Ultralow Thermal Conductivity and High-Temperature Thermoelectric Performance in n-Type K2.5Bi8.5Se14

Zhong Zhen Luo, Songting Cai, Shiqiang Hao, Trevor P. Bailey, Xiaobing Hu, Riley Hanus, Runchu Ma, Gangjian Tan, Daniel G. Chica, G. Jeffrey Snyder, Ctirad Uher, Christopher Wolverton, Vinayak P. Dravid, Qingyu Yan, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

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Abstract

We studied the narrow band-gap (0.55 eV) semiconductor K2.5Bi8.5Se14 as a potential thermoelectric material for power generation. Samples of polycrystalline K2.5Bi8.5Se14 prepared by spark plasma sintering exhibit exceptionally low lattice thermal conductivities (κlat) of 0.57-0.33 W m-1 K-1 in the temperature range of 300-873 K. The physical origin of such low κlat in K2.5Bi8.5Se14 is related to the strong anharmonicity and low phonon velocity caused by its complex low symmetry, large unit cell crystal structure, and mixed occupancy of Bi and K atoms in the lattice. High-resolution scanning transmission electron microscopy studies and microanalysis indicate that the K2.5Bi8.5Se14 sample is a single phase without intergrowth of the structurally related K2Bi8Se13 phase. The undoped material exhibits an n-type character and a figure-of-merit (ZT) value of 0.67 at 873 K. Electronic band structure calculations indicate that K2.5Bi8.5Se14 is an indirect band-gap semiconductor with multiple conduction bands close to the Fermi level. Phonon dispersion calculations suggest that K2.5Bi8.5Se14 has low phonon velocities and large Grüneisen parameters that can account for the observed ultralow κlat. The degree of n-type doping can be controlled by introducing Se deficiencies in the structure, providing a simple route to increase the ZT to ∼1 at 873 K.

Original languageEnglish
Pages (from-to)5943-5952
Number of pages10
JournalChemistry of Materials
Volume31
Issue number15
DOIs
Publication statusPublished - Aug 13 2019

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Thermal conductivity
Energy gap
Semiconductor materials
Spark plasma sintering
Microanalysis
Crystal symmetry
Fermi level
Conduction bands
Band structure
Temperature
Power generation
Crystal structure
Doping (additives)
Transmission electron microscopy
Atoms
Scanning electron microscopy

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

Ultralow Thermal Conductivity and High-Temperature Thermoelectric Performance in n-Type K2.5Bi8.5Se14 . / Luo, Zhong Zhen; Cai, Songting; Hao, Shiqiang; Bailey, Trevor P.; Hu, Xiaobing; Hanus, Riley; Ma, Runchu; Tan, Gangjian; Chica, Daniel G.; Snyder, G. Jeffrey; Uher, Ctirad; Wolverton, Christopher; Dravid, Vinayak P.; Yan, Qingyu; Kanatzidis, Mercouri G.

In: Chemistry of Materials, Vol. 31, No. 15, 13.08.2019, p. 5943-5952.

Research output: Contribution to journalArticle

Luo, ZZ, Cai, S, Hao, S, Bailey, TP, Hu, X, Hanus, R, Ma, R, Tan, G, Chica, DG, Snyder, GJ, Uher, C, Wolverton, C, Dravid, VP, Yan, Q & Kanatzidis, MG 2019, 'Ultralow Thermal Conductivity and High-Temperature Thermoelectric Performance in n-Type K2.5Bi8.5Se14 ', Chemistry of Materials, vol. 31, no. 15, pp. 5943-5952. https://doi.org/10.1021/acs.chemmater.9b02327
Luo, Zhong Zhen ; Cai, Songting ; Hao, Shiqiang ; Bailey, Trevor P. ; Hu, Xiaobing ; Hanus, Riley ; Ma, Runchu ; Tan, Gangjian ; Chica, Daniel G. ; Snyder, G. Jeffrey ; Uher, Ctirad ; Wolverton, Christopher ; Dravid, Vinayak P. ; Yan, Qingyu ; Kanatzidis, Mercouri G. / Ultralow Thermal Conductivity and High-Temperature Thermoelectric Performance in n-Type K2.5Bi8.5Se14 In: Chemistry of Materials. 2019 ; Vol. 31, No. 15. pp. 5943-5952.
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abstract = "We studied the narrow band-gap (0.55 eV) semiconductor K2.5Bi8.5Se14 as a potential thermoelectric material for power generation. Samples of polycrystalline K2.5Bi8.5Se14 prepared by spark plasma sintering exhibit exceptionally low lattice thermal conductivities (κlat) of 0.57-0.33 W m-1 K-1 in the temperature range of 300-873 K. The physical origin of such low κlat in K2.5Bi8.5Se14 is related to the strong anharmonicity and low phonon velocity caused by its complex low symmetry, large unit cell crystal structure, and mixed occupancy of Bi and K atoms in the lattice. High-resolution scanning transmission electron microscopy studies and microanalysis indicate that the K2.5Bi8.5Se14 sample is a single phase without intergrowth of the structurally related K2Bi8Se13 phase. The undoped material exhibits an n-type character and a figure-of-merit (ZT) value of 0.67 at 873 K. Electronic band structure calculations indicate that K2.5Bi8.5Se14 is an indirect band-gap semiconductor with multiple conduction bands close to the Fermi level. Phonon dispersion calculations suggest that K2.5Bi8.5Se14 has low phonon velocities and large Gr{\"u}neisen parameters that can account for the observed ultralow κlat. The degree of n-type doping can be controlled by introducing Se deficiencies in the structure, providing a simple route to increase the ZT to ∼1 at 873 K.",
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AU - Bailey, Trevor P.

