Abstract
Cu3SbSe4 is a potential p-type thermoelectric material, distinguished by its earth-abundant, inexpensive, innocuous, and environmentally friendly components. Nonetheless, the thermoelectric performance is poor and remains subpar. Herein, the electrical and thermal transport properties of Cu3SbSe4 were synergistically optimized by S alloying. Firstly, S alloying widened the band gap, effectively alleviating the bipolar effect. Additionally, the substitution of S in the lattice significantly increased the carrier effective mass, leading to a large Seebeck coefficient of ~730 μVK-1. Moreover, S alloying yielded point defect and Umklapp scattering to significantly depress the lattice thermal conductivity, and thus brought about an ultralow κlat ~0.50 Wm-1K-1 at 673 K in the solid solution. Consequently, multiple effects induced by S alloying enhanced the thermoelectric performance of the Cu3SbSe4-Cu3SbS4 solid solution, resulting in a maximum ZT value of ~0.72 at 673 K for the Cu3SbSe2.8S1.2 sample, which was ~44% higher than that of pristine Cu3SbSe4. This work offers direction on improving the comprehensive TE in solid solutions via elemental alloying.
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