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Atomic Resolution Structural and Chemical Imaging Revealing the Sequential Migration of Ni, Co, and Mn upon the Battery Cycling of Layered Cathode

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TLDR
This work highlights that Ni ions, though acting as the dominant redox species in many LTMO, are labile to migrate to cause lattice disordering upon battery cycling, while the Mn ions are more stable as compared with Ni and Co and can act as pillar to stabilize layered structure.
Abstract
Layered lithium transition metal oxides (LTMO) are promising candidate cathode materials for next-generation high-energy density lithium ion battery. The challenge for using this category of cathode is the capacity and voltage fading, which is believed to be associated with the layered structure disordering, a process that is initiated from the surface or solid-electrolyte interface and facilitated by transition metal (TM) reduction and oxygen vacancy formation. However, the atomic level dynamic mechanism of such a layered structure disordering is still not fully clear. In this work, utilizing atomic resolution electron energy loss spectroscopy (EELS), we map, for the first time at atomic scale, the spatial evolution of Ni, Co and Mn in a cycled LiNi1/3Mn1/3Co1/3O2 layered cathode. In combination with atomic level structural imaging, we discovered the direct correlation of TM ions migration behavior with lattice disordering, featuring the residing of TM ions in the tetrahedral site and a sequential migrat...

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Citations
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Simultaneously Dual Modification of Ni-Rich Layered Oxide Cathode for High-Energy Lithium-Ion Batteries

TL;DR: In this article, a dual-modification strategy of synchronous synthesis and in situ modification of LiNi0.8Co0.1Mn 0.1O2 cathodes was proposed to solve the problem of fast capacity drop and voltage fading due to the interfacial instability and bulk structural degradation of the cathodes during battery operation.
Journal ArticleDOI

Electrode Degradation in Lithium-Ion Batteries.

TL;DR: This Review highlights the developments of electrode materials and characterization tools for rechargeable lithium-ion batteries, with a focus on the structural and electrochemical degradation mechanisms that plague these systems.
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Reviving lithium cobalt oxide-based lithium secondary batteries-toward a higher energy density

TL;DR: This review summarizes the key challenges of synthesizing L CO-based LBs with a higher energy density from the perspectives of structure and interface stability, and gives an account of effective modification strategies in view of the electrodes, liquid electrolytes, binders, separators, solid electrolytes and LCO-based full cells.
References
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Journal ArticleDOI

Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries

TL;DR: It was found that the surface reconstruction exhibits a strong anisotropic characteristic, which predominantly occurs along lithium diffusion channels, and the surface reaction layer is composed of lithium fluoride embedded in a complex organic matrix.
Journal ArticleDOI

Nickel-Rich and Lithium-Rich Layered Oxide Cathodes: Progress and Perspectives

TL;DR: Li-rich layered oxides have attracted much research interest as cathodes for Li-ion batteries due to their low cost and higher discharge capacities compared to those of LiCoO2 and LiMn2O4 as mentioned in this paper.
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Identifying surface structural changes in layered Li-excess nickel manganese oxides in high voltage lithium ion batteries: A joint experimental and theoretical study

TL;DR: In this article, a detailed lithium de-intercalation mechanism was proposed for high voltage high energy density cathode materials, which showed clear evidence of a new spinel-like solid phase formed on the surface of the electrode materials after high-voltage cycling.
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