Mechanism of Degradation of Capacity and Charge/Discharge Voltages of High‐Ni Cathode During Fast Long‐Term Cycling Without Voltage Margin

Park, Jae Yeol; Jo, Minji; Hong, Soon Hyeok; Park, Seunggyu; Park, Jae‐Ho; Kim, Yong‐Il; Kim, Sang‐Ok; Chung, Kyung Yoon; Byun, Dongjin; Kim, Seung Min; Chang, Wonyoung

doi:10.1002/aenm.202201151

Cited by 11 publications

(3 citation statements)

References 25 publications

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“…Reference EELS spectra corresponding to the oxidation states of Mn 2+ , Mn 3+ , and Mn 4+ are presented in Figure S4. The O K pre-edge/main edge ratio also indicates the total oxidation states of TMs and O because the O K pre-edge peak originates from the concentration of the unoccupied states in the hybridized orbital between the 2p orbital of O and 3d orbital of TMs. , …”

Section: Results and Discussionmentioning

confidence: 99%

Controlling Surface Structure and Primary Particle Size to Enhance Performance and Reduce Gas Evolution in Lithium- and Manganese-Rich Layered Oxide Cathodes

Park,

Choi,

Lee

et al. 2024

ACS Appl. Mater. Interfaces

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Practical application of lithium-and manganese-rich layered oxide cathodes has been hindered despite their high performance and low cost owing to high gas evolution accompanying capacity loss even in a conservative voltage window. Here, we control the surface structure and primary particle size of lithium-and manganese-rich layered oxide cathodes not only to enhance the electrochemical performance but also to reduce gas evolution. Sulfur-coated Fm3̅ m/R3̅ m double reduced surface layers and Mo doping dramatically reduce gas evolution, which entails the improvement of electrochemical performance. With the optimization, we prove that it is competitive enough to conventional high-nickel cathodes in the aspects of gas evolution as well as electrochemical performance in the conservative voltage window of 2.5−4.4 V. Our findings provide invaluable insights on the improvement of electrochemical performance and gas evolution properties in lithium-and manganese-rich layered oxide cathodes.

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Section: Results and Discussionmentioning

confidence: 99%

Controlling Surface Structure and Primary Particle Size to Enhance Performance and Reduce Gas Evolution in Lithium- and Manganese-Rich Layered Oxide Cathodes

Park,

Choi,

Lee

et al. 2024

ACS Appl. Mater. Interfaces

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“…The voltage decay may be due to the involvement of anionic oxygen in the redox reaction at high charge voltage (> 4.2 V) and the irreversible hexagonal H2→H3 transition. 45 H2→H3 phase transition leads to lattice distortion, and the transfer of Ni ions to Li layer leads to increased cation mixing and structural phase transition, which will hinder the migration of Li ions, increase the overpotential of the material, and reduce the electrode potential. [45][46][47][48] By constructing an artificial CEI film on the surface of NCM, a Q-NCM material with excellent cycling performance and suppressed voltage decay can be obtained.…”

Section: Resultsmentioning

confidence: 99%

“…45 H2→H3 phase transition leads to lattice distortion, and the transfer of Ni ions to Li layer leads to increased cation mixing and structural phase transition, which will hinder the migration of Li ions, increase the overpotential of the material, and reduce the electrode potential. [45][46][47][48] By constructing an artificial CEI film on the surface of NCM, a Q-NCM material with excellent cycling performance and suppressed voltage decay can be obtained. Among them, Q-NCM-4 demonstrates the best electrochemical performance and is abbreviated as Q-NCM.…”

Section: Resultsmentioning

confidence: 99%

Quenching-Induced Ultrathin LiF-Rich Interphases on LiNi_0.8Co_0.1Mn_0.1O₂ Cathode

Li,

Zhang,

Chen

et al. 2024

J. Electrochem. Soc.

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Nickel-rich layered oxides (NCM) are a promising contender material for the cathode electrode of high-energy lithium-ion batteries (LIBs) due to their large reversible capacity and high operating voltage. However, the poor surface/interfacial stability and the dissolution of transition metal ions hinder the commercial application of NCM. To create an artificial cathode electrolyte interphase (CEI) with LiF-rich inorganic phase on the NCM surface, a practical and efficient way of quenching the NCM powder from high temperature in 1,1,2,2-Tetrafluoroethyl 2,2,2-trifluoroethyl ether (HFE) was devised. With this artificial CEI film, the side reactions between NCM and electrolytes are inhibited, and the dissolution of TM ions is retarded. The quenched-NCM achieved fantastic cycling performance and suppressed voltage decay. Our research offers an efficient and worthy approach for improving the surface/interfacial stabilization of nickel-rich cathode materials for high-energy-density LIBs.

