Lithium‐Ion Batteries: Tuning Anionic Redox Activity and Reversibility for a High‐Capacity Li‐Rich Mn‐Based Oxide Cathode via an Integrated Strategy (Adv. Funct. Mater. 10/2019)

Li, Qingyuan; Zhou, Dong; Zhang, Lijuan; Ning, De; Chen, Zhenhua; Xu, Zijian; Gao, Rui; Liu, Xinzhi; Xie, Donghao; Schumacher, G.; Liu, Xiangfeng

doi:10.1002/adfm.201970064

Cited by 29 publications

(29 citation statements)

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“…In addition, the cycling and structural stability of the LOR sample at higher temperatures were improved, which could be used as an indicator of oxygen release at room temperature. [ 27 ] For the LOR cathode, a reversible capacity of 293.5 mAh g −1 was observed after cycling at 0.5 C, 55 °C, which is significantly higher than that of the pristine Li‐rich cathode of 249.7 mAh g −1 (Figure S11c, Supporting Information). The relatively higher reversible capacity at 55 °C than at room temperature originates from the complex reaction mechanism under heating.…”

Section: Resultsmentioning

confidence: 98%

“…Despite the loss of lattice oxygen from both the samples, the much higher content of the lattice O 2− species in the LOR sample, according to the features of the 529.40 eV peak in the O 1s spectra, validates its stabilized oxygen redox reaction. [ 27 ] In addition, the O 1s peak of the electrolyte oxidation species emerged at 533.20 eV in the XPS profile of the pristine sample, but was absent in that of the LOR sample, suggesting suppressed electrolyte decomposition on the surface of the LOR particles. [ 7 ] Moreover, the peaks located at 531.31 eV in the O 1s spectra and 290.05 eV in the C 1s spectra can be assigned to CO 3 2− derived from the decoordination of the lattice oxygen atoms in Li 2 CO 3 .…”

Section: Resultsmentioning

confidence: 99%

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Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Liu

Zhu

et al. 2021

Advanced Energy Materials

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Anionic redox chemistry is emerging as a key concept in the development of high‐energy lithium‐ion batteries, as it enables a nearly doubled charge storage capacity, aiding the development of high‐capacity batteries. However, the anionic reactivity is frequently irreversible from charge to discharge, leading to rapid decay of the capacity and voltage of batteries over long‐term cycling. Although the possibility of controlling the anionic redox reactions by tuning the geometric and electronic structures has recently been proposed, the implementation of this strategy is still a critical challenge. Herein, a strategy is proposed to improve the anionic redox reversibility of a model anionic redox active cathode material, Li1.2Ni0.13Co0.13Mn0.54O2, by tuning the surface ligand geometry via the growth of a lattice‐compatible spinel LiCoO2 coating layer on the particle surface. Detailed local structure and first principles investigations reveal that the shape and orientation of the octahedral layer in the host lattice are modified. Accordingly, a two‐band oxygen redox behavior is triggered in the ligand‐orientation‐regulated Li‐rich cathode, leading to enhanced reversibility, and thus, remarkably improved capacity and voltage retention over cycling. This study highlights the importance of controllable ligand orientation, carving a new path for the development and design of Li‐rich cathodes in the future.

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Section: Resultsmentioning

confidence: 98%

Section: Resultsmentioning

confidence: 99%

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Liu

Zhu

et al. 2021

Advanced Energy Materials

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“…As a result, the O‐ K sXAS pre‐edge has been overwhelmingly used in scientific literature as the evidence of the oxygen redox states, that is, oxidized oxygen during charging, in battery electrodes based on its variation in either the intensity or the lineshape. [ 6–24 ]…”

Section: Introductionmentioning

confidence: 99%

Deciphering the Oxygen Absorption Pre‐edge: A Caveat on its Application for Probing Oxygen Redox Reactions in Batteries

Roychoudhury

Qiao

Zhuo

et al. 2020

Energy & Environ Materials

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“…To build the next generation LIBs with higher performances, high energy density materials are urgently pursued worldwide . Lithium‐rich (Li‐rich) materials, with the specific capacity over 260 mAh g −1 and energy density up to ≈1000 Wh kg −1 , have attracted great interest in the past decades. It is reported that Li‐rich materials are composed of two phases of Li 2 MnO 3 ( C 2/m ) and LiMO 2 (

R \bar{3} m

) (M = Ni, Co, Mn, etc.)…”

