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Influence of sintering temperatures on microstructure and electrochemical performances of LiNi_0.93Co_0.04Al_0.03O₂ cathode for high energy lithium ion batteries.

ABSTRACT: In this study, we present a method for synthesizing Ni-rich LiNi_0.93Co_0.04Al_0.03O₂ (NCA) with a high-energy cathode material by the solid-phase method. The sintering temperature plays a very important role in the electrochemical performance of the LiNi_0.93Co_0.04Al_0.03O₂ since it affects the crystallinity and structural stability. Therefore, various sintering temperatures (660 °C/690 °C/720 °C/750 °C/780 °C/810 °C) are studied to get optimum electrochemical performances. The electrochemical performance of LiNi_0.93Co_0.04Al_0.03O₂ sintered at 720 °C shows the highest discharge capacity of 217.48 mAh g^-1 with excellent Coulombic efficiency of 87.84% at 0.1 C. Moreover, the LiNi_0.93Co_0.04Al_0.03O₂ sintered at 720 °C exhibits excellent rate-capability (181.1 mAh g^-1 at 2.0 C) as well as superior cycle stability (95.4% after 80 cycles at 0.5 C). This is because optimized sintering temperature leads to good structural stability with low cation disorder and residual lithium content.

SUBMITTER: Park HJ

PROVIDER: S-EPMC9187639 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Influence of sintering temperatures on microstructure and electrochemical performances of LiNi0.93Co0.04Al0.03O2 cathode for high energy lithium ion batteries.

Park Hye-Jin HJ Sim Seong-Ju SJ Jin Bong-Soo BS Lee Seung-Hwan SH Kim Hyun-Soo HS

Scientific reports 20220610 1

In this study, we present a method for synthesizing Ni-rich LiNi0.93Co0.04Al0.03O2 (NCA) with a high-energy cathode material by the solid-phase method. The sintering temperature plays a very important role in the electrochemical performance of the LiNi0.93Co0.04Al0.03O2 since it affects the crystallinity and structural stability. Therefore, various sintering temperatures (660 °C/690 °C/720 °C/750 °C/780 °C/81 ...[more]

PMID: 35688883

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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

Influence of sintering temperatures on microstructure and electrochemical performances of LiNi_0.93Co_0.04Al_0.03O₂ cathode for high energy lithium ion batteries.

Publications

Influence of sintering temperatures on microstructure and electrochemical performances of LiNi<sub>0.93</sub>Co<sub>0.04</sub>Al<sub>0.03</sub>O<sub>2</sub> cathode for high energy lithium ion batteries.

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