First-principles prediction of extraordinary thermoelectric efficiency in superionic Li2SnX3(X=S,Se)

TL;DR

This study uses first-principles calculations to predict exceptionally high thermoelectric efficiency in Li2SnX3 compounds, highlighting their potential as high-performance thermoelectric materials due to favorable electronic and thermal properties.

Contribution

The paper demonstrates that Li2SnX3 compounds exhibit high zT values, combining high Seebeck coefficients, electrical conductivity, and low thermal conductivity, revealing their potential as efficient thermoelectrics.

Findings

Maximum zT of 1.05 in p-type Li2SnS3 at 700K

Maximum zT of 3.07 in n-type Li2SnSe3 at 700K

High power factors and low thermal conductivity in Li2SnX3

Abstract

Thermoelectric materials create an electric potential when subject to a temperature gradient and vice versa hence they can be used to harvest waste heat into electricity and in thermal management applications. However, finding highly efficient thermoelectrics with high figures of merit, zT$\geq$1, is very challenging because the combination of high power factor and low thermal conductivity is rare in materials. Here, we use first-principles methods to analyze the thermoelectric properties of Li$_2$Sn$X_3$ ($X$=S,Se), a recently synthesized class of lithium fast-ion conductors presenting high thermal stability. In p-type Li$_2$Sn$X_3$, we estimate highly flat electronic valence bands that render high Seebeck coefficients exceeding 400 ${\mu}$VK$^{-1}$ at 700K. In n-type Li$_2$Sn$X_3$, the electronic conduction bands are slightly dispersive however the accompanying weak electron-acoustic phonon scattering induces high electrical conductivity. The combination of high Seebeck coefficient and electrical conductivity gives rise to high power factors, reaching a maximum of 4 mWm$^{-1}$K$^{-2}$ in p-type Li$_2$SnS$_3$ and 8 mWm$^{-1}$K$^{-2}$ in n-type Li$_2$SnSe$_3$ at 300 K. Likewise, the thermal conductivity in Li$_2$Sn$X_3$ is low as compared to conventional thermoelectric materials, 2-5 Wm$^{-1}$K$^{-1}$ at room temperature. As a result, we estimate a maximum zT = 1.05 in p-type Li$_2$SnS$_3$ at 700 K and an extraordinary 3.07 (1.5) in n-type Li$_2$SnSe$_3$ at the same temperature (300 K). Our findings of huge zT in Li$_2$Sn$X_3$ suggest that lithium fast-ion conductors, typically employed as electrolytes in solid-state batteries, hold exceptional promise as thermoelectric materials.