High Performance Thermoelectric Power of Bi0.5Sb1.5Te3 Through Synergistic Cu2GeSe3 and Se Incorporations

Abstract

Bi₂Te₃-based alloys are the benchmark for commercial thermoelectric (TE) materials, the widespread demand for low-grade waste heat recovery and solid-state refrigeration makes it imperative to enhance the figure-of-merits. In this study, high-performance Bi_0.5Sb_1.5Te₃ (BST) is realized by incorporating Cu₂GeSe₃ and Se. Concretely, the diffusion of Cu and Ge atoms optimizes the hole concentration and raises the density-of-states effective mass (m_d ^*), compensating for the loss of "donor-like effect" exacerbated by ball milling. The subsequent Se addition further increases m_d ^*, enabling a total 28% improvement of room-temperature power factor (S²σ), reaching 43.6 µW cm^-1 K^-2 compared to the matrix. Simultaneously, the lattice thermal conductivity is also significantly suppressed by multiscale scattering sources represented by Cu-rich nanoparticles and dislocation arrays. The synergistic effects yield a peak ZT of 1.41 at 350 K and an average ZT of 1.23 (300-500 K) in the Bi_0.5Sb_1.5Te_2.94Se_0.06 + 0.11 wt.% Cu₂GeSe₃ sample. More importantly, the integrated 17-pair TE module achieves a conversion efficiency of 6.4%, 80% higher than the commercial one at ΔT = 200 K. These results validate that the facile composition optimization of the BST/Cu₂GeSe₃/Se is a promising strategy to improve the application of BST-based TE modules.

Keywords: Bi0.5Sb1.5Te3; band engineering; high performance; microstructure modulation; thermoelectric module.