Lithium-ion (de)intercalation mechanism in core-shell layered Li(Ni,Co,Mn)O2 cathode materials

Hua, Weibo; Schwarz, Björn; Azmi, Raheleh; Müller, Marcus; Darma, Mariyam Susana Dewi; Knapp, Michael; Senyshyn, Anatoliy; Heere, Michael; Missyul, Alkesandr; Simonelli, Laura; Binder, Joachim R.; Indris, Sylvio; Ehrenberg, Helmut

doi:10.1016/j.nanoen.2020.105231

Cited by 59 publications

(41 citation statements)

References 38 publications

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“…Time-resolved in situ high-resolution synchrotron radiation diffraction (SRD) is a powerful approach to trace the structural evolution and phase transformation during inorganic reactions. [22][23][24] To study the formation mechanism of LNCM622O, in situ high-temperature SRD (HTSRD) was used to observe the changes of various phases from a mixture of the Li-free precursor, Ni 0.6 Co 0.2 Mn 0.2 (OH) 2 (NCM622OH) or Ni 0.6 Co 0.2 Mn 0.2 CO 3 (NCM622CO), together with lithium source to the final product under both isothermal and nonisothermal conditions. The experimental details are shown in the supplementary information.…”

Section: Resultsmentioning

confidence: 99%

Kinetic Control of Long‐Range Cationic Ordering in the Synthesis of Layered Ni‐Rich Oxides

Wang

Hua

Missyul

et al. 2021

Adv Funct Materials

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Deciphering the sophisticated interplay between thermodynamics and kinetics of high‐temperature lithiation reaction is fundamentally significant for designing and preparing cathode materials. Here, the formation pathway of Ni‐rich layered ordered LiNi0.6Co0.2Mn0.2O2 (O‐LNCM622O) is carefully characterized using in situ synchrotron radiation diffraction. A fast nonequilibrium phase transition from the reactants to a metastable disordered Li1−x(Ni0.6Co0.2Mn0.2)1+xO2 (D‐LNCM622O, 0 < x < 0.95) takes place while lithium/oxygen is incorporated during heating before the generation of the equilibrium phase (O‐LNCM622O). The time evolution of the lattice parameters for layered nonstoichiometric D‐LNCM622O is well‐fitted to a model of first‐order disorder‐to‐order transition. The long‐range cation disordering parameter, Li/TM (TM = Ni, Co, Mn) ion exchange, decreases exponentially and finally reaches a steady‐state as a function of heating time at selected temperatures. The dominant kinetic pathways revealed here will be instrumental in achieving high‐performance cathode materials. Importantly, the O‐LNCM622O tends to form the D‐LNCM622O with Li/O loss above 850 °C. In situ XRD results exhibit that the long‐range cationic (dis)ordering in the Ni‐rich cathodes could affect the structural evolution during cycling and thus their electrochemical properties. These insights may open a new avenue for the kinetic control of the synthesis of advanced electrode materials.

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Section: Resultsmentioning

confidence: 99%

Kinetic Control of Long‐Range Cationic Ordering in the Synthesis of Layered Ni‐Rich Oxides

Wang

Hua

Missyul

et al. 2021

Adv Funct Materials

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“…The core-shell structure for Ni-rich NMC materials, in which the core contains more Ni while the shell is richer in Mn, was previously investigated. This strategy can reduce volume expansion and protect the core from electrolyte reactions [76][77][78]. It is reported that the LiNiO 2 core with the LiNi 0.83 Mg 0.17 O 2 shell is capable of providing an initial discharge capacity of 194 mAh g −1 and 230 mAh g −1 for the LiNi 0.83 Al 0.17 O 2 shell and Li-Ni 0.83 Mn 0.17 O 2 shell at 0.2 C. In addition, cathodes with the LNO-LiNi 0.83 Mg 0.17 O 2 and LNO-Li-Ni 0.83 Mn 0.17 O 2 core-shell structures were able to maintain 94 and 92% of their initial capacity, respectively, after 55 cycles, while the LNO-LiNi 0.83 Al 0.17 O 2 electrodes maintained 93% of the initial capacity after 55 cycles at 0.2 C. Although the capacity obtained is quite high, the metal dopant diffuses from the shell to the core structure during the sintering process, indicating that the core-shell structure was not fully successful.…”

