carbon additives in the composite. Electronic conductivity measurements indicate that the MnF2 decreases film conductivity by threefold compared to LiF, suggesting that this CEI component may impede both the ionic and electronic properties of the cathode. Ultimately, to prevent transition metal dissolution and the associated side reactions in spinel-type cathodes (particularly those that operate at high voltages like LNMO), the use of electrolytes that offer improved anodic stability and prevent acid byproducts will likely be necessary.

Dataset Information

Optimized Morphology and Tuning the Mn³⁺ Content of LiNi_0.5Mn_1.5O₄ Cathode Material for Li-Ion Batteries.

Publications

Optimized Morphology and Tuning the Mn<sup>3+</sup> Content of LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> Cathode Material for Li-Ion Batteries.

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