Resolving Charge Distribution for Compositionally Heterogeneous Battery Cathode Materials

Linqin Mu; Jin Zhang; Yahong Xu; Chenxi Wei; Muhammad Mominur Rahman; Dennis Nordlund; Yijin Liu; Feng Lin

doi:10.1021/acs.nanolett.1c04464

Resolving Charge Distribution for Compositionally Heterogeneous Battery Cathode Materials

Linqin Mu, Jin Zhang, Yahong Xu, Chenxi Wei, Muhammad Mominur Rahman, Dennis Nordlund, Yijin Liu, Feng Lin

Research output: Contribution to journal › Article › peer-review

9 Scopus citations

Abstract

The isostructural nature of Li-layered cathodes allows for accommodating multiple transition metals (TMs). However, little is known about how the local TM stoichiometry influences the charging behavior of battery particles thus impacting battery performance. Here, we develop heterogeneous compositional distributions in polycrystalline LiNi1-x-yMnxCoyO2 (NMC) particles to investigate the interplay between local stoichiometry and charge distribution. These NMC particles exhibit a broad, continuous distribution of local Ni/Mn/Co stoichiometry, which does not compromise the global layeredness. The local Mn and Ni concentrations in individual NMC particles are positively and negatively correlated with the electrochemically induced Ni oxidation, respectively, whereas the Co concentration does not impose a clear effect on the Ni oxidation. The resulting material delivers excellent reversible capacity, rate capability, and cycle life at high operating voltages. Engineering Ni/Mn/Co distribution in NMC particles may provide a path toward controlling the charge distribution and thus chemomechanical properties of polycrystalline battery particles.

Original language	English
Pages (from-to)	1278-1286
Number of pages	9
Journal	Nano Letters
Volume	22
Issue number	3
DOIs	https://doi.org/10.1021/acs.nanolett.1c04464
State	Published - Feb 9 2022
Externally published	Yes

Funding

The work was supported by the Department of Chemistry Startup at Virginia Tech and the National Science Foundation (DMR-1832613). The results presented were obtained in part with the instruments and staff expertise at Virginia Tech’s Nanoscale Characterization and Fabrication Laboratory (NCFL). Use of the Stanford Synchrotron Radiation Light source, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The authors acknowledge the technical support from Dr. Ryan Davis at Beamline 4-1 and Tim Dunn at Beamline 11-3 of SSRL. The authors thank D. Van Campen, V. Borzenets, and Dave Day for their engineering support for experiments at beamline 6-2C of SSRL. The authors thank David Kautz and James Steiner for discussion.

Funders	Funder number
Department of Chemistry Startup at Virginia Tech
National Science Foundation	DMR-1832613
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC02-76SF00515

Keywords

NMC cathode
Polycrystalline
charge distribution
heterogeneity
local stoichiometry

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10.1021/acs.nanolett.1c04464

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abstract = "The isostructural nature of Li-layered cathodes allows for accommodating multiple transition metals (TMs). However, little is known about how the local TM stoichiometry influences the charging behavior of battery particles thus impacting battery performance. Here, we develop heterogeneous compositional distributions in polycrystalline LiNi1-x-yMnxCoyO2 (NMC) particles to investigate the interplay between local stoichiometry and charge distribution. These NMC particles exhibit a broad, continuous distribution of local Ni/Mn/Co stoichiometry, which does not compromise the global layeredness. The local Mn and Ni concentrations in individual NMC particles are positively and negatively correlated with the electrochemically induced Ni oxidation, respectively, whereas the Co concentration does not impose a clear effect on the Ni oxidation. The resulting material delivers excellent reversible capacity, rate capability, and cycle life at high operating voltages. Engineering Ni/Mn/Co distribution in NMC particles may provide a path toward controlling the charge distribution and thus chemomechanical properties of polycrystalline battery particles.",

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AU - Nordlund, Dennis

AU - Liu, Yijin

AU - Lin, Feng

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N2 - The isostructural nature of Li-layered cathodes allows for accommodating multiple transition metals (TMs). However, little is known about how the local TM stoichiometry influences the charging behavior of battery particles thus impacting battery performance. Here, we develop heterogeneous compositional distributions in polycrystalline LiNi1-x-yMnxCoyO2 (NMC) particles to investigate the interplay between local stoichiometry and charge distribution. These NMC particles exhibit a broad, continuous distribution of local Ni/Mn/Co stoichiometry, which does not compromise the global layeredness. The local Mn and Ni concentrations in individual NMC particles are positively and negatively correlated with the electrochemically induced Ni oxidation, respectively, whereas the Co concentration does not impose a clear effect on the Ni oxidation. The resulting material delivers excellent reversible capacity, rate capability, and cycle life at high operating voltages. Engineering Ni/Mn/Co distribution in NMC particles may provide a path toward controlling the charge distribution and thus chemomechanical properties of polycrystalline battery particles.

AB - The isostructural nature of Li-layered cathodes allows for accommodating multiple transition metals (TMs). However, little is known about how the local TM stoichiometry influences the charging behavior of battery particles thus impacting battery performance. Here, we develop heterogeneous compositional distributions in polycrystalline LiNi1-x-yMnxCoyO2 (NMC) particles to investigate the interplay between local stoichiometry and charge distribution. These NMC particles exhibit a broad, continuous distribution of local Ni/Mn/Co stoichiometry, which does not compromise the global layeredness. The local Mn and Ni concentrations in individual NMC particles are positively and negatively correlated with the electrochemically induced Ni oxidation, respectively, whereas the Co concentration does not impose a clear effect on the Ni oxidation. The resulting material delivers excellent reversible capacity, rate capability, and cycle life at high operating voltages. Engineering Ni/Mn/Co distribution in NMC particles may provide a path toward controlling the charge distribution and thus chemomechanical properties of polycrystalline battery particles.

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Resolving Charge Distribution for Compositionally Heterogeneous Battery Cathode Materials

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Keywords

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