Thermoelectric properties of high-entropy wolframite oxide: (CoCuNiFeZn)$_{1-x}$Ga$_x$WO$_4$

TL;DR

This study synthesizes high-entropy wolframite oxides with varying Ga content, revealing their structural, optical, and thermoelectric properties, notably low thermal conductivity and improved thermoelectric efficiency.

Contribution

It introduces a novel high-entropy wolframite oxide synthesis method and characterizes its enhanced thermoelectric performance due to lattice disorder.

Findings

Monoclinic structure confirmed by XRD

Thermal conductivity significantly lower than MgWO4

zT increases with Ga doping

Abstract

In this report, the synthesis of high-entropy wolframite oxide (CoCuNiFeZn)$_{1-x}$Ga$_x$WO$_4$ through standard solid-state route followed by spark plasma sintering (SPS) and their structural, microstructural, and thermoelectric properties are investigated. X-ray diffraction pattern followed by pattern matching refinement shows monoclinic structure with volume of the unit cell decreasing with increasing Ga content. The optical band gap for these oxides shows a cocktail effect in high entropy configuration. The Seebeck coefficient indicates electrons as dominating charge carriers with a non-degenerate behavior. The electrical resistivity decreases with increasing temperature depicting a semiconducting nature. Thermal conductivity in high-entropy samples ($\kappa\sim$2.1 W/mK @ 300\,K) is significantly lower as compared to MgWO$_4$ ($\kappa\sim$11.5 W/mK @ 300\,K), which can be explained by the strong phonon scattering due to large lattice disorder in high entropy configuration. The thermoelectric figure of merit zT increases with Ga doping via modifying all three thermoelectric parameters positively.