Ductile P‐Type AgCu(Se,S,Te) Thermoelectric Materials

Abstract Ductile inorganic thermoelectric (TE) materials open a new approach to develop high‐performance flexible TE devices. N‐type Ag₂(S,Se,Te) and p‐type AgCu(Se,S,Te) pseudoternary solid solutions are two typical categories of ductile inorganic TE materials reported so far. Comparing with the Ag₂(S,Se,Te) pseudoternary solid solutions, the phase composition, crystal structure, and physical properties of AgCu(Se,S,Te) pseudoternary solid solutions are more complex, but their relationships are still ambiguous now. In this work, via systematically investigating the phase composition, crystal structure, mechanical, and TE properties of about 60 AgCu(Se,S,Te) pseudoternary solid solutions, the comprehensive composition–structure–property phase diagrams of the AgCuSe‐AgCuS‐AgCuTe pseudoternary system is constructed. By mapping the complex phases, the “ductile‐brittle” and “n‐p” transition boundaries are determined and the composition ranges with high TE performance and inherent ductility are illustrated. On this basis, high performance p‐type ductile TE materials are obtained, with a maximum zT of 0.81 at 340 K. Finally, flexible in‐plane TE devices are prepared by using the AgCu(Se,S,Te)‐based ductile TE materials, showing high output performance that is superior to those of organic and inorganic–organic hybrid flexible devices.