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Voltage Hysteresis in Transition Metal Oxide Cathodes for Li/Na‐Ion Batteries

Liu

et al. 2023

Adv Funct Materials

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essential for the commercial application of Li/Na-ion batteries. The investigated cathode materials mainly include oxides, polyanion compounds, Prussian blue analogues, and organic salts. Among them, layered transition metal oxides contained in oxides are promising candidates due to their suitable operational potentials, 2D ions diffusion channels, and simple synthesis. Meanwhile, it was generally believed that to achieve a fast ions diffusion, the atomic configuration in the crystal structure of layered cathode materials must be well ordered. [7,8] However, this stereotype is now being reconsidered with the discovery of the percolation theory about 3D ions diffusion in a disordered rock-salt (DRX) structure. [9,10] This percolation occurs when Li-ions hop from one octahedral site to another through an intermediate tetrahedral site, where the Liions in the tetrahedral sites are identified as an active Li for the hopping. [11] In this regard, various new types of Li-rich DRX cathode materials with promising capacities (>250 mAh g −1 ) have been discovered. [12][13][14][15][16][17][18][19] Given their unique advantages, these oxide materials have attracted extensive attention from researchers worldwide.Although demonstrating a high capacity, application-wise, these oxide materials also exhibit voltage hysteresis and significant loss of energy density, since the voltage associated with this redox process on charge cannot be recovered on discharge, which represents a key challenge that inhibits exploiting the full potential of these materials. This voltage hysteresis persists throughout the electrochemical cycling, resulting in a continuous decrease of the average discharge voltage. Therefore, the understanding of voltage hysteresis is particularly important because it not only minimizes energy density and drastically reduces energy efficiency but also hinders further development and commercialization of Li/Na-ion batteries. When voltage hysteresis was discovered in LiFePO 4 materials in the early years, experimental limitations and the lack of a theoretical framework prevented researchers from drawing concrete conclusions about the phenomenon. With the development of increasingly sophisticated analytical techniques for studying voltage hysteresis, reassessing the understanding of the origin of voltage hysteresis can now be done from a mechanical perspective and even reveal new discoveries that were previously unavailable due to experimental limitations. [20]

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Mechanism of Degradation of Capacity and Charge/Discharge Voltages of High‐Ni Cathode During Fast Long‐Term Cycling Without Voltage Margin

Cited by 11 publications

References 25 publications

Controlling Surface Structure and Primary Particle Size to Enhance Performance and Reduce Gas Evolution in Lithium- and Manganese-Rich Layered Oxide Cathodes

Controlling Surface Structure and Primary Particle Size to Enhance Performance and Reduce Gas Evolution in Lithium- and Manganese-Rich Layered Oxide Cathodes

Quenching-Induced Ultrathin LiF-Rich Interphases on LiNi_0.8Co_0.1Mn_0.1O₂ Cathode

Voltage Hysteresis in Transition Metal Oxide Cathodes for Li/Na‐Ion Batteries

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Mechanism of Degradation of Capacity and Charge/Discharge Voltages of High‐Ni Cathode During Fast Long‐Term Cycling Without Voltage Margin

Cited by 11 publications

References 25 publications

Controlling Surface Structure and Primary Particle Size to Enhance Performance and Reduce Gas Evolution in Lithium- and Manganese-Rich Layered Oxide Cathodes

Controlling Surface Structure and Primary Particle Size to Enhance Performance and Reduce Gas Evolution in Lithium- and Manganese-Rich Layered Oxide Cathodes

Quenching-Induced Ultrathin LiF-Rich Interphases on LiNi0.8Co0.1Mn0.1O2 Cathode

Voltage Hysteresis in Transition Metal Oxide Cathodes for Li/Na‐Ion Batteries

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Quenching-Induced Ultrathin LiF-Rich Interphases on LiNi_0.8Co_0.1Mn_0.1O₂ Cathode