High-Performance Tellurium-Free Thermoelectrics: All-Scale Hierarchical Structuring of p-Type PbSe–MSe Systems (M = Ca, Sr, Ba)

Lee, Yeseul; Lo, Shih Han; Androulakis, J.; Wu, Chun I.; Zhao, Li‐Dong; Chung, Duck Young; Hogan, Timothy P.; Dravid, Vinayak P.; Kanatzidis, Mercouri G.

doi:10.1021/ja400069s

Cited by 138 publications

(135 citation statements)

References 37 publications

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“…Lead chalcogenides are the most studied thermoelectric materials with high ZT values between 1.4 and 2.2, 4,12,[14][15][16] although concerns about Pb (e.g. toxicity) limit their large scale application.…”

Section: -15mentioning

confidence: 99%

“…An approach to obtaining high power factors involves manipulation of the density of states through band engineering, including band convergence/degeneracy [4][5][6] or introduction of resonant impurity levels near the Fermi level. 7,8 Methods to block the propagation of phonons include the introduction of point defects, 9,10 second phase nanoprecipitates 11,12 and mesoscale grain boundaries.…”

Section: Introductionmentioning

confidence: 99%

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Lead-free SnTe-based thermoelectrics: enhancement of thermoelectric performance by doping with Gd/Ag

et al. 2016

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SnTe, with the same rock-salt structure as PbTe, is a potentially attractive thermoelectric material. Pristine SnTe has poor thermoelectric performance because of its very high hole concentration resulting from intrinsic Sn vacancies, which leads to a high thermal conductivity and a low Seebeck coefficient. In this work, the thermoelectric properties of SnTe were modified by doping with different contents of gadolinium and silver. It is found that SnTe doped with optimal gadolinium (i.e. Gd0.06Sn0.94Te) exhibited extraordinarily low lattice thermal conductivity that is close to the theoretical minimum. The drastic reduction of lattice thermal conductivity is attributed to the formation of nanoprecipitates, which strongly scatter phonons by mass fluctuation between a second phase and matrix coupled with mesoscale scattering via grain boundaries. Further doping Gd0.06Sn0.94Te with Ag leads to a higher Seebeck coefficient due to the decreased carrier concentration and adjusted phase composition. Optimal Ag doping leads to a 3 times and 2 times enhancement of the figure of merit (ZT) in comparison with SnTe and Gd0.06Sn0.94Te, respectively, i.e. a ZT of ∼1.1 was obtained for 11 atom% Ag-containing Gd0.06Sn0.94Te at 873 K.

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Section: -15mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Lead-free SnTe-based thermoelectrics: enhancement of thermoelectric performance by doping with Gd/Ag

et al. 2016

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“…The well-known PbSe system [19][20][21][22][23] is now attracting considerable attention as a promising thermoelectric material for high temperature power generation applications. Heavily doped p-type PbSe has shown ZTs as high as ~ 1.2 at 850 K [24,25], while after the simultaneous improvement of both electrical and thermal…”

Section: Introductionmentioning

confidence: 99%

“…properties ZT values of ~ 1.4 -1.6 can be obtained [9,12,25]. Theoretical calculations have suggested that hole-doped PbSe can potentially reach ZT ~ 2 at 1000 K [26] indicating prospects for further performance improvements.…”

Section: Introductionmentioning

confidence: 99%

Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe

Chasapis¹,

Lee²,

Hatzikraniotis

et al. 2015

Phys. Rev. B

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“…This is achieved by substituting some of the atoms with dopant elements of different valance [7]. Sodium is the most viable p--type dopant [1,2,10,11] for Pb chalcogenides, though its solubility has been shown to be limited [12,13]. Sodium doping results in considerably higher thermoelectric performance of p--type multiphase compounds when the alloys are doped at concentrations greater than the solubility limit of the matrix [2,5,11,14].…”

Section: Introductionmentioning

confidence: 99%

Elemental distributions within multiphase quaternary Pb chalcogenide thermoelectric materials determined through three-dimensional atom probe tomography

Yamini

Mitchell

et al. 2016

Nano Energy

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Nanostructured multiphase p-type lead chalcogenides have shown the highest efficiencies amongst thermoelectric materials. However, their electronic transport properties have been described assuming homogenous distribution of dopants between phases. Here, we have analyzed elemental distributions in precipitates and matrices of nanostructured multiphase quaternary Pb chalcogenides doped to levels below and above the solubility limit of the matrix, using three-dimensional atom probe tomography. We demonstrate that partitioning of sodium and selenium occur between the matrix and secondary phase in both lightly-and heavily-doped compounds and that the concentrations of sodium and selenium in precipitates are higher than those in the matrices. This can contribute to the transport properties of such multiphase compounds The sodium concentration reached ~3 at% in sulfur-rich (PbS) precipitates and no nano precipitates of Na-rich phases were observed within either phase, a result that is supported by high resolution TEM analysis, indicating that the solubility limit of sodium in PbS is much higher than previously thought. However, non-equilibrium segregation of sodium is identified at the precipitates/matrix interfaces. These findings can lead to further advances in designing and characterizing multiphase thermoelectric materials. AbstractNanostructured multiphase p--type lead chalcogenides have shown the highest efficiencies amongst thermoelectric materials. However, their electronic transport properties have been described assuming homogenous distribution of dopants between phases. Here, we have analyzed elemental distributions in precipitates and matrices of nanostructured multiphase quaternary Pb chalcogenides doped to levels below and above the solubility limit of the matrix, using three--dimensional atom probe tomography. We demonstrate that partitioning of sodium and selenium occur between the matrix and secondary phase in both lightly-- and heavily--doped compounds and that the concentrations of sodium and selenium in precipitates are higher than those in the matrices. This can contribute to the transport properties of such multiphase compounds The sodium concentration reached ~3 at.% in sulfur--rich (PbS) precipitates and no nano precipitates of Na--rich phases were observed within either phase, a result that is supported by high resolution TEM analysis, indicating that the solubility limit of sodium in PbS is much higher than previously thought. However, non--equilibrium segregation of sodium is identified at the precipitates/matrix interfaces. These findings can lead to further advances in designing and characterizing multiphase thermoelectric materials.

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High-Performance Tellurium-Free Thermoelectrics: All-Scale Hierarchical Structuring of p-Type PbSe–MSe Systems (M = Ca, Sr, Ba)

Cited by 138 publications

References 37 publications

Lead-free SnTe-based thermoelectrics: enhancement of thermoelectric performance by doping with Gd/Ag

Lead-free SnTe-based thermoelectrics: enhancement of thermoelectric performance by doping with Gd/Ag

Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe

Elemental distributions within multiphase quaternary Pb chalcogenide thermoelectric materials determined through three-dimensional atom probe tomography

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