Thermoelectric technology allows conversion between heat and electricity. Many good thermoelectric materials contain rare or toxic elements, so developing low-cost and high-performance thermoelectric materials is warranted. Here, we report the temperature-dependent interplay of three separate electronic bands in hole-doped tin sulfide (SnS) crystals. This behavior leads to synergistic optimization between effective mass (m*) and carrier mobility (μ) and can be boosted through introducing selenium (Se). This enhanced the power factor from ~30 to ~53 microwatts per centimeter per square kelvin (μW cm−1 K−2 at 300 K), while lowering the thermal conductivity after Se alloying. As a result, we obtained a maximum figure of merit ZT (ZTmax) of ~1.6 at 873 K and an average ZT (ZTave) of ~1.25 at 300 to 873 K in SnS0.91Se0.09 crystals. Our strategy for band manipulation offers a different route for optimizing thermoelectric performance. The high-performance SnS crystals represent an important step toward low-cost, Earth-abundant, and environmentally friendly thermoelectrics.
The layered oxyselenide BiCuSeO system is known as one of the high‐performance thermoelectric materials with intrinsically low thermal conductivity. By employing atomic, nano‐ to mesoscale structural optimizations, low thermal conductivity coupled with enhanced electrical transport properties can be readily achieved. Upon partial substitution of Bi3+ by Ca2+ and Pb2+, the thermal conductivity can be reduced to as low as 0.5 W m−1 K−1 at 873 K through dual‐atomic point‐defect scattering, while a high power factor of ≈1 × 10−3 W cm−1 K−2 is realized over a broad temperature range from 300 to 873 K. The synergistically optimized power factor and intrinsically low thermal conductivity result in a high ZT value of ≈1.5 at 873 K for Bi0.88Ca0.06Pb0.06CuSeO, a promising candidate for high‐temperature thermoelectric applications. It is envisioned that the all‐scale structural optimization is critical for optimizing the thermoelectricity of quaternary compounds.
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