Abstract
The series of Pb9.6Sb0.2Te10-xSe x compounds with different Se content (x) were prepared, and their structure was investigated at the atomic and nanosized regime level. Thermoelectric properties were measured in the temperature range from 300 to 700 K. The Pb9.6Sb0.2Te10-xSex series was designed after the refinement of the single-crystal structure of Pb 3.82Sb0.12Te4 (Pb9.6Sb 0.3Te10; S.G. Pm3̄m) by substituting isoelectronically in anion positions Te by Se. The Pb9.6Sb 0.2Te10-xSex compounds show significantly lower lattice thermal conductivity (κL) compared to the well-known PbTe1-xSex solid solutions. For Pb9.6Sb 0.2Te3Se7 (x = 7), a κL value as low as 0.40 W/m-K was determined at 700 K. High-resolution transmission electron microscopy of several Pb9.6Sb0.2Te 10-xSex samples showed widely distributed Sb-rich nanocrystals in the samples which is the key feature for the strong reduction of the lattice thermal conductivity. The reduction of κL results in a significantly enhanced thermoelectric figure of merit of Pb 9.6Sb0.2Te10-xSex compared to the corresponding PbTe1-xSex solid solution alloys. For Pb9.6Sb0.2Te3Se7 (x= 7), a maximum figure of merit of ZT ≈ 1.2 was obtained at ∼650 K. This value is about 50% higher than that of the state-of-the-art n-type PbTe. The work provides experimental validation of the theoretical concept that embedded nanocrystals can promote strong scattering of acoustic phonons.
| Original language | English |
|---|---|
| Pages (from-to) | 14347-14355 |
| Number of pages | 9 |
| Journal | Journal of the American Chemical Society |
| Volume | 128 |
| Issue number | 44 |
| DOIs | |
| Publication status | Published - Nov 8 2006 |
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Nanostructures versus solid solutions : Low lattice thermal conductivity and enhanced thermoelectric figure of merit in Pb9.6Sb 0.2Te10-xSex bulk materials. / Poudeu, Pierre F P; D'Angelo, Jonathan; Kong, Huijun; Downey, Adam; Short, Jarrod L.; Pcionek, Robert; Hogan, Timothy P.; Uher, Ctirad; Kanatzidis, Mercouri G.
In: Journal of the American Chemical Society, Vol. 128, No. 44, 08.11.2006, p. 14347-14355.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Nanostructures versus solid solutions
T2 - Low lattice thermal conductivity and enhanced thermoelectric figure of merit in Pb9.6Sb 0.2Te10-xSex bulk materials
AU - Poudeu, Pierre F P
AU - D'Angelo, Jonathan
AU - Kong, Huijun
AU - Downey, Adam
AU - Short, Jarrod L.
AU - Pcionek, Robert
AU - Hogan, Timothy P.
AU - Uher, Ctirad
AU - Kanatzidis, Mercouri G
PY - 2006/11/8
Y1 - 2006/11/8
N2 - The series of Pb9.6Sb0.2Te10-xSe x compounds with different Se content (x) were prepared, and their structure was investigated at the atomic and nanosized regime level. Thermoelectric properties were measured in the temperature range from 300 to 700 K. The Pb9.6Sb0.2Te10-xSex series was designed after the refinement of the single-crystal structure of Pb 3.82Sb0.12Te4 (Pb9.6Sb 0.3Te10; S.G. Pm3̄m) by substituting isoelectronically in anion positions Te by Se. The Pb9.6Sb 0.2Te10-xSex compounds show significantly lower lattice thermal conductivity (κL) compared to the well-known PbTe1-xSex solid solutions. For Pb9.6Sb 0.2Te3Se7 (x = 7), a κL value as low as 0.40 W/m-K was determined at 700 K. High-resolution transmission electron microscopy of several Pb9.6Sb0.2Te 10-xSex samples showed widely distributed Sb-rich nanocrystals in the samples which is the key feature for the strong reduction of the lattice thermal conductivity. The reduction of κL results in a significantly enhanced thermoelectric figure of merit of Pb 9.6Sb0.2Te10-xSex compared to the corresponding PbTe1-xSex solid solution alloys. For Pb9.6Sb0.2Te3Se7 (x= 7), a maximum figure of merit of ZT ≈ 1.2 was obtained at ∼650 K. This value is about 50% higher than that of the state-of-the-art n-type PbTe. The work provides experimental validation of the theoretical concept that embedded nanocrystals can promote strong scattering of acoustic phonons.
AB - The series of Pb9.6Sb0.2Te10-xSe x compounds with different Se content (x) were prepared, and their structure was investigated at the atomic and nanosized regime level. Thermoelectric properties were measured in the temperature range from 300 to 700 K. The Pb9.6Sb0.2Te10-xSex series was designed after the refinement of the single-crystal structure of Pb 3.82Sb0.12Te4 (Pb9.6Sb 0.3Te10; S.G. Pm3̄m) by substituting isoelectronically in anion positions Te by Se. The Pb9.6Sb 0.2Te10-xSex compounds show significantly lower lattice thermal conductivity (κL) compared to the well-known PbTe1-xSex solid solutions. For Pb9.6Sb 0.2Te3Se7 (x = 7), a κL value as low as 0.40 W/m-K was determined at 700 K. High-resolution transmission electron microscopy of several Pb9.6Sb0.2Te 10-xSex samples showed widely distributed Sb-rich nanocrystals in the samples which is the key feature for the strong reduction of the lattice thermal conductivity. The reduction of κL results in a significantly enhanced thermoelectric figure of merit of Pb 9.6Sb0.2Te10-xSex compared to the corresponding PbTe1-xSex solid solution alloys. For Pb9.6Sb0.2Te3Se7 (x= 7), a maximum figure of merit of ZT ≈ 1.2 was obtained at ∼650 K. This value is about 50% higher than that of the state-of-the-art n-type PbTe. The work provides experimental validation of the theoretical concept that embedded nanocrystals can promote strong scattering of acoustic phonons.
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U2 - 10.1021/ja0647811
DO - 10.1021/ja0647811
M3 - Article
VL - 128
SP - 14347
EP - 14355
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 44
ER -