Evidence for a Solid-Electrolyte Inductive Effect in the Superionic Conductor Li10Ge1–xSnxP2S12

Culver, Sean P.; Squires, Alexander G.; Minafra, Nicolò; Armstrong, Callum W. F.; Krauskopf, Thorben; Böcher, Felix; Li, Cheng; Morgan, Benjamin J.; Zeier, Wolfgang G.

doi:10.1021/jacs.0c10735

Title: Evidence for a Solid-Electrolyte Inductive Effect in the Superionic Conductor Li₁₀Ge_1–xSn_xP₂S₁₂

Journal Article · Mon Dec 07 00:00:00 EST 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c10735· OSTI ID:1816470

Culver, Sean P. ^[1]; Squires, Alexander G. ^[2]; Minafra, Nicolò ^[3]; Armstrong, Callum W. F. ^[4]; Krauskopf, Thorben ^[1]; Böcher, Felix ^[1];

^[5]; Morgan, Benjamin J. ^[2];

^[3]

Justus-Liebig-Univ. Giessen (Germany)
Univ. of Bath (United Kingdom); The Faraday Institution, Didcot (United Kingdom)
Univ. of Münster (Germany)
Univ. of Bath (United Kingdom)
Forschungszentrum Jülich GmbH, Oak Ridge, TN (United States)

Strategies to enhance ionic conductivities in solid electrolytes typically focus on the effects of modifying their crystal structures or of tuning mobile-ion stoichiometries. A less-explored approach is to modulate the chemical bonding interactions within a material to promote fast lithium-ion diffusion. Recently, the idea of a solid-electrolyte inductive effect has been proposed, whereby changes in bonding within the solid-electrolyte host framework modify the potential energy landscape for the mobile ions, resulting in an enhanced ionic conductivity. Direct evidence for a solid-electrolyte inductive effect, however, is lacking—in part because of the challenge of quantifying changes in local bonding interactions within a solid-electrolyte host framework. Here, we consider the evidence for a solid-electrolyte inductive effect in the archetypal superionic lithium-ion conductor Li₁₀Ge_1–xSn_xP₂S₁₂. Substituting Ge for Sn weakens the {Ge,Sn}–S bonding interactions and increases the charge density associated with the S^2– ions. This charge redistribution modifies the Li⁺ substructure causing Li⁺ ions to bind more strongly to the host framework S^2– anions, which in turn modulates the Li⁺ ion potential energy surface, increasing local barriers for Li⁺ ion diffusion. Each of these effects is consistent with the predictions of the solid-electrolyte inductive effect model. Density functional theory calculations predict that this inductive effect occurs even in the absence of changes to the host framework geometry due to Ge → Sn substitution. These results provide direct evidence in support of a measurable solid–electrolyte inductive effect and demonstrate its application as a practical strategy for tuning ionic conductivities in superionic lithium-ion conductors.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1816470

Journal Information:: Journal of the American Chemical Society, Vol. 142, Issue 50; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Diffusion
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Lithium
Potential energy
Solid electrolytes

Title: Evidence for a Solid-Electrolyte Inductive Effect in the Superionic Conductor Li10Ge1–xSnxP2S12

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Title: Evidence for a Solid-Electrolyte Inductive Effect in the Superionic Conductor Li₁₀Ge_1–xSn_xP₂S₁₂