Section: Particles and Synthesis Engineeringmentioning

confidence: 99%

Recent Development of Nickel-Rich and Cobalt-Free Cathode Materials for Lithium-Ion Batteries

et al. 2021

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The exponential growth in the production of electric vehicles requires an increasing supply of low-cost, high-performance lithium-ion batteries. The increased production of lithium-ion batteries raises concerns over the availability of raw materials, especially cobalt for batteries with nickel-rich cathodes, in which these constraints can impact the high price of cobalt. The reliance on cobalt in these cathodes is worrisome because it is a high-cost, rare material, with an unstable supply chain. This review describes the need and feasibility of developing cobalt-free high-nickel cathode materials for lithium-ion batteries. The new type of cathode material, LiNi1−x−yMnxAlyO2 promises a completely cobalt-free composition with almost the same electrochemical performance as that of the conventional high-nickel cathode. Therefore, this new type of cathode needs further research for its commercial applications.

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“…Reaction of amine and ketone in presence of NCM 175 mAh g −1 at 1 C rate; CR of 88.8% after 100 cycles at 1 C; voltage range 2.8-4.5 V [199] The concept of core-shell (CS) consists in the synthesis of particles with Ni-enriched core to maximize the capacity and a Ni-depleted shell to avoid the problems met with the surface layer of the Ni-rich materials. This strategy has been employed for more than a decade, with NCM811 core and LiNi 0.5 Mn 0.5 shell [207][208][209][210], and the progress using this strategy was constant through the years [211][212][213][214] [215]. In the corresponding full-cell against the graphite anode between 3.0 and 4.2 V at 1 C, the discharge capacity was nearly 190 mAh g −1 , retained at 165 mAh g −1 after 1000 cycles, performance that paves the route to the synthesis of lithium-ion batteries with higher energy density.…”

Section: Coating Ncmmentioning

confidence: 99%

“…It is very difficult to increase the cycle life up to 1000 cycles with NCM811 alone. It can be used, however, in a core-shell structure of spherical particles designed to a LiNiO2 core and a 0.5 µm-thick NCM811 encapsulating shell, which fulfilled this goal [214]. As recalled above, the radial texturing was essential to achieve the outstanding performance of the compositionally partitioned Li[Ni 0.9 Co 0.05 Mn 0.05 ]O 2 material.…”

Section: The Route To Co-free Ni-rich Batteriesmentioning

confidence: 99%

NCA, NCM811, and the Route to Ni-Richer Lithium-Ion Batteries

Julien

Mauger

2020

Energies

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The aim of this article is to examine the progress achieved in the recent years on two advanced cathode materials for EV Li-ion batteries, namely Ni-rich layered oxides LiNi0.8Co0.15Al0.05O2 (NCA) and LiNi0.8Co0.1Mn0.1O2 (NCM811). Both materials have the common layered (two-dimensional) crystal network isostructural with LiCoO2. The performance of these electrode materials are examined, the mitigation of their drawbacks (i.e., antisite defects, microcracks, surface side reactions) are discussed, together with the prospect on a next generation of Li-ion batteries with Co-free Ni-rich Li-ion batteries.

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Lithium-ion (de)intercalation mechanism in core-shell layered Li(Ni,Co,Mn)O2 cathode materials

Cited by 59 publications

References 38 publications

Kinetic Control of Long‐Range Cationic Ordering in the Synthesis of Layered Ni‐Rich Oxides

Kinetic Control of Long‐Range Cationic Ordering in the Synthesis of Layered Ni‐Rich Oxides

Recent Development of Nickel-Rich and Cobalt-Free Cathode Materials for Lithium-Ion Batteries

NCA, NCM811, and the Route to Ni-Richer Lithium-Ion Batteries

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