DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Thermoelectric transport properties of polycrystalline SnSe alloyed with PbSe

Abstract

Single-crystal SnSe has been found to exhibit exceptional thermoelectric performance, but the efficiency of polycrystalline samples is still far from satisfactory. In this paper, with an intention to effectively suppress heat conduction and minimally affect hole transport, we alloyed p-type polycrystalline SnSe with PbSe. Single-phase Sn1-xPbxSe solid solutions were formed up to x ≈ 0.12. The lattice thermal conductivity was reduced from 1.4 to 0.85 W m-1 K-1 by 12 at. % PbSe alloying due to strain and mass fluctuations. Interestingly, the Seebeck coefficient and carrier concentration were nearly unchanged by Pb substitution, indicating a constant effective mass and an undisrupted valence band maximum. A peak figure of merit (ZT) of 0.85 at 800 K was obtained in the x = 0 sample, and relatively high performance was also achieved in solid solutions. Finally, a concise model was developed involving multiple carrier scattering mechanisms, capturing the dependence of the mobility on composition and temperature.

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [3]; ORCiD logo [1];  [4];  [2]
  1. Tsinghua Univ., Beijing (China). State Key Lab. of New Ceramics and Fine Processing. School of Materials Science and Engineering
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  3. Beihang Univ., Beijing (China). School of Materials Science and Engineering
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States); Tsinghua Univ., Beijing (China); Beihang Univ., Beijing (China); Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); 973 Program (China)
OSTI Identifier:
1465976
Alternate Identifier(s):
OSTI ID: 1351028
Grant/Contract Number:  
SC0014520; SC0001299; 11474176; 2013CB632503
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 110; Journal Issue: 5; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; polycrystals; phonons; lead; solid solutions; carrier mobility; transport properties; thermoelectric effects; acoustic scattering; thermal conductivity; alloys

Citation Formats

Wei, Tian-Ran, Tan, Gangjian, Wu, Chao-Feng, Chang, Cheng, Zhao, Li-Dong, Li, Jing-Feng, Snyder, G. Jeffrey, and Kanatzidis, Mercouri G.. Thermoelectric transport properties of polycrystalline SnSe alloyed with PbSe. United States: N. p., 2017. Web. doi:10.1063/1.4975603.
Wei, Tian-Ran, Tan, Gangjian, Wu, Chao-Feng, Chang, Cheng, Zhao, Li-Dong, Li, Jing-Feng, Snyder, G. Jeffrey, & Kanatzidis, Mercouri G.. Thermoelectric transport properties of polycrystalline SnSe alloyed with PbSe. United States. https://doi.org/10.1063/1.4975603
Wei, Tian-Ran, Tan, Gangjian, Wu, Chao-Feng, Chang, Cheng, Zhao, Li-Dong, Li, Jing-Feng, Snyder, G. Jeffrey, and Kanatzidis, Mercouri G.. Fri . "Thermoelectric transport properties of polycrystalline SnSe alloyed with PbSe". United States. https://doi.org/10.1063/1.4975603. https://www.osti.gov/servlets/purl/1465976.
@article{osti_1465976,
title = {Thermoelectric transport properties of polycrystalline SnSe alloyed with PbSe},
author = {Wei, Tian-Ran and Tan, Gangjian and Wu, Chao-Feng and Chang, Cheng and Zhao, Li-Dong and Li, Jing-Feng and Snyder, G. Jeffrey and Kanatzidis, Mercouri G.},
abstractNote = {Single-crystal SnSe has been found to exhibit exceptional thermoelectric performance, but the efficiency of polycrystalline samples is still far from satisfactory. In this paper, with an intention to effectively suppress heat conduction and minimally affect hole transport, we alloyed p-type polycrystalline SnSe with PbSe. Single-phase Sn1-xPbxSe solid solutions were formed up to x ≈ 0.12. The lattice thermal conductivity was reduced from 1.4 to 0.85 W m-1 K-1 by 12 at. % PbSe alloying due to strain and mass fluctuations. Interestingly, the Seebeck coefficient and carrier concentration were nearly unchanged by Pb substitution, indicating a constant effective mass and an undisrupted valence band maximum. A peak figure of merit (ZT) of 0.85 at 800 K was obtained in the x = 0 sample, and relatively high performance was also achieved in solid solutions. Finally, a concise model was developed involving multiple carrier scattering mechanisms, capturing the dependence of the mobility on composition and temperature.},
doi = {10.1063/1.4975603},
journal = {Applied Physics Letters},
number = 5,
volume = 110,
place = {United States},
year = {2017},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 47 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Rationally Designing High-Performance Bulk Thermoelectric Materials
journal, August 2016


