TY - JOUR
T1 - High thermoelectric performance of p-type SnTe via a synergistic band engineering and nanostructuring approach
AU - Tan, Gangjian
AU - Zhao, Li Dong
AU - Shi, Fengyuan
AU - Doak, Jeff W.
AU - Lo, Shih Han
AU - Sun, Hui
AU - Wolverton, Chris
AU - Dravid, Vinayak P.
AU - Uher, Ctirad
AU - Kanatzidis, Mercouri G.
PY - 2014/5/14
Y1 - 2014/5/14
N2 - SnTe is a potentially attractive thermoelectric because it is the lead-free rock-salt analogue of PbTe. However, SnTe is a poor thermoelectric material because of its high hole concentration arising from inherent Sn vacancies in the lattice and its very high electrical and thermal conductivity. In this study, we demonstrate that SnTe-based materials can be controlled to become excellent thermoelectrics for power generation via the successful application of several key concepts that obviate the well-known disadvantages of SnTe. First, we show that Sn self-compensation can effectively reduce the Sn vacancies and decrease the hole carrier density. For example, a 3 mol % self-compensation of Sn results in a 50% improvement in the figure of merit ZT. In addition, we reveal that Cd, nominally isoelectronic with Sn, favorably impacts the electronic band structure by (a) diminishing the energy separation between the light-hole and heavy-hole valence bands in the material, leading to an enhanced Seebeck coefficient, and (b) enlarging the energy band gap. Thus, alloying with Cd atoms enables a form of valence band engineering that improves the high-temperature thermoelectric performance, where p-type samples of SnCd0.03Te exhibit ZT values of ∼0.96 at 823 K, a 60% improvement over the Cd-free sample. Finally, we introduce endotaxial CdS or ZnS nanoscale precipitates that reduce the lattice thermal conductivity of SnCd0.03Te with no effect on the power factor. We report that SnCd0.03Te that are endotaxially nanostructured with CdS and ZnS have a maximum ZTs of ∼1.3 and ∼1.1 at 873 K, respectively. Therefore, SnTe-based materials could be ideal alternatives for p-type lead chalcogenides for high temperature thermoelectric power generation.
AB - SnTe is a potentially attractive thermoelectric because it is the lead-free rock-salt analogue of PbTe. However, SnTe is a poor thermoelectric material because of its high hole concentration arising from inherent Sn vacancies in the lattice and its very high electrical and thermal conductivity. In this study, we demonstrate that SnTe-based materials can be controlled to become excellent thermoelectrics for power generation via the successful application of several key concepts that obviate the well-known disadvantages of SnTe. First, we show that Sn self-compensation can effectively reduce the Sn vacancies and decrease the hole carrier density. For example, a 3 mol % self-compensation of Sn results in a 50% improvement in the figure of merit ZT. In addition, we reveal that Cd, nominally isoelectronic with Sn, favorably impacts the electronic band structure by (a) diminishing the energy separation between the light-hole and heavy-hole valence bands in the material, leading to an enhanced Seebeck coefficient, and (b) enlarging the energy band gap. Thus, alloying with Cd atoms enables a form of valence band engineering that improves the high-temperature thermoelectric performance, where p-type samples of SnCd0.03Te exhibit ZT values of ∼0.96 at 823 K, a 60% improvement over the Cd-free sample. Finally, we introduce endotaxial CdS or ZnS nanoscale precipitates that reduce the lattice thermal conductivity of SnCd0.03Te with no effect on the power factor. We report that SnCd0.03Te that are endotaxially nanostructured with CdS and ZnS have a maximum ZTs of ∼1.3 and ∼1.1 at 873 K, respectively. Therefore, SnTe-based materials could be ideal alternatives for p-type lead chalcogenides for high temperature thermoelectric power generation.
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U2 - 10.1021/ja500860m
DO - 10.1021/ja500860m
M3 - Article
C2 - 24785377
AN - SCOPUS:84900803805
SN - 0002-7863
VL - 136
SP - 7006
EP - 7017
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 19
ER -