Section: Introductionmentioning

confidence: 99%

Local Electric‐Field‐Driven Fast Li Diffusion Kinetics at the Piezoelectric LiTaO₃ Modified Li‐Rich Cathode–Electrolyte Interphase

et al. 2019

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HEVs (PHEVs), besides the traditional applications in portable devices. To build the next generation LIBs with higher performances, high energy density materials are urgently pursued worldwide. [1][2][3] Lithium-rich (Li-rich) materials, with the specific capacity over 260 mAh g −1 and energy density up to ≈1000 Wh kg −1 , [4] have attracted great interest in the past decades. It is reported that Li-rich materials are composed of two phases of Li 2 MnO 3 (C 2/m ) and LiMO 2 (R m 3 ) (M = Ni, Co, Mn, etc.). [5][6][7][8][9] Despite the above advantages, several concerns including structural instability and the resulted voltage degradation, as well as the poor diffusion kinetics at the interface have become the bottlenecks of Li-rich materials. [9][10][11][12][13] In this regard, multifarious modification approaches, such as doping and surface coating, have been intensively investigated. [14][15][16] Particularly, Li + diffusion at the cathode-electrolyte interphase (CEI) is widely regarded as the rate determining step in LIBs. [17][18][19] From this viewpoint, metal fluorides (FeF 3 , [20] MOF, [21,22] AlF 3 , [23,24] etc.), metal oxides (MgO, [25] Al 2 O 3 , [26,27] etc.), metal phosphates (AlPO 4 , [28] LaPO 4 , [29] Li 3 PO 4 , [30] FePO 4 /Li 3 PO 4 , [31] Li-Mn-PO 4 , [32] etc.), and those with similar structure of Li-rich Li 2 MnO 3 (Li 2 SiO 3 [33,34] and Li 2 SnO 3 , [35] ) have been widely applied to modify the surface of bulk Li-rich materials. Recently, fast lithium-ion conductors (LiVO 3 , [36] Li 2 ZrO 3 , [37] Li-La-Ti-O, [38,39] LiPON, [40] etc.) have also been proposed to decorate the surface of Li-rich cathodes to enhance the apparent diffusion coefficients. All the aforesaid surface modification materials, unexceptionally, have been proved to be effective in both stabilizing the structure and facilitating the Li + kinetics. Nevertheless, in general, the decoration layers themselves seem rather "passive" in promoting Li + diffusion. Assuming they are Li + conductive (e.g., solid electrolyte materials), fast Li + diffusion channels will be provided besides the general separation effect (in suppressing side reactions and inevitable TM dissolution). As for Li + insulators (e.g., metal fluorides), only the benefit of physical barriers could be exploited. Therefore, a more "initiative" function interface is imperative to be built to more effectively promote the Li + transport at the electrode-electrolyte interphase.It is noteworthy that piezoelectric material, as an important category in the energy-conversion community, works on the As one of the most promising cathodes for next-generation lithium ion batteries (LIBs), Li-rich materials have been extensively investigated for their high energy densities. However, the practical application of Li-rich cathodes is extremely retarded by the sluggish electrode-electrolyte interface kinetics and structure instability. In this context, piezoelectric LiTaO 3 is employed to functionalize the surface of Li 1.2 Ni 0.17 Mn 0.56 Co 0.07 O 2 (LNMCO), aiming to boost t...

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Lithium‐Ion Batteries: Tuning Anionic Redox Activity and Reversibility for a High‐Capacity Li‐Rich Mn‐Based Oxide Cathode via an Integrated Strategy (Adv. Funct. Mater. 10/2019)

Cited by 29 publications

References 0 publications

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Deciphering the Oxygen Absorption Pre‐edge: A Caveat on its Application for Probing Oxygen Redox Reactions in Batteries

Local Electric‐Field‐Driven Fast Li Diffusion Kinetics at the Piezoelectric LiTaO₃ Modified Li‐Rich Cathode–Electrolyte Interphase

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Lithium‐Ion Batteries: Tuning Anionic Redox Activity and Reversibility for a High‐Capacity Li‐Rich Mn‐Based Oxide Cathode via an Integrated Strategy (Adv. Funct. Mater. 10/2019)

Cited by 29 publications

References 0 publications

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Deciphering the Oxygen Absorption Pre‐edge: A Caveat on its Application for Probing Oxygen Redox Reactions in Batteries

Local Electric‐Field‐Driven Fast Li Diffusion Kinetics at the Piezoelectric LiTaO3 Modified Li‐Rich Cathode–Electrolyte Interphase

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Local Electric‐Field‐Driven Fast Li Diffusion Kinetics at the Piezoelectric LiTaO₃ Modified Li‐Rich Cathode–Electrolyte Interphase