High-performance Ni-rich Li[Ni0.9–xCo0.1Alx]O2 cathodes via multi-stage microstructural tailoring from hydroxide precursor to the lithiated oxide

Park, Geon Tae; Park, Nam Yung; Noh, Tae Chong; Namkoong, Been; Ryu, Hoon; Shin, Ji Yong; Beierling, Thorsten; Yoon, Chong Seung; Sun, Yang Kook

doi:10.1039/d1ee01773j

Cited by 65 publications

(52 citation statements)

References 42 publications

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“…This demonstrates that CSG‐NCAB87, whose microstructure is tolerant to crack formation, suppresses cathode degradation even when the electrolyte exposure time at a high SoC is extended, whereas the exposure time critically affects the degradation of CSG‐NCA88, because the particle interior is exposed to the electrolyte via the microcracks. [ 18,24,27–30 ]…”

Section: Resultsmentioning

confidence: 99%

“…Microstructural manipulation can be achieved by compositional gradient design of transition metal ions [ 19,24,25,31 ] or by doping with various atoms (e.g., B, Ta, Mo, W, and Sb) during lithiation. [ 18,26–30,32,33 ] Furthermore, a reduction in volume deformation and internal stress inside the particle via Al doping can enhance the structural integrity and robustness of cathode. [ 30,34,35 ]…”

Section: Introductionmentioning

confidence: 99%

“…[ 18,26–30,32,33 ] Furthermore, a reduction in volume deformation and internal stress inside the particle via Al doping can enhance the structural integrity and robustness of cathode. [ 30,34,35 ]…”

Section: Introductionmentioning

confidence: 99%

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High‐Energy Ni‐Rich Cathode Materials for Long‐Range and Long‐Life Electric Vehicles

Namkoong

Park

et al. 2022

Advanced Energy Materials

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of the global EV market, Li-ion battery (LIB) technology has progressed to meet the demand for longer driving ranges and extended service lives, while increasing the thermal stability and reducing the cost of the battery. As the performance of LIBs is largely determined by the cathode material, the development of high-performance LIBs for EVs has focused on increasing the capacity of the cathode by usingHowever, cathodes with a high Ni content suffer from inherent structural and chemical instabilities, which lead to rapid capacity fading and thermal instability. [3][4][5][6][7][8][9] In particular, the rapid capacity fading of Ni-rich layered cathodes is largely caused by microcracking and the resultant microstructural instability. [9][10][11][12][13][14][15][16][17][18][19] Microcracks create channels through which the electrolyte can infiltrate the cathode particles, which increases the surface area exposed to electrolyte and worsens parasitic electrolyte attack. The subsequent degradation of the internal surfaces accelerates the accumulation of NiO-like impurity layers at the cathode-electrolyte interface, which hinders electrochemical reactions. [9,[19][20][21][22][23][24][25] As microcracking is caused by abrupt contraction of the unit cells during the H2-H3 phase transition at a high state of charge (SoC), microstructural engineering to facilitate the dissipation of internal mechanical strain and mitigate microcracking in the cathode particles has been extensively investigated. [19,21,[24][25][26][27][28][29][30] One such engineered microstructure is a highly oriented microstructure in which elongated primary particles are aligned along the radial direction in the secondary particle periphery. This radial alignment of rod-shaped primary particles effectively dissipates localized strain by allowing the unit cell to contract and expand uniformly. Microstructural manipulation can be achieved by compositional gradient design of transition metal ions [19,24,25,31] or by doping with various atoms (e.g., B, Ta, Mo, W, and Sb) during lithiation. [18,[26][27][28][29][30]32,33] Furthermore, a reduction in volume deformation and internal stress inside the particle via Al doping can enhance the structural integrity and robustness of cathode. [30,34,35] In addition to microcracking, the time during which highly reactive Ni 4+ ions are exposed to the electrolyte when the cathode is in a highly charged state also affects the deterioration of the cathode. Although the exposure time is not Li-ion batteries (LIBs) in electric vehicles (EVs) are usually operated intermittently and maintained at high states of charge (SoCs) for long periods. Because the internal particles of Ni-rich cathodes are easily exposed to the electrolyte at high SoCs owing to mechanical instability, the electrolyte exposure time-during which highly reactive Ni 4+ ions react with the electrolyte-critically affects the degradation of the cathode. Here, 1 mol% B doping of a core-shell concentration gradient (CSG) Li[Ni 0.88 Co 0.10 Al 0.02 ]O 2 cathode (C...

