First-principles investigation of pressure-induced structural, electronic, and thermoelectric properties in CoSb3−xAx compounds (A = Ge, Se, Te)

The enhancement of thermoelectric properties in CoSb3 through atom substitution and hydrostatic pressure application is a promising avenue. Herein, we conducted a comprehensive theoretical investigation into the structural, electronic, and thermoelectric characteristics of CoSb3−xAx (A = Ge, Se, Te; x = 0.125, 0.250) using density functional theory coupled with Boltzmann transport theory. By subjecting the system to pressures ranging from 0 to 20 GPa and substituting Sb atoms, we evaluated the enthalpy of formation to predict stability, with CoSb2.875Te0.125 exhibiting superior stability under 20 GPa. The bandgap of doped compounds is direct, ranging from 0.33 to 0.56 eV along the Γ point, and was calculated to elucidate electronic properties. Additionally, employing the Slack model, we computed lattice thermal conductivity based on elastic constants to provide a comprehensive analysis of thermoelectric efficiency. Remarkably, our study not only highlights the effect of hydrostatic pressure on structural and electronic properties but also reveals a beneficial impact on increasing ZT values to 2.77 for CoSb2.750Ge0.250 at 800 K and 20 GPa, indicating predominantly p-type behavior.