AU - Hu, Xiaobing

AU - Hanus, Riley

AU - Ma, Runchu

AU - Tan, Gangjian

AU - Chica, Daniel G.

AU - Snyder, G. Jeffrey

AU - Uher, Ctirad

AU - Wolverton, Christopher

AU - Dravid, Vinayak P.

AU - Yan, Qingyu

AU - Kanatzidis, Mercouri G

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N2 - We studied the narrow band-gap (0.55 eV) semiconductor K2.5Bi8.5Se14 as a potential thermoelectric material for power generation. Samples of polycrystalline K2.5Bi8.5Se14 prepared by spark plasma sintering exhibit exceptionally low lattice thermal conductivities (κlat) of 0.57-0.33 W m-1 K-1 in the temperature range of 300-873 K. The physical origin of such low κlat in K2.5Bi8.5Se14 is related to the strong anharmonicity and low phonon velocity caused by its complex low symmetry, large unit cell crystal structure, and mixed occupancy of Bi and K atoms in the lattice. High-resolution scanning transmission electron microscopy studies and microanalysis indicate that the K2.5Bi8.5Se14 sample is a single phase without intergrowth of the structurally related K2Bi8Se13 phase. The undoped material exhibits an n-type character and a figure-of-merit (ZT) value of 0.67 at 873 K. Electronic band structure calculations indicate that K2.5Bi8.5Se14 is an indirect band-gap semiconductor with multiple conduction bands close to the Fermi level. Phonon dispersion calculations suggest that K2.5Bi8.5Se14 has low phonon velocities and large Grüneisen parameters that can account for the observed ultralow κlat. The degree of n-type doping can be controlled by introducing Se deficiencies in the structure, providing a simple route to increase the ZT to ∼1 at 873 K.

AB - We studied the narrow band-gap (0.55 eV) semiconductor K2.5Bi8.5Se14 as a potential thermoelectric material for power generation. Samples of polycrystalline K2.5Bi8.5Se14 prepared by spark plasma sintering exhibit exceptionally low lattice thermal conductivities (κlat) of 0.57-0.33 W m-1 K-1 in the temperature range of 300-873 K. The physical origin of such low κlat in K2.5Bi8.5Se14 is related to the strong anharmonicity and low phonon velocity caused by its complex low symmetry, large unit cell crystal structure, and mixed occupancy of Bi and K atoms in the lattice. High-resolution scanning transmission electron microscopy studies and microanalysis indicate that the K2.5Bi8.5Se14 sample is a single phase without intergrowth of the structurally related K2Bi8Se13 phase. The undoped material exhibits an n-type character and a figure-of-merit (ZT) value of 0.67 at 873 K. Electronic band structure calculations indicate that K2.5Bi8.5Se14 is an indirect band-gap semiconductor with multiple conduction bands close to the Fermi level. Phonon dispersion calculations suggest that K2.5Bi8.5Se14 has low phonon velocities and large Grüneisen parameters that can account for the observed ultralow κlat. The degree of n-type doping can be controlled by introducing Se deficiencies in the structure, providing a simple route to increase the ZT to ∼1 at 873 K.

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