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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High‐Energy Ni‐Rich Cathode Materials for Long‐Range and Long‐Life Electric Vehicles

Namkoong

Park

et al. 2022

Advanced Energy Materials

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“…A secondary particle with pure radially-aligned primary particles improves the rate performance and structure integrity further compared to the double-layer design at the cost of energy density due to the absence of a Ni-rich core. 54 At the electrode level, porosity and thickness are more influential for electrodes with small particles as only a fraction of the electrode close to the separator is affected by the SST, in contrast to that with large particles. Building on this knowledge, electrode with layered particle size distribution is proved to further enhance the rate performance without sacrificing the gravimetric energy density.…”

Section: Single Crystal Vs Polycrystalline Nmc Electrodesmentioning

confidence: 99%

Multi-length scale microstructural design of lithium-ion battery electrodes for improved discharge rate performance

Zhang

Tan

et al. 2021

Energy Environ. Sci.

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“…The most extensive efforts to improve the performance of LIBs have focused on the intrinsic chemistry, via the electrolytes, 4-10 binders, [11][12][13][14] anodes, [15][16][17][18] and cathode materials. [19][20][21][22][23][24][25][26] However, only incremental changes in the cell chemistry (e.g., increasing Ni content in cathode; increased Si loading in blended anodes with graphite) have found commercial success over the past decade. The slow commercial progress of new chemistries dictates the need for alternative electrode and cell designs that can enhance battery performance.…”

Section: Introductionmentioning

confidence: 99%

Camphene-Assisted Fabrication of Free-Standing Lithium-Ion Battery Electrode Composites

Weeks

Lauro

Burrow

et al. 2022

Preprint

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Continually increasing technological demands and widespread adoption of electric vehicles has spurred significant motivation to improve the performance of lithium-ion batteries (LIBs). In addition to improving intrinsic battery chemistry, optimizing electrode morphology and cell design can unlock increased energy density and rate capability to enable the adoption of next generation LIBs for societal decarbonization. Although free-standing electrode (FSE) architectures hold the potential to dramatically increase the gravimetric and volumetric energy density of LIBs by eliminating the parasitic dead weight and volume associated with traditional metal foil current collectors, current FSE fabrication methods suffer from insufficient mechanical stability, electrochemical performance, or industrial adaptability. Here, we demonstrate a scalable camphene-assisted fabrication method that allows simultaneous casting and templating of FSEs comprised of common LIB materials with performance superior to foil-cast counterparts. These porous, lightweight, and robust electrodes simultaneously enable enhanced rate performance by improving mass and ion transport within the percolating conductive carbon pore network and eliminating current collectors for efficient and stable Li+ storage (> 1000 cycle in half-cells) at increased gravimetric and areal energy densities. Compared to conventional foil-cast counterparts, the camphene-derived electrodes exhibit ~1.5x enhanced gravimetric energy density, increased rate capability, and improved capacity retention in coin-cell configurations. A full cell with freestanding anode and cathode cycled for over 250 cycles with greater than 80% capacity retention at an areal capacity of 0.73 mAh/cm2 . This active-material-agnostic electrode fabrication method holds the potential to tailor the morphology of flexible, current-collector-free electrodes to optimize LIBs for high power or high energy density Li+ storage and is applicable to other electrochemical technologies and advanced manufacturing methods

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High-performance Ni-rich Li[Ni_0.9–xCo_0.1Al_x]O₂ cathodes via multi-stage microstructural tailoring from hydroxide precursor to the lithiated oxide

Abstract: Recharging capability of Ni-rich layered cathodes deteriorates rapidly upon cycling mainly from mechanical instability caused by removing a large amount of Li ions from the host structure. Through multi-stage microstructural...

Cited by 65 publications

References 42 publications

High‐Energy Ni‐Rich Cathode Materials for Long‐Range and Long‐Life Electric Vehicles

High‐Energy Ni‐Rich Cathode Materials for Long‐Range and Long‐Life Electric Vehicles

Multi-length scale microstructural design of lithium-ion battery electrodes for improved discharge rate performance

Camphene-Assisted Fabrication of Free-Standing Lithium-Ion Battery Electrode Composites

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