High‐Entropy Cubic Pseudo‐Ternary Ag2(S, Se, Te) Materials With Excellent Ductility and Thermoelectric Performance

The discovery of ductile Ag2(S, Se, Te) materials opens a new avenue toward high‐performance flexible/hetero‐shaped thermoelectrics. Specifically, the cubic‐structured materials are quite attractive by combining remarkable plasticity, decent thermoelectric figure of merit (zT), and no phase transition above room temperature. However, such materials are quite few and the understanding is inadequate on their mechanical and thermoelectric properties. Enlightened by the high‐entropy principles, a series of pseudo‐ternary Ag2S‐Ag2Se‐Ag2Te alloys is designed and comprehensive diagrams of composition‐structure‐plasticity‐zT are compiled. Subsequently, the compositional region for the cubic phase is outlined. As a high‐entropy example featuring with anion‐site alloying and disordered Ag ions, Ag2‐xS1/3Se1/3Te1/3 materials exhibit impressively large elongations of 60–97%, ultralow lattice thermal conductivities of ≈0.2 W m−1 K−1, and decent zT values of 0.45 at 300 K, 0.8 at 460 K. The materials can be readily rolled into thin foils, showing excellent flexibility. Finally, a six‐leg in‐plane device is fabricated, achieving an output voltage of 13.6 mV, a maximal power of 12.8 µW, and a power density of 14.3 W m−2 under the temperature difference of 30 K, much higher than the organic counterparts. This study largely enriches the members of cubic ductile inorganic materials for the applications in flexible and hetero‐shaped energy and electronic devices. The authors compile comprehensive diagrams of the composition‐structure‐plasticity‐zT correlation for the Ag2S‐Ag2Se‐Ag2Te system, and subsequently develop a series of high‐entropy cubic‐structured pseudo‐ternary materials. Typically, Ag2‐xS1/3Se1/3Te1/3 materials show remarkably large elongations of 60‐97%, high zT values of 0.45 at room temperature and 0.8 at 460 K. The study enriches ductile inorganic materials for flexible and hetero‐shaped thermoelectrics.