Thermoelectric transport properties of pristine and Na-doped SnSe 1−x Te x polycrystals
journal, January 2015

  • Wei, Tian-Ran; Wu, Chao-Feng; Zhang, Xiaozhi
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 44
  • DOI: 10.1039/C5CP05510E

Complex thermoelectric materials
journal, February 2008

  • Snyder, G. Jeffrey; Toberer, Eric S.
  • Nature Materials, Vol. 7, Issue 2, p. 105-114
  • DOI: 10.1038/nmat2090

Optimizing the thermoelectric performance of low-temperature SnSe compounds by electronic structure design
journal, January 2015

  • Hong, A. J.; Li, L.; Zhu, H. X.
  • Journal of Materials Chemistry A, Vol. 3, Issue 25
  • DOI: 10.1039/C5TA01703C

Strain field fluctuation effects on lattice thermal conductivity of ZrNiSn-based thermoelectric compounds
journal, August 2004

  • Yang, J.; Meisner, G. P.; Chen, L.
  • Applied Physics Letters, Vol. 85, Issue 7
  • DOI: 10.1063/1.1783022

Distinct Impact of Alkali-Ion Doping on Electrical Transport Properties of Thermoelectric p -Type Polycrystalline SnSe
journal, July 2016

  • Wei, Tian-Ran; Tan, Gangjian; Zhang, Xiaomi
  • Journal of the American Chemical Society, Vol. 138, Issue 28
  • DOI: 10.1021/jacs.6b04181

Convergence of electronic bands for high performance bulk thermoelectrics
journal, May 2011

  • Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron
  • Nature, Vol. 473, Issue 7345, p. 66-69
  • DOI: 10.1038/nature09996

Realizing High Figure of Merit in Phase-Separated Polycrystalline Sn 1– x Pb x Se
journal, October 2016

  • Tang, Guodong; Wei, Wei; Zhang, Jian
  • Journal of the American Chemical Society, Vol. 138, Issue 41
  • DOI: 10.1021/jacs.6b07010

Entropically Stabilized Local Dipole Formation in Lead Chalcogenides
journal, December 2010


Thermal Conductivity and Phonon Scattering by Magnetic Impurities in CdTe
journal, January 1964


The electrical properties of polycrystalline silicon films
journal, December 1975

  • Seto, John Y. W.
  • Journal of Applied Physics, Vol. 46, Issue 12
  • DOI: 10.1063/1.321593

Thermal Resistance due to Point Defects at High Temperatures
journal, July 1960


Alloy scattering in ternary III-V compounds
journal, June 1976


Achieving ZT=2.2 with Bi-doped n-type SnSe single crystals
journal, December 2016

  • Duong, Anh Tuan; Nguyen, Van Quang; Duvjir, Ganbat
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13713

The Pb-Sn-Se system: Phase equilibria and reactions in the PbSe-SnSe-Se subternary
journal, August 1995

  • Corso, S. Dal; Liautard, B.; Tedenac, J. C.
  • Journal of Phase Equilibria, Vol. 16, Issue 4
  • DOI: 10.1007/BF02645286

Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals
journal, April 2014

  • Zhao, Li-Dong; Lo, Shih-Han; Zhang, Yongsheng
  • Nature, Vol. 508, Issue 7496, p. 373-377
  • DOI: 10.1038/nature13184

Neutron diffraction study of the structural phase transition in SnS and SnSe
journal, January 1986

  • Chattopadhyay, T.; Pannetier, J.; Von Schnering, H. G.
  • Journal of Physics and Chemistry of Solids, Vol. 47, Issue 9, p. 879-885
  • DOI: 10.1016/0022-3697(86)90059-4

SnSe: a remarkable new thermoelectric material
journal, January 2016

  • Zhao, Li-Dong; Chang, Cheng; Tan, Gangjian
  • Energy & Environmental Science, Vol. 9, Issue 10
  • DOI: 10.1039/C6EE01755J

