Capacity Fading Mechanisms in Ni-Rich Single-Crystal NCM Cathodes

Hoon Hee Ryu; Been Namkoong; Jae Hyung Kim; Ilias Belharouak; Chong S. Yoon; Yang Kook Sun

doi:10.1021/acsenergylett.1c01089

Capacity Fading Mechanisms in Ni-Rich Single-Crystal NCM Cathodes

Hoon Hee Ryu, Been Namkoong, Jae Hyung Kim, Ilias Belharouak, Chong S. Yoon, Yang Kook Sun

Electrification and Energy Infrastructur

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320 Scopus citations

Abstract

A series of single-crystal, Ni-rich Li[NixCoyMn1-x-y]O2 (NCM) cathodes (x = 0.7, 0.8, and 0.9) with particle diameters of ∼3 μm are systematically compared with polycrystalline cathodes with corresponding Ni contents. Despite their high resistance to microcracking, the electrochemical performances of single-crystal NCM cathodes, in terms of capacity and cycling stability, are inferior to those of polycrystalline NCM cathodes. In situ XRD and TEM analyses reveal that the lithium concentrations in single-crystal NCM cathodes become spatially inhomogeneous during cycling; this phenomenon is exacerbated by high C rates and Ni contents, resulting in the coexistence of phases with widely different unit cell dimensions within a single cathode particle. This coexistence of two phases induces nonuniform stress that generates structural defects, impairing the diffusion of lithium ions and, eventually, leading to rapid capacity fading.

Original language	English
Pages (from-to)	2726-2734
Number of pages	9
Journal	ACS Energy Letters
Volume	6
Issue number	8
DOIs	https://doi.org/10.1021/acsenergylett.1c01089
State	Published - Aug 13 2021

Funding

This work was mainly supported by a Human Resources Development programme (No. 20184010201720) of a Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant, funded by the Ministry of Trade, Industry and Energy of the Korean government. This work was also supported by National Research Foundation of Korea (NRF) grant funded by the Korea government Ministry of Education and Science Technology (MEST) (NRF-2018R1A2B3008794).

Funders	Funder number
NRF-2018R1A2B3008794
Ministry of Trade, Industry and Energy
National Research Foundation of Korea
Ministry of Education, Science and Technology
Korea Institute of Energy Technology Evaluation and Planning

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title = "Capacity Fading Mechanisms in Ni-Rich Single-Crystal NCM Cathodes",

abstract = "A series of single-crystal, Ni-rich Li[NixCoyMn1-x-y]O2 (NCM) cathodes (x = 0.7, 0.8, and 0.9) with particle diameters of ∼3 μm are systematically compared with polycrystalline cathodes with corresponding Ni contents. Despite their high resistance to microcracking, the electrochemical performances of single-crystal NCM cathodes, in terms of capacity and cycling stability, are inferior to those of polycrystalline NCM cathodes. In situ XRD and TEM analyses reveal that the lithium concentrations in single-crystal NCM cathodes become spatially inhomogeneous during cycling; this phenomenon is exacerbated by high C rates and Ni contents, resulting in the coexistence of phases with widely different unit cell dimensions within a single cathode particle. This coexistence of two phases induces nonuniform stress that generates structural defects, impairing the diffusion of lithium ions and, eventually, leading to rapid capacity fading.",

author = "Ryu, {Hoon Hee} and Been Namkoong and Kim, {Jae Hyung} and Ilias Belharouak and Yoon, {Chong S.} and Sun, {Yang Kook}",

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T1 - Capacity Fading Mechanisms in Ni-Rich Single-Crystal NCM Cathodes

AU - Ryu, Hoon Hee

AU - Namkoong, Been

AU - Kim, Jae Hyung

AU - Belharouak, Ilias

AU - Yoon, Chong S.

AU - Sun, Yang Kook

PY - 2021/8/13

Y1 - 2021/8/13

N2 - A series of single-crystal, Ni-rich Li[NixCoyMn1-x-y]O2 (NCM) cathodes (x = 0.7, 0.8, and 0.9) with particle diameters of ∼3 μm are systematically compared with polycrystalline cathodes with corresponding Ni contents. Despite their high resistance to microcracking, the electrochemical performances of single-crystal NCM cathodes, in terms of capacity and cycling stability, are inferior to those of polycrystalline NCM cathodes. In situ XRD and TEM analyses reveal that the lithium concentrations in single-crystal NCM cathodes become spatially inhomogeneous during cycling; this phenomenon is exacerbated by high C rates and Ni contents, resulting in the coexistence of phases with widely different unit cell dimensions within a single cathode particle. This coexistence of two phases induces nonuniform stress that generates structural defects, impairing the diffusion of lithium ions and, eventually, leading to rapid capacity fading.

AB - A series of single-crystal, Ni-rich Li[NixCoyMn1-x-y]O2 (NCM) cathodes (x = 0.7, 0.8, and 0.9) with particle diameters of ∼3 μm are systematically compared with polycrystalline cathodes with corresponding Ni contents. Despite their high resistance to microcracking, the electrochemical performances of single-crystal NCM cathodes, in terms of capacity and cycling stability, are inferior to those of polycrystalline NCM cathodes. In situ XRD and TEM analyses reveal that the lithium concentrations in single-crystal NCM cathodes become spatially inhomogeneous during cycling; this phenomenon is exacerbated by high C rates and Ni contents, resulting in the coexistence of phases with widely different unit cell dimensions within a single cathode particle. This coexistence of two phases induces nonuniform stress that generates structural defects, impairing the diffusion of lithium ions and, eventually, leading to rapid capacity fading.

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SP - 2726

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JO - ACS Energy Letters

JF - ACS Energy Letters

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ER -

Capacity Fading Mechanisms in Ni-Rich Single-Crystal NCM Cathodes

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