Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

High Thermoelectric Performance in Supersaturated Solid Solutions and Nanostructured n-Type PbTe-GeTe

Journal Article · · Advanced Functional Materials
 [1];  [2];  [2];  [2];  [3];  [4];  [3];  [2];  [2];  [5];  [2]
  1. Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States); Northwestern University
  2. Northwestern Univ., Evanston, IL (United States)
  3. Univ. of Michigan, Ann Arbor, MI (United States)
  4. A*STAR (Agency for Science, Technology and Research), Innovis (Singapore)
  5. Nanyang Technological Univ. (Singapore)
Sb-doped and GeTe-alloyed n-type thermoelectric materials that show an excellent figure of merit ZT in the intermediate temperature range (400–800 K) are reported. The synergistic effect of favorable changes to the band structure resulting in high Seebeck coefficient and enhanced phonon scattering by point defects and nanoscale precipitates resulting in reduction of thermal conductivity are demonstrated. The samples can be tuned as single-phase solid solution (SS) or two-phase system with nanoscale precipitates (Nano) based on the annealing processes. The GeTe alloying results in band structure modification by widening the bandgap and increasing the density-ofstates effective mass of PbTe, resulting in significantly enhanced Seebeck coefficients. The nanoscale precipitates can improve the power factor in the low temperature range and further reduce the lattice thermal conductivity (κlat). Specifically, the Seebeck coefficient of Pb0.988Sb0.012Te–13%GeTe–Nano approaches -280 μV K-1 at 673 K with a low κlat of 0.56 W m-1 K-1 at 573 K. Consequently, a peak ZT value of 1.38 is achieved at 623 K. Furthermore, a high average ZTavg value of ≈1.04 is obtained in the temperature range from 300 to 773 K for n-type Pb0.988Sb0.012Te–13%GeTe–Nano.
Research Organization:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Organization:
International Institute for Nanotechnology; Keck Foundation; NSF; Nanyang Technological Univ.; National Natural Science Foundation of China; Singapore A*STAR Pharos Program; Singapore MOE AcRF Tier 1; State of Illinois; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357; SC0014520
OSTI ID:
1775351
Alternate ID(s):
OSTI ID: 1440785
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 31 Vol. 28; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (70)