Phase relations between germanium, tin, and lead chalcogenides in pseudobinary systems containing orthorhombic phases
journal, April 2008


Thinking Like a Chemist: Intuition in Thermoelectric Materials
journal, April 2016

  • Zeier, Wolfgang G.; Zevalkink, Alex; Gibbs, Zachary M.
  • Angewandte Chemie International Edition, Vol. 55, Issue 24
  • DOI: 10.1002/anie.201508381

Crystal structure and phase transition of thermoelectric SnSe
journal, May 2016

  • Sist, Mattia; Zhang, Jiawei; Brummerstedt Iversen, Bo
  • Acta Crystallographica Section B Structural Science, Crystal Engineering and Materials, Vol. 72, Issue 3, p. 310-316
  • DOI: 10.1107/S2052520616003334

Assessment of the thermoelectric performance of polycrystalline p-type SnSe
journal, May 2014

  • Sassi, S.; Candolfi, C.; Vaney, J.-B.
  • Applied Physics Letters, Vol. 104, Issue 21, Article No. 212105
  • DOI: 10.1063/1.4880817

Electronic structure of tin monochalcogenides from SnO to SnTe
journal, July 1998

  • Lefebvre, I.; Szymanski, M. A.; Olivier-Fourcade, J.
  • Physical Review B, Vol. 58, Issue 4
  • DOI: 10.1103/PhysRevB.58.1896

Effect of extended strain fields on point defect phonon scattering in thermoelectric materials
journal, January 2015

  • Ortiz, Brenden R.; Peng, Haowei; Lopez, Armando
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 29
  • DOI: 10.1039/C5CP02174J

Understanding of the Extremely Low Thermal Conductivity in High-Performance Polycrystalline SnSe through Potassium Doping
journal, August 2016

  • Chen, Yue-Xing; Ge, Zhen-Hua; Yin, Meijie
  • Advanced Functional Materials, Vol. 26, Issue 37
  • DOI: 10.1002/adfm.201602652

Thermoelectric properties of p-type polycrystalline SnSe doped with Ag
journal, January 2014

  • Chen, Cheng-Lung; Wang, Heng; Chen, Yang-Yuan
  • Journal of Materials Chemistry A, Vol. 2, Issue 29, p. 11171-11176
  • DOI: 10.1039/c4ta01643b

Temperature dependent solubility of Yb in Yb–CoSb3 skutterudite and its effect on preparation, optimization and lifetime of thermoelectrics
journal, March 2015


Raising thermoelectric performance of n-type SnSe via Br doping and Pb alloying
journal, January 2016

  • Chang, Cheng; Tan, Qing; Pei, Yanling
  • RSC Advances, Vol. 6, Issue 100
  • DOI: 10.1039/C6RA21884A

The Criteria for Beneficial Disorder in Thermoelectric Solid Solutions
journal, October 2012

  • Wang, Heng; LaLonde, Aaron D.; Pei, Yanzhong
  • Advanced Functional Materials, Vol. 23, Issue 12
  • DOI: 10.1002/adfm.201201576

Studies on Thermoelectric Properties of n-type Polycrystalline SnSe 1- x S x by Iodine Doping
journal, April 2015

  • Zhang, Qian; Chere, Eyob Kebede; Sun, Jingying
  • Advanced Energy Materials, Vol. 5, Issue 12
  • DOI: 10.1002/aenm.201500360

Higher mobility in bulk semiconductors by separating the dopants from the charge-conducting band – a case study of thermoelectric PbSe
journal, January 2015

  • Wang, Heng; Cao, Xianlong; Takagiwa, Yoshiki
  • Materials Horizons, Vol. 2, Issue 3
  • DOI: 10.1039/C5MH00021A

Ultrahigh power factor and thermoelectric performance in hole-doped single-crystal SnSe
journal, November 2015


Heavily Doped p-Type PbSe with High Thermoelectric Performance: An Alternative for PbTe
journal, February 2011

  • Wang, Heng; Pei, Yanzhong; LaLonde, Aaron D.
  • Advanced Materials, Vol. 23, Issue 11, p. 1366-1370
  • DOI: 10.1002/adma.201004200

Thermal Conductivity
book, January 2004


Works referencing / citing this record:

