Effects of Ge and Sn substitution on the metal–semiconductor transition and thermoelectric properties of Cu12Sb4S13 tetrahedrite. Issue 13 (15th March 2017)

• Record Type: Journal Article
• Authors: Kosaka, Yasufumi; Suekuni, Koichiro; Hashikuni, Katsuaki; Bouyrie, Yohan; Ohta, Michihiro; Takabatake, Toshiro
• Is Part Of: Physical chemistry chemical physics. Volume 19:Issue 13(2017)
• Page Start: 8874
• Page End: 8879
• Publication Date: 2017-03-15
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/c7cp00351j
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : The substitutions of Ge and Sn for Cu in Cu12 Sb4 S13 tetrahedrite lead to the suppression of the metal–semiconductor transition and enhancement of the thermoelectric performance. Abstract : The synthetic tetrahedrites Cu12− y Tr y Sb4 S13 (Tr: Mn, Fe, Co, Ni, Zn) have been extensively studied due to interest in metal–semiconductor transition as well as in superior thermoelectric performance. We have prepared Ge- and Sn-bearing tetrahedrites, Cu12− x M x Sb4 S13 (M = Ge, Sn; x ≤ 0.6), and investigated the effects of the substitutions on the phase transition and the thermoelectric properties. The substitutions of Ge and Sn for Cu suppress the metal–semiconductor transition and increase the electrical resistivity ρ and the positive thermopower S . This finding suggests that the phase transition is prevented by electron doping into the unoccupied states of the valence band. The variations of ρ, S, and magnetic susceptibility for the present systems correspond well with those for the system with Tr = Zn 2+, confirming the tetravalent states for Ge and Sn. The substitution of M 4+ for Cu 1+ decreases the power factor S 2 / ρ but enhances the dimensionless thermoelectric figure of merit ZT, due to reductions in both the charge carrier contribution and lattice contribution to the thermal conductivity. As a result, ZT has a maximum value of ∼0.65 at 665 K for x = 0.3–0.5 in Cu12− x M x Sb4 S13 with M = Ge and Sn.