Strain Stabilization of Superionicity in Copper and Lithium Selenides

Daniel Dumett Torres, Prashant Jain

Research output: Contribution to journalArticle

Abstract

Superionic (SI) phases have utility as solid electrolytes for next generation battery technology, but these phases are typically not stable at room temperature. Our density functional theory calculations demonstrate that compressive lattice strain can stabilize SI phases of Cu2Se and Li2Se, two potential solid electrolytes. Electronic and bonding insights into this effect are obtained. In the ordered, non-SI phase, cations are localized primarily in tetrahedral (T) interstices with little access to the higher-energy octahedral (O) sites, but 1-2% compressive strain promotes attractive stabilization of the O cations with 6-fold coordination to Se anions, at the expense of the stability of 4-fold-coordinated T cations. In such compressed lattices, cations can access both T and O sites, resulting in a cation-disordered, SI phase. Thus, lattice strain is demonstrated as a handle for controlling ionic structure and transport and accomplishing ambient temperature superionicity.

Original languageEnglish (US)
Pages (from-to)1200-1205
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume9
Issue number6
DOIs
StatePublished - Mar 15 2018

Fingerprint

copper selenides
selenides
Lithium
Cations
Copper
Stabilization
lithium
stabilization
Positive ions
cations
Solid electrolytes
solid electrolytes
interstices
ambient temperature
Density functional theory
Anions
electric batteries
Negative ions
density functional theory
anions

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

Strain Stabilization of Superionicity in Copper and Lithium Selenides. / Dumett Torres, Daniel; Jain, Prashant.

In: Journal of Physical Chemistry Letters, Vol. 9, No. 6, 15.03.2018, p. 1200-1205.

Research output: Contribution to journalArticle

@article{3ba9ca77904847828f06d1f53afa0231,
title = "Strain Stabilization of Superionicity in Copper and Lithium Selenides",
abstract = "Superionic (SI) phases have utility as solid electrolytes for next generation battery technology, but these phases are typically not stable at room temperature. Our density functional theory calculations demonstrate that compressive lattice strain can stabilize SI phases of Cu2Se and Li2Se, two potential solid electrolytes. Electronic and bonding insights into this effect are obtained. In the ordered, non-SI phase, cations are localized primarily in tetrahedral (T) interstices with little access to the higher-energy octahedral (O) sites, but 1-2{\%} compressive strain promotes attractive stabilization of the O cations with 6-fold coordination to Se anions, at the expense of the stability of 4-fold-coordinated T cations. In such compressed lattices, cations can access both T and O sites, resulting in a cation-disordered, SI phase. Thus, lattice strain is demonstrated as a handle for controlling ionic structure and transport and accomplishing ambient temperature superionicity.",
author = "{Dumett Torres}, Daniel and Prashant Jain",
year = "2018",
month = "3",
day = "15",
doi = "10.1021/acs.jpclett.8b00236",
language = "English (US)",
volume = "9",
pages = "1200--1205",
journal = "Journal of Physical Chemistry Letters",
issn = "1948-7185",
publisher = "American Chemical Society",
number = "6",

}

TY - JOUR

T1 - Strain Stabilization of Superionicity in Copper and Lithium Selenides

AU - Dumett Torres, Daniel

AU - Jain, Prashant

PY - 2018/3/15

Y1 - 2018/3/15

N2 - Superionic (SI) phases have utility as solid electrolytes for next generation battery technology, but these phases are typically not stable at room temperature. Our density functional theory calculations demonstrate that compressive lattice strain can stabilize SI phases of Cu2Se and Li2Se, two potential solid electrolytes. Electronic and bonding insights into this effect are obtained. In the ordered, non-SI phase, cations are localized primarily in tetrahedral (T) interstices with little access to the higher-energy octahedral (O) sites, but 1-2% compressive strain promotes attractive stabilization of the O cations with 6-fold coordination to Se anions, at the expense of the stability of 4-fold-coordinated T cations. In such compressed lattices, cations can access both T and O sites, resulting in a cation-disordered, SI phase. Thus, lattice strain is demonstrated as a handle for controlling ionic structure and transport and accomplishing ambient temperature superionicity.

AB - Superionic (SI) phases have utility as solid electrolytes for next generation battery technology, but these phases are typically not stable at room temperature. Our density functional theory calculations demonstrate that compressive lattice strain can stabilize SI phases of Cu2Se and Li2Se, two potential solid electrolytes. Electronic and bonding insights into this effect are obtained. In the ordered, non-SI phase, cations are localized primarily in tetrahedral (T) interstices with little access to the higher-energy octahedral (O) sites, but 1-2% compressive strain promotes attractive stabilization of the O cations with 6-fold coordination to Se anions, at the expense of the stability of 4-fold-coordinated T cations. In such compressed lattices, cations can access both T and O sites, resulting in a cation-disordered, SI phase. Thus, lattice strain is demonstrated as a handle for controlling ionic structure and transport and accomplishing ambient temperature superionicity.

UR - http://www.scopus.com/inward/record.url?scp=85044008527&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85044008527&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.8b00236

DO - 10.1021/acs.jpclett.8b00236

M3 - Article

AN - SCOPUS:85044008527

VL - 9

SP - 1200

EP - 1205

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

SN - 1948-7185

IS - 6

ER -