Direct Melt‐Calendaring of Highly Textured (Bi,Sb)₂Te₃ Thick Films: Superior Thermoelectric and Mechanical Performance via Strain Engineering

Abstract

The evolutions of chip thermal management and micro energy harvesting put forward urgent need for micro thermoelectric devices. Nevertheless, low‐performance thermoelectric thick films as well as the complicated precision cutting process for hundred‐micron thermoelectric legs still remain the bottleneck hindering the advancement of micro thermoelectric devices. In this work, an innovative direct melt‐calendaring manufacturing technology is first proposed with specially designed and assembled equipment, that enables direct, rapid, and cost‐effective continuous manufacturing of Bi2Te3‐based films with thickness of hundred microns. Based on the strain engineering with external glass coating confinement and controlled calendaring deformation degree, enhanced thermoelectric performance has been achieved for (Bi,Sb)2Te3 thick films with highly textured nanocrystals, which can promote carrier mobility over 182.6 cm2 V−1 s−1 and bring out a record‐high zT value of 0.96 and 1.16 for n‐type and p‐type (Bi,Sb)2Te3 thick films, respectively. The nanoscale interfaces also further improve the mechanical strength with excellent elastic modules (over 42.0 GPa) and hardness (over 1.7 GPa), even superior to the commercial zone‐melting ingots and comparable to the hot‐extrusion (Bi,Sb)2Te3 alloys. This new fabrication strategy is versatile to a wide range of inorganic thermoelectric thick films, which lays a solid foundation for the development of micro thermoelectric devices.