Thermoelectric Devices for Power Generation: Recent Progress and Future Challenges : Thermoelectric Devices for Power Generation journal September 2015
The Criteria for Beneficial Disorder in Thermoelectric Solid Solutions journal October 2012
Beneficial Contribution of Alloy Disorder to Electron and Phonon Transport in Half-Heusler Thermoelectric Materials journal April 2013
Promising Thermoelectric Bulk Materials with 2D Structures journal July 2017
High Thermoelectric Figure of Merit in PbTe Alloys Demonstrated in PbTe-CdTe journal April 2012
Controlling Metallurgical Phase Separation Reactions of the Ge 0.87 Pb 0.13 Te Alloy for High Thermoelectric Performance journal March 2013
Optimum Carrier Concentration in n-Type PbTe Thermoelectrics journal May 2014
Functional Graded Germanium-Lead Chalcogenide-Based Thermoelectric Module for Renewable Energy Applications journal April 2015
Subtle Roles of Sb and S in Regulating the Thermoelectric Properties of N-Type PbTe to High Performance journal May 2017
n-Type SnSe 2 Oriented-Nanoplate-Based Pellets for High Thermoelectric Performance journal December 2017
Thermoelectric Figure of Merit of Some Compositions in the System (GeTe)1−x[(Ag2Te)1−y(Sb2Te3)y]x journal December 1991
Highly efficient bismuth telluride doped p-type Pb0.13Ge0.87Te for thermoelectric applications journal November 2007
Ge-Te (Germanium-Tellurium) book January 1996
Thermoelectric properties of dilute PbTe-GeTe alloys journal December 1971
Structural Evolution Following Spinodal Decomposition of the Pseudoternary Compound (Pb0.3Sn0.1Ge0.6)Te journal November 2009
Nature of the defects in germanium telluride journal March 1967
Optical properties of GeTe journal March 1967
Energy harvesting, reuse and upgrade to reduce primary energy usage in the USA journal October 2011
High thermoelectric performance of n-type PbTe1−S due to deep lying states induced by indium doping and spinodal decomposition journal April 2016
Extremely Low Thermal Conductivity in Thermoelectric Ge 0.55 Pb 0.45 Te Solid Solutions via Se Substitution journal August 2016
Rationally Designing High-Performance Bulk Thermoelectric Materials journal August 2016
Thermoelectric Performance of n -Type (PbTe) 0.75 (PbS) 0.15 (PbSe) 0.1 Composites journal June 2014
Molten salt synthesis and properties of three new solid-state ternary bismuth chalcogenides, .beta.-CsBiS2, .gamma.-CsBiS2, and K2Bi8Se13 journal March 1993
Nanostructured Thermoelectrics: The New Paradigm? journal February 2010
Heavy Doping and Band Engineering by Potassium to Improve the Thermoelectric Figure of Merit in p-Type PbTe, PbSe, and PbTe 1– y Se y journal June 2012
Thermoelectrics with Earth Abundant Elements: High Performance p-type PbS Nanostructured with SrS and CaS journal April 2012
Remarkable Roles of Cu To Synergistically Optimize Phonon and Carrier Transport in n-Type PbTe-Cu 2 Te journal December 2017
Convergence of electronic bands for high performance bulk thermoelectrics journal May 2011
High-performance bulk thermoelectrics with all-scale hierarchical architectures journal September 2012
Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals journal April 2014
Strained endotaxial nanostructures with high thermoelectric figure of merit journal January 2011
Non-equilibrium processing leads to record high thermoelectric figure of merit in PbTe–SrTe journal July 2016
Resonant bonding leads to low lattice thermal conductivity journal April 2014
Contrasting role of antimony and bismuth dopants on the thermoelectric performance of lead selenide journal May 2014
Broad temperature plateau for thermoelectric figure of merit ZT>2 in phase-separated PbTe0.7S0.3 journal July 2014
Giant anharmonic phonon scattering in PbTe journal June 2011
Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites journal October 2015
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect journal February 2020
Enhancement of thermoelectric figure-of-merit by resonant states of aluminium doping in lead selenide journal January 2012
Chemical composition tuning in quaternary p-type Pb-chalcogenides – a promising strategy for enhanced thermoelectric performance journal January 2014
Measuring thermoelectric transport properties of materials journal January 2015
Power generation from nanostructured PbTe-based thermoelectrics: comprehensive development from materials to modules journal January 2016
Enhanced average thermoelectric figure of merit of n-type PbTe 1−x I x –MgTe journal January 2015
Significant band engineering effect of YbTe for high performance thermoelectric PbTe journal January 2015
PbTe–PbSnS2 thermoelectric composites: low lattice thermal conductivity from large microstructures journal January 2012
Enhanced thermoelectric properties of p-type nanostructured PbTe–MTe (M = Cd, Hg) materials journal January 2013
All-scale hierarchical thermoelectrics: MgTe in PbTe facilitates valence band convergence and suppresses bipolar thermal transport for high performance journal January 2013
Nature of the cubic to rhombohedral structural transformation in (AgSbTe2)15(GeTe)85 thermoelectric material journal March 2007
Thermoelectric properties of Bi-doped PbTe composites journal May 2011
Improvements of the thermoelectric properties of PbTe via simultaneous doping with indium and iodine journal March 2012
Validity of rigid band approximation of PbTe thermoelectric materials journal July 2013
High thermoelectric potential of n -type Pb 1− x Ti x Te alloys journal August 2016
Weak electron-phonon coupling contributing to high thermoelectric performance in n-type PbSe journal May 2012
Inhomogeneous Electron Gas journal November 1964
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
Special points for Brillouin-zone integrations journal June 1976
Structure of the second valence band in PbTe journal July 1977
Projector augmented-wave method journal December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Thermoelectric enhancement in PbTe with K or Na codoping from tuning the interaction of the light- and heavy-hole valence bands journal September 2010
Calculated electronic structure of Pb 1 − x Mn x Te ( 0 ⩽ x < 11 % ) : The role of L and Σ valence band maxima journal March 2011
Minority carrier blocking to enhance the thermoelectric figure of merit in narrow-band-gap semiconductors journal April 2016
Generalized Gradient Approximation Made Simple journal October 1996
Inhomogeneous Electron Gas journal March 1973
Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States journal July 2008
Entropically Stabilized Local Dipole Formation in Lead Chalcogenides journal December 2010
Effect of elastic stresses on the thermoelectric properties of Pb1−x GexTe epitaxial layers journal July 2006
Influences of Potential Barrier Scattering on the Thermoelectric Properties of Sintered n-Type PbTe with a Small Grain Size journal February 2003
Ge-Te (Germanium-Tellurium) journal September 2000
Thermoelectric enhancement in PbTe with K, Na co-doping from tuning the interaction of the light and heavy hole valence bands text January 2010

Cited By (11)

Amphoteric Indium Enables Carrier Engineering to Enhance the Power Factor and Thermoelectric Performance in n ‐Type Ag n Pb 100 In n Te 100+2 n (LIST) journal March 2019
Anisotropy of Selected Mechanical Properties of PbTe journal February 2019
Ion Beam Induced Artifacts in Lead-Based Chalcogenides journal May 2019
Realizing high performance n-type PbTe by synergistically optimizing effective mass and carrier mobility and suppressing bipolar thermal conductivity journal January 2018
Effect of polymer nanolayers on tin-chalcogenide nanosheet/conductive polymer flexible composite films and their enhanced thermoelectric performance journal January 2019
Multifunctional inorganic nanomaterials for energy applications journal January 2020
Achieving high thermoelectric performance through constructing coherent interfaces and building interface potential barriers in n-type Bi 2 Te 3 /Bi 2 Te 2.7 Se 0.3 nanocomposites journal January 2019
Discordant nature of Cd in GeTe enhances phonon scattering and improves band convergence for high thermoelectric performance journal January 2020
Electrostatic self-assembly of a AgI/Bi 2 Ga 4 O 9 p–n junction photocatalyst for boosting superoxide radical generation journal January 2020
Non-stoichiometric defect-controlled reduction toward mixed-valence Mn-doped hexaaluminates and their optical applications journal January 2019
The high thermoelectric performance of slightly Sb doped PbTe alloys journal January 2020

Similar Records

High Figure of Merit in Gallium-Doped Nanostructured n-Type PbTe-xGeTe with Midgap States
Journal Article · Tue Sep 10 20:00:00 EDT 2019 · Journal of the American Chemical Society · OSTI ID:1776870

Extraordinary role of Zn in enhancing thermoelectric performance of Ga-doped n-type PbTe
Journal Article · Sun Dec 05 19:00:00 EST 2021 · Energy & Environmental Science · OSTI ID:1867598