Structure solution of metal-oxide Li battery cathodes from simulated annealing and lithium NMR spectroscopy

Kristopher J. Harris; Jamie Foster; Matteo Z. Tessaro; Meng Jiang; Xingyi Yang; Yan Wu; Bartosz Protas; Gillian R. Goward

doi:10.1021/acs.chemmater.7b00836

Structure solution of metal-oxide Li battery cathodes from simulated annealing and lithium NMR spectroscopy

Kristopher J. Harris
, Jamie Foster
, Matteo Z. Tessaro
, Meng Jiang
, Xingyi Yang
, Yan Wu
, Bartosz Protas
, Gillian R. Goward

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

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Abstract

Discerning the arrangement of transition metal atoms in Li[Ni_xMn_yCo_zO₂] cathode materials has remained an open problem for many years despite the commercial importance of some stoichiometries and the even more promising characteristics of others. We present a method for structural determination in this class of cathode materials. A simple definition of the total energy, based on the chemical principle of electroneutrality, is used in combination with a simulated annealing algorithm to generate model structures. The method reproduces the well known structure of Li[Li_1/3Mn_2/3O₂] and produces structures of the disordered Li[Ni_xMn_xCo_1-2_xO₂] phases (where x = 0.02, 0.1, 0.33) that are verified by detailed ⁷Li NMR spectra. For each Li[Ni_xMn_xCo_1-2_xO₂]
phase, the solution is found to be heavily disordered, yet retaining significant ion pairing. Since the underlying notion of favoring charge-neutral regions is generic, we anticipate its utility in a much broader family of materials.

Original language	English
Journal	Chemistry of Materials
Early online date	5 Jun 2017
DOIs	https://doi.org/10.1021/acs.chemmater.7b00836
Publication status	Early online - 5 Jun 2017

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This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see: http://pubs.acs.org/doi/abs/10.1021/acs.chemmater.7b00836
Accepted author manuscript (Post-print), 4.55 MB

Cite this

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title = "Structure solution of metal-oxide Li battery cathodes from simulated annealing and lithium NMR spectroscopy",

abstract = "Discerning the arrangement of transition metal atoms in Li[NixMnyCozO2] cathode materials has remained an open problem for many years despite the commercial importance of some stoichiometries and the even more promising characteristics of others. We present a method for structural determination in this class of cathode materials. A simple definition of the total energy, based on the chemical principle of electroneutrality, is used in combination with a simulated annealing algorithm to generate model structures. The method reproduces the well known structure of Li[Li1/3Mn2/3O2] and produces structures of the disordered Li[NixMnxCo1-2xO2] phases (where x = 0.02, 0.1, 0.33) that are verified by detailed 7Li NMR spectra. For each Li[NixMnxCo1-2xO2] phase, the solution is found to be heavily disordered, yet retaining significant ion pairing. Since the underlying notion of favoring charge-neutral regions is generic, we anticipate its utility in a much broader family of materials.",

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year = "2017",

month = jun,

day = "5",

doi = "10.1021/acs.chemmater.7b00836",

language = "English",

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T1 - Structure solution of metal-oxide Li battery cathodes from simulated annealing and lithium NMR spectroscopy

AU - Harris, Kristopher J.

AU - Foster, Jamie

AU - Tessaro, Matteo Z.

AU - Jiang, Meng

AU - Yang, Xingyi

AU - Wu, Yan

AU - Protas, Bartosz

AU - Goward, Gillian R.

PY - 2017/6/5

Y1 - 2017/6/5

N2 - Discerning the arrangement of transition metal atoms in Li[NixMnyCozO2] cathode materials has remained an open problem for many years despite the commercial importance of some stoichiometries and the even more promising characteristics of others. We present a method for structural determination in this class of cathode materials. A simple definition of the total energy, based on the chemical principle of electroneutrality, is used in combination with a simulated annealing algorithm to generate model structures. The method reproduces the well known structure of Li[Li1/3Mn2/3O2] and produces structures of the disordered Li[NixMnxCo1-2xO2] phases (where x = 0.02, 0.1, 0.33) that are verified by detailed 7Li NMR spectra. For each Li[NixMnxCo1-2xO2] phase, the solution is found to be heavily disordered, yet retaining significant ion pairing. Since the underlying notion of favoring charge-neutral regions is generic, we anticipate its utility in a much broader family of materials.

AB - Discerning the arrangement of transition metal atoms in Li[NixMnyCozO2] cathode materials has remained an open problem for many years despite the commercial importance of some stoichiometries and the even more promising characteristics of others. We present a method for structural determination in this class of cathode materials. A simple definition of the total energy, based on the chemical principle of electroneutrality, is used in combination with a simulated annealing algorithm to generate model structures. The method reproduces the well known structure of Li[Li1/3Mn2/3O2] and produces structures of the disordered Li[NixMnxCo1-2xO2] phases (where x = 0.02, 0.1, 0.33) that are verified by detailed 7Li NMR spectra. For each Li[NixMnxCo1-2xO2] phase, the solution is found to be heavily disordered, yet retaining significant ion pairing. Since the underlying notion of favoring charge-neutral regions is generic, we anticipate its utility in a much broader family of materials.

U2 - 10.1021/acs.chemmater.7b00836

DO - 10.1021/acs.chemmater.7b00836

M3 - Article

SN - 0897-4756

JO - Chemistry of Materials

JF - Chemistry of Materials

ER -

Structure solution of metal-oxide Li battery cathodes from simulated annealing and lithium NMR spectroscopy

Abstract

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