Reaction Mechanisms of Layered Lithium‐Rich Cathode Materials for High‐Energy Lithium‐Ion Batteries

Zhao, Shuoqing; Yan, Kang; Zhang, Jinqiang; Sun, Bing; Wang, Guoxiu

doi:10.1002/anie.202000262

Cited by 190 publications

(120 citation statements)

References 81 publications

(255 reference statements)

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“…Detailed reasons will be explained later when discussing the valence profile change during cycling. The outcome of oxygen redox may be in the form of O − 45 , 46 , oxygen vacancy 9 , or O 2 in the lattice 30 . They all can lead to a decrease in the valence of TM, or very likely Mn.…”

Section: Resultsmentioning

confidence: 99%

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Zhang

Wang

et al. 2020

Nat Commun

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Lithium-rich nickel-manganese-cobalt (LirNMC) layered material is a promising cathode for lithium-ion batteries thanks to its large energy density enabled by coexisting cation and anion redox activities. It however suffers from a voltage decay upon cycling, urging for an in-depth understanding of the particle-level structure and chemical complexity. In this work, we investigate the Li1.2Ni0.13Mn0.54Co0.13O2 particles morphologically, compositionally, and chemically in three-dimensions. While the composition is generally uniform throughout the particle, the charging induces a strong depth dependency in transition metal valence. Such a valence stratification phenomenon is attributed to the nature of oxygen redox which is very likely mostly associated with Mn. The depth-dependent chemistry could be modulated by the particles’ core-multi-shell morphology, suggesting a structural-chemical interplay. These findings highlight the possibility of introducing a chemical gradient to address the oxygen-loss-induced voltage fade in LirNMC layered materials.

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Section: Resultsmentioning

confidence: 99%

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Zhang

Wang

et al. 2020

Nat Commun

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“…Compared with the conventional commercial cathode materials, layered lithium-rich manganese-based cathode materials, xLi 2 MnO 3 •(1x)LiMO 2 (M = Mn, Ni, Co, etc. ), which consist of two components of α-NaFeO 2 -structured LiMO 2 (R-3m symmetry) phase and monoclinic Li 2 MnO 3 (C2/m symmetry) phase, have attracted extensive interest due to their low price and higher discharge capacity of more than 250 mA h g −1 (Lin et al, 2008;Yan et al, 2014;Nayak et al, 2018;Yang et al, 2018;Xiang et al, 2019;Gao et al, 2020;Jiang et al, 2020;Zhao et al, 2020). However, several drawbacks, including intrinsic poor capability, poor cycling stability, and voltage fading, hindered its practical applications (Song et al, 2016;Xiang et al, 2017;Hu et al, 2019;Zhang et al, 2019;Sigel et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

Improved Electrochemical Performance of 0.5Li2MnO3·0.5LiNi0.5Mn0.5O2 Cathode Materials for Lithium Ion Batteries Synthesized by Ionic-Liquid-Assisted Hydrothermal Method

et al. 2020

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Well-dispersed Li-rich Mn-based 0.5Li2MnO3·0.5LiNi0.5Mn0.5O2 nanoparticles with diameter ranging from 50 to 100 nm are synthesized by a hydrothermal method in the presence of N-hexyl pyridinium tetrafluoroborate ionic liquid ([HPy][BF4]). The microstructures and electrochemical performance of the prepared cathode materials are characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and electrochemical measurements. The XRD results show that the sample prepared by ionic-liquid-assisted hydrothermal method exhibits a typical Li-rich Mn-based pure phase and lower cation mixing. SEM and TEM images indicate that the extent of particle agglomeration of the ionic-liquid-assisted sample is lower compared to the traditional hydrothermal sample. Electrochemical test results indicate that the materials synthesized by ionic-liquid-assisted hydrothermal method exhibit better rate capability and cyclability. Besides, electrochemical impedance spectroscopy (EIS) results suggest that the charge transfer resistance of 0.5Li2MnO3· 0.5LiNi0.5Mn0.5O2 synthesized by ionic-liquid-assisted hydrothermal method is much lower, which enhances the reaction kinetics.

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“…However, the current LIBs, which are based on conventional carbonaceous anodes, are rapidly falling behind the high energy demands. [ 3,4 ] Thus, significant advances in terms of power density, energy density, cycle life, and safety are in need. [ 5,6 ] Among various candidate materials, silicon has long been proposed as one of the most promising anode materials for next‐generation LIBs due to its high theoretical lithium storage capacity (4200 mAh g −1 ), which is about ten times higher than that of commercial graphite (372 mAh g −1 ).…”

Section: Introductionmentioning

confidence: 99%

Ultrathin Silicon Nanolayer Implanted Ni_xSi/Ni Nanoparticles as Superlong‐Cycle Lithium‐Ion Anode Material

et al. 2020

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It has been claimed that the mechanical properties of electrodes in lithium‐ion batteries have a huge impact on their electrochemical performance. This is especially critical for Si‐based electrodes, which suffer from pulverization and formation of an unstable solid–electrolyte interphase during cycling. Herein, thin silicon‐coated nickel silicide nanoparticles grown on a nickel inner core support (designated as Si@NixSi/Ni) as anode material for a Li‐ion battery are reported. The ultrathin nano silicon layer contributes to achieve reasonably high energy density and allows fast Li‐ion diffusion due to its high specific capacity and shortened Li‐ion diffusion length. While the gradiently distributed NixSi layer enables the attainment of superior cycling stability and further enhances the specific capacity, the Ni inner core provides mechanical support to maintain the structural integrity of the nanoparticles during the extended lithiation/delithiation process. The Si@NixSi/Ni core–shell electrode exhibits a charge‐specific capacity of 706.1 mAh g−1 at a current density of 500 mA g−1. This structure also shows a high first‐cycle Coulombic efficiency of 81.5%. Interestingly, the Si@NixSi/Ni core–shell electrode demonstrates a cycle life of over 5000 cycles with capacity retention of 74% at a current density of 500 mA g−1.

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Reaction Mechanisms of Layered Lithium‐Rich Cathode Materials for High‐Energy Lithium‐Ion Batteries

Cited by 190 publications

References 81 publications

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Improved Electrochemical Performance of 0.5Li2MnO3·0.5LiNi0.5Mn0.5O2 Cathode Materials for Lithium Ion Batteries Synthesized by Ionic-Liquid-Assisted Hydrothermal Method

Ultrathin Silicon Nanolayer Implanted Ni_xSi/Ni Nanoparticles as Superlong‐Cycle Lithium‐Ion Anode Material

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Reaction Mechanisms of Layered Lithium‐Rich Cathode Materials for High‐Energy Lithium‐Ion Batteries

Cited by 190 publications

References 81 publications

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Improved Electrochemical Performance of 0.5Li2MnO3·0.5LiNi0.5Mn0.5O2 Cathode Materials for Lithium Ion Batteries Synthesized by Ionic-Liquid-Assisted Hydrothermal Method

Ultrathin Silicon Nanolayer Implanted NixSi/Ni Nanoparticles as Superlong‐Cycle Lithium‐Ion Anode Material

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Ultrathin Silicon Nanolayer Implanted Ni_xSi/Ni Nanoparticles as Superlong‐Cycle Lithium‐Ion Anode Material