zT = 1.1 in CuInTe₂ Solid Solutions Enabled by Rational Defect Engineering

In this study, the synthesis and thermoelectric performance of CuInTe2–In2Te3 and Cu0.85Ag0.15InTe2–In2Te3 solid solutions are reported. The experimental results associated with model fitting reveal that the cation vacancies generated by creating solid solutions with a compound with a smaller cation-to-anion ratio can strongly scatter phonons with high frequency, which remarkably decrease the total as well as lattice thermal conductivity of the CuInTe2 system and finally realize an enhanced thermoelectric properties compared to the pristine sample. Furthermore, substitutional Ag/Cu defects integrated with vacancies lead to a further reduction in lattice thermal conductivity. With the benefit from the rational defect design, a high figure of merit of 1.1 is gained at 840 K for the sample (Cu0.85Ag0.15InTe2)0.98(In2Te3)0.02. In addition, a 188% improvement on average zT is obtained. This work provides an effective method for boosting thermoelectric performance of chalcopyrite compounds by defect engineering on multiple types of defects.