Synergistic tuning of carrier mobility, effective mass, and point defects scattering triggered high thermoelectric performance in n -type Ge-doped PbTe
journal, February 2019

  • Wang, Zhengshang; He, Huan; Cui, Xudong
  • Journal of Applied Physics, Vol. 125, Issue 5
  • DOI: 10.1063/1.5084083

Recent progress towards high performance of tin chalcogenide thermoelectric materials
journal, January 2018

  • Li, Shan; Li, Xiaofang; Ren, Zhifeng
  • Journal of Materials Chemistry A, Vol. 6, Issue 6
  • DOI: 10.1039/c7ta09941j

Carrier tuning and multiple phonon scattering induced high thermoelectric performance in n-type Sb-doped PbTe alloys
journal, March 2019


Realizing High‐Ranged Out‐of‐Plane ZTs in N‐Type SnSe Crystals through Promoting Continuous Phase Transition
journal, June 2019

  • Chang, Cheng; Wang, Dongyang; He, Dongsheng
  • Advanced Energy Materials, Vol. 9, Issue 28
  • DOI: 10.1002/aenm.201901334

Towards the high-throughput synthesis of bulk materials: thermoelectric PbTe–PbSe–SnTe–SnSe alloys
journal, January 2019

  • Ortiz, Brenden R.; Adamczyk, Jesse M.; Gordiz, Kiarash
  • Molecular Systems Design & Engineering, Vol. 4, Issue 2
  • DOI: 10.1039/c8me00073e

Optimizing the average power factor of p-type (Na, Ag) co-doped polycrystalline SnSe
journal, January 2019

  • Wang, Si; Su, Xianli; Bailey, Trevor P.
  • RSC Advances, Vol. 9, Issue 13
  • DOI: 10.1039/c9ra00566h

Nanostructured SnSe: Synthesis, doping, and thermoelectric properties
journal, March 2018

  • Liu, Shuhao; Sun, Naikun; Liu, Mei
  • Journal of Applied Physics, Vol. 123, Issue 11
  • DOI: 10.1063/1.5018860

High‐Performance Thermoelectric SnSe: Aqueous Synthesis, Innovations, and Challenges
journal, February 2020


Fermi-surface dynamics and high thermoelectric performance along the out-of-plane direction in n-type SnSe crystals
journal, January 2020

  • Mao, Lisha; Yin, Yinong; Zhang, Qiang
  • Energy & Environmental Science, Vol. 13, Issue 2
  • DOI: 10.1039/c9ee03897c

Effects of High-Pressure High-Temperature Sintering on the Band Gap and Thermoelectric Properties of PbSe
journal, November 2017


Mg Deficiency in Grain Boundaries of n‐Type Mg 3 Sb 2 Identified by Atom Probe Tomography
journal, April 2019

  • Kuo, Jimmy Jiahong; Yu, Yuan; Kang, Stephen Dongmin
  • Advanced Materials Interfaces, Vol. 6, Issue 13
  • DOI: 10.1002/admi.201900429

Electrical Transport and Thermoelectric Properties of SnSe–SnTe Solid Solution
journal, November 2019

  • Cho, Jun-Young; Siyar, Muhammad; Jin, Woo Chan
  • Materials, Vol. 12, Issue 23
  • DOI: 10.3390/ma12233854

Thermally enhanced Fröhlich coupling in SnSe
journal, February 2019


Improved figure of merit and other thermoelectric properties of Sn 1− x Cu x Se
journal, December 2018

  • Gowthamaraju, S.; Bhobe, P. A.; Nigam, A. K.
  • Applied Physics Letters, Vol. 113, Issue 24
  • DOI: 10.1063/1.5051227

Electrical Transport and Thermoelectric Properties of SnSe–SnTe Solid Solution
journal, November 2019

  • Cho, Jun-Young; Siyar, Muhammad; Jin, Woo Chan
  • Materials, Vol. 12, Issue 23
  • DOI: 10.3390/ma12233854

Dopant-induced indirect-direct transition and semiconductor-semimetal transition of bilayer SnSe
journal, December 2019

  • Sirikumara, Hansika I.; Morshed, Mahir; Jameson, Casey
  • Journal of Applied Physics, Vol. 126, Issue 22
  • DOI: 10.1063/1.5128337