P-type lead telluride (PbTe) emerged as a promising thermoelectric material for intermediate-temperature waste-heat-energy harvesting. However, n-type PbTe still confronted with a considerable challenge owing to its relatively low figure of merit ZT and conversion efficiency η, limiting widespread thermoelectric applications. Here, we report that Ga-doping in n-type PbTe can optimize carrier concentration and thus improve the power factor. Moreover, further experimental and theoretical evidence reveals that Ga-doping-induced multiphase structures with nano- to micrometer size can simultaneously modulate phonon transport, leading to dramatic reduction of lattice thermal conductivity. As a consequence, a tremendous enhancement of ZT value at 823 K reaches ∼1.3 for n-type PbGaTe. In particular, in a wide temperature range from 323 to 823 K, the average ZT value of ∼0.9 and the calculated conversion efficiency η of ∼13% are achieved by Ga doping. The present findings demonstrate the great potential in Ga-doped PbTe thermoelectric materials through a synergetic carrier tuning and multiphase engineering strategy.
Texturization tuning is of crucial significance for designing
and
developing high-performance thermoelectric materials and devices.
Here, we report for the first time that a strong texturization effect
induces an in-plane high-performance thermoelectric and an out-of-plane
low lattice thermal conductivity in Sb-substituted misfit-layered
(SnS)1.2(TiS2)2 alloys. In the in-plane
direction, the oriented texture promotes a high carrier mobility,
contributing to the maximization of the power factor (∼0.90
mW K–2 m–1). Moreover, the in-plane
lattice thermal conductivity dramatically reduces deriving from the
point defects due to the Sb substitution and weakened transverse sound
velocity owing to the softening of bonding, ultimately leading to
one of the highest thermoelectric performances ever reported among
misfit-layered chalcogenides. In particular, in the out-of-plane direction,
the texturization triggers the lowest lattice thermal conductivity
(∼0.39 W K–1 m–1), exceeding
the theoretical limit of the Debye–Cahill model, which provides
a precious opportunity to investigate this real Sb-substituted (SnS)1.2(TiS2)2 material. The present finding
in misfit-layered chalcogenides provides a novel strategy for manipulating
thermoelectrics via texturization engineering.
The traditional thermoelectric material GeTe has drawn much attention recently because of the reported high thermoelectric performance of the rhombohedral phase in lowtemperature ranges, where the split L and Σ band can be reconverged to have a small energy offset and thus high density of state effective mass according to the rhombohedral angle. In addition, In doping in GeTe is also reported to enhance the density of effective mass and therefore increase the Seebeck coefficient because of the induced resonant levels. In this work, In and Pb are doped in GeTe, and In doping leads to an increase in the rhombohedral angle and thus enhanced density of state effective mass in addition to the resonant effect. However, the improved Seebeck coefficient result from In doping is compensated for by a sharp reduction of Hall mobility, leading to no significant enhancement of electronic performance in the rhombohedral phase. By further Pb/Ge doping in the matrix Ge 0.95 In 0.05 Te for the optimization of carrier concentration and reduction of lattice thermal conductivity (as low as 0.7 W/mK), a zT as high as ∼1.2 at 550 K and average zT of ∼0.75 between 300 and 550 K are realized in this work, demonstrating GeTe as a promising candidate for near-room-temperature application.
We have systematically studied the thermoelectric properties in Zn-doped SnTe. Strikingly, band convergence and embedded precipitates arising from Zn doping, can trigger a prominent improvement of thermoelectric performance. In particular, the value of dimensionless figure of merit zT has increased by 100% and up to ∼ 0.5 at 775 K for the optimal sample with 2% Zn content. Present findings demonstrate that carrier concentration and effective mass play crucial roles on the Seebeck coefficient and power factor. The obvious deviation from the Pisarenko line (Seebeck coefficient versus carrier concentration) due to Zn-doping reveals the convergence of valence bands. When the doping concentration exceeds the solubility, precipitates occur and lead to a reduction of lattice thermal conductivity. In addition, bipolar conduction is suppressed, indicating an enlargement of band gap. The Zn-doped SnTe is shown to be a promising candidate for thermoelectric applications.
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