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Thermoelectric performance of the p-type semiconductor bornite, Cu5FeS4, is greatly enhanced through chemical substitution. Nonstoichiometric materials in which the Cu:Fe ratio and overall cation-vacancy content were adjusted are reported, and a figure of merit, ZT = 0.79, is achieved at temperatures as low as 550 K in Cu4.972Fe0.968S4. All materials were synthesized mechanochemically and characterized by powder X-ray diffraction, differential scanning calorimetry (DSC), and thermal and electrical transport property measurements. Single-phase behavior is retained in copper deficient phases, Cu5–xFeS4, for vacancy levels up to x = 0.1, while in materials Cu5+yFe1–yS4, in which the Cu:Fe ratio is varied while maintaining full occupancy of cation sites, single-phase behavior persists for y ≤ 0.08. Adjusting the Cu:Fe ratio at a constant cation-vacancy level of 0.06 in Cu4.94+zFe1–zS4, leads to single phases for z ≤ 0.04. DSC measurements indicate the temperature of the intermediate- (2a) to high-temperature ...

High Thermoelectric Performance of Bornite through Control of the Cu(II) Content and Vacancy Concentration