Electrochemical Properties of Three Li2Ni2TeO6 Structural Polymorphs

Nicholas S. Grundish; Ieuan D. Seymour; Graeme Henkelman; John B. Goodenough

doi:10.1021/acs.chemmater.9b02956

Electrochemical Properties of Three Li₂Ni₂TeO₆ Structural Polymorphs

Nicholas S. Grundish^* (Corresponding Author), Ieuan D. Seymour, Graeme Henkelman, John B. Goodenough^* (Corresponding Author)

^*Corresponding author for this work

Chemistry

University of Texas at Austin

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

29 Citations (Scopus)

Abstract

Three different structures of the composition Li₂Ni₂TeO₆ have been synthesized and their electrochemical properties characterized: a disordered orthorhombic phase with tellurium ordering and strong Li/Ni cation mixing, a T^#2-layered phase, and an O3-layered phase; each have a distinct cycling performance. The disordered orthorhombic structure is the most stable at room temperature and has the highest capacity with the lowest overpotential. The T^#2 phase is the least stable and undergoes a phase transformation once lithium is extracted. Density functional theory calculations reconcile the relative structural stabilities and physical properties of each phase with their electrochemical performances. Calculations also confirmed experimental observations regarding the synthesis of each structure and indicated the mechanism for capacity fade of each Li₂Ni₂TeO₆ cathode. Strong tellurium-oxygen covalent bonding increases the voltage of the Ni^2+/3+ redox couple in each of these materials over what is normally observed in layered oxides.

Original language	English
Pages (from-to)	9379-9388
Number of pages	10
Journal	Chemistry of Materials
Volume	31
Issue number	22
Early online date	7 Oct 2019
DOIs	https://doi.org/10.1021/acs.chemmater.9b02956
Publication status	Published - 26 Nov 2019

Bibliographical note

Funding Information:
G.H. and J.B.G. would like to acknowledge the support of the Robert A. Welch Foundation, Houston, Texas (Grant Nos. F-1066 and F-1841). N.S.G. would like to acknowledge financial support by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0005397. Computational resources were provided by the Texas Advanced Computing Center and the National Energy Research Scientific Computing Center. The authors would like to acknowledge the X-ray diffraction facilities within the Texas Materials Institute.

Publisher Copyright:
Copyright © 2019 American Chemical Society.

Data Availability Statement

No data availability statement

Keywords

Chemical structure
Energy
Layers
Lithium
Phase Transitions

Access to Document

10.1021/acs.chemmater.9b02956

Cite this

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title = "Electrochemical Properties of Three Li2Ni2TeO6 Structural Polymorphs",

abstract = "Three different structures of the composition Li2Ni2TeO6 have been synthesized and their electrochemical properties characterized: a disordered orthorhombic phase with tellurium ordering and strong Li/Ni cation mixing, a T#2-layered phase, and an O3-layered phase; each have a distinct cycling performance. The disordered orthorhombic structure is the most stable at room temperature and has the highest capacity with the lowest overpotential. The T#2 phase is the least stable and undergoes a phase transformation once lithium is extracted. Density functional theory calculations reconcile the relative structural stabilities and physical properties of each phase with their electrochemical performances. Calculations also confirmed experimental observations regarding the synthesis of each structure and indicated the mechanism for capacity fade of each Li2Ni2TeO6 cathode. Strong tellurium-oxygen covalent bonding increases the voltage of the Ni2+/3+ redox couple in each of these materials over what is normally observed in layered oxides.",

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author = "Grundish, {Nicholas S.} and Seymour, {Ieuan D.} and Graeme Henkelman and Goodenough, {John B.}",

note = "Funding Information: G.H. and J.B.G. would like to acknowledge the support of the Robert A. Welch Foundation, Houston, Texas (Grant Nos. F-1066 and F-1841). N.S.G. would like to acknowledge financial support by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0005397. Computational resources were provided by the Texas Advanced Computing Center and the National Energy Research Scientific Computing Center. The authors would like to acknowledge the X-ray diffraction facilities within the Texas Materials Institute. Publisher Copyright: Copyright {\textcopyright} 2019 American Chemical Society.",

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N2 - Three different structures of the composition Li2Ni2TeO6 have been synthesized and their electrochemical properties characterized: a disordered orthorhombic phase with tellurium ordering and strong Li/Ni cation mixing, a T#2-layered phase, and an O3-layered phase; each have a distinct cycling performance. The disordered orthorhombic structure is the most stable at room temperature and has the highest capacity with the lowest overpotential. The T#2 phase is the least stable and undergoes a phase transformation once lithium is extracted. Density functional theory calculations reconcile the relative structural stabilities and physical properties of each phase with their electrochemical performances. Calculations also confirmed experimental observations regarding the synthesis of each structure and indicated the mechanism for capacity fade of each Li2Ni2TeO6 cathode. Strong tellurium-oxygen covalent bonding increases the voltage of the Ni2+/3+ redox couple in each of these materials over what is normally observed in layered oxides.

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