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Title: New insight into the material parameter B to understand the enhanced thermoelectric performance of Mg 2Sn 1-x-yGe xSb y

Abstract

Historically, a material parameter B incorporating weighted mobility and lattice thermal conductivity has guided the exploration of novel thermoelectric materials. However, the conventional definition of B neglects the bipolar effect which can dramatically change the thermoelectric energy conversion efficiency at high temperatures. A generalized material parameter B* is derived, which connects weighted mobility, lattice thermal conductivity, and the band gap. Based on the new parameter B*, we explain the successful tuning of the electron and phonon transport in Mg 2Sn 1-x-yGe xSb y, with an improved ZT value from 0.6 in Mg 2Sn 0.99Sb 0.01 to 1.4 in Mg 2Sn 0.73Ge 0.25Sb 0.02. We uncover that the Ge alloying approach simultaneously improves all the key variables in the material parameter B*, with an ~25% enhancement in the weighted mobility, ~27% band gap widening, and ~50% reduction in the lattice thermal conductivity. We show that a higher generalized parameter B* leads to a higher optimized ZT in Mg 2Sn 0.73Ge 0.25Sb 0.02, and some common thermoelectric materials. The new parameter B* provides a better characterization of material's thermoelectric transport, particularly at high temperatures, and therefore can facilitate the search for good thermoelectric materials.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [2];  [1]
  1. Univ. of Houston, TX (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1371019
Grant/Contract Number:  
SC0001299; FG02-09ER46577
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Liu, Weishu, Zhou, Jiawei, Jie, Qing, Li, Yang, Kim, Hee Seok, Bao, Jiming, Chen, Gang, and Ren, Zhifeng. New insight into the material parameter B to understand the enhanced thermoelectric performance of Mg2Sn1-x-yGexSby. United States: N. p., 2015. Web. doi:10.1039/C5EE02600H.
Liu, Weishu, Zhou, Jiawei, Jie, Qing, Li, Yang, Kim, Hee Seok, Bao, Jiming, Chen, Gang, & Ren, Zhifeng. New insight into the material parameter B to understand the enhanced thermoelectric performance of Mg2Sn1-x-yGexSby. United States. doi:10.1039/C5EE02600H.
Liu, Weishu, Zhou, Jiawei, Jie, Qing, Li, Yang, Kim, Hee Seok, Bao, Jiming, Chen, Gang, and Ren, Zhifeng. Thu . "New insight into the material parameter B to understand the enhanced thermoelectric performance of Mg2Sn1-x-yGexSby". United States. doi:10.1039/C5EE02600H. https://www.osti.gov/servlets/purl/1371019.
@article{osti_1371019,
title = {New insight into the material parameter B to understand the enhanced thermoelectric performance of Mg2Sn1-x-yGexSby},
author = {Liu, Weishu and Zhou, Jiawei and Jie, Qing and Li, Yang and Kim, Hee Seok and Bao, Jiming and Chen, Gang and Ren, Zhifeng},
abstractNote = {Historically, a material parameter B incorporating weighted mobility and lattice thermal conductivity has guided the exploration of novel thermoelectric materials. However, the conventional definition of B neglects the bipolar effect which can dramatically change the thermoelectric energy conversion efficiency at high temperatures. A generalized material parameter B* is derived, which connects weighted mobility, lattice thermal conductivity, and the band gap. Based on the new parameter B*, we explain the successful tuning of the electron and phonon transport in Mg2Sn1-x-yGexSby, with an improved ZT value from 0.6 in Mg2Sn0.99Sb0.01 to 1.4 in Mg2Sn0.73Ge0.25Sb0.02. We uncover that the Ge alloying approach simultaneously improves all the key variables in the material parameter B*, with an ~25% enhancement in the weighted mobility, ~27% band gap widening, and ~50% reduction in the lattice thermal conductivity. We show that a higher generalized parameter B* leads to a higher optimized ZT in Mg2Sn0.73Ge0.25Sb0.02, and some common thermoelectric materials. The new parameter B* provides a better characterization of material's thermoelectric transport, particularly at high temperatures, and therefore can facilitate the search for good thermoelectric materials.},
doi = {10.1039/C5EE02600H},
journal = {Energy & Environmental Science},
number = 2,
volume = 9,
place = {United States},
year = {2015},
month = {11}
}

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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Power Factor Enhancement by Modulation Doping in Bulk Nanocomposites
journal, June 2011

  • Zebarjadi, Mona; Joshi, Giri; Zhu, Gaohua
  • Nano Letters, Vol. 11, Issue 6
  • DOI: 10.1021/nl201206d

Optimum band gap of a thermoelectric material
journal, February 1994


Improvement of Thermoelectric Performance of CoSb 3− x Te x Skutterudite Compounds by Additional Substitution of IVