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

School of Mathematics & Physics

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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.",

author = "Harris, {Kristopher J.} and Jamie Foster and Tessaro, {Matteo Z.} and Meng Jiang and Xingyi Yang and Yan Wu and Bartosz Protas and Goward, {Gillian R.}",

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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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