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Gu, Yan; Shi, Xiao‐Lei; Pan, Lin; Liu, Wei‐Di; Sun, Qiang; Tang, Xiao; Kou, Liang‐Zhi; Liu, Qing‐Feng; Wang, Yi‐Feng; Chen, Zhi‐Gang
Advanced functional materials, 06/2021, Volume: 31, Issue: 25Journal Article
In this work, a record high thermoelectric figure‐of‐merit ZT of 1.6 ± 0.2 at 873 K in p‐type polycrystalline Bi0.94Pb0.06CuSe1.01O0.99 by a synergy of rational band manipulation and novel nanostructural design is reported. First‐principles density functional theory calculation results indicate that the density of state at the Fermi level that crosses the valence band can be significantly reduced and the measured optical bandgap can be enlarged from 0.70 to 0.74 eV by simply replacing 1% O with 1% Se, both indicating a potentially reduced carrier concentration and in turn, an improved carrier mobility and a boosted power factor up to 9.0 µW cm−1 K−2. Meanwhile, comprehensive characterizations reveal that under Se‐rich condition, Cu2Se secondary microphases and significant lattice distortions triggered by Pb‐doping and Se‐substitution can be simultaneously achieved, contributing to a reduced lattice thermal conductivity of 0.4 W m−1 K−1. Furthermore, a unique shear exfoliation technique enables an effective grain refinement with higher anisotropy of the polycrystalline pellet, leading to a further improved power factor up to 10.9 µW cm−1 K−2 and a further reduced lattice thermal conductivity of 0.30 W m−1 K−1, which gives rise to record high ZT. A record high thermoelectric figure‐of‐merit ZT of 1.6 ± 0.2 at 873 K in p‐type polycrystalline Bi0.94Pb0.06CuSe1.01O0.99 by a synergy of rational band manipulation and novel nanostructural design is reported.
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