Realizing High Thermoelectric Performance of Bi-Sb-Te-Based Printed Films through Grain Interface Modification by an In Situ-Grown β-Cu2-δSe Phase

It has been a substantial challenge to develop a printed thermoelectric (TE) material with a figure-of-merit ZT > 1. In this work, high ZT p-type Bi0.5Sb1.5Te3-based printable TE materials have been advanced by interface modification of the TE grains with a nonstoichiometric β-Cu2-δSe-based inorganic binder (IB) through a facile printing–sintering process. As a result, a very high TE power factor of ∼17.5 μW cm–1 K–2 for a p-type printed material is attained in the optimized compounds at room temperature (RT). In addition, a high ZT of ∼1.2 at RT and of ∼1.55 at 360 K is realized using thermal conductivity (κ) of a pellet made of the prepared printable material containing 10 wt % of IB. Using the same material for p-type TE legs and silver paste for n-type TE legs, a printed TE generator (print-TEG) of four thermocouples has been fabricated for demonstration. An open-circuit voltage (VOC) of 14 mV and a maximum power output (Pmax) of 1.7 μW are achieved for ΔT = 40 K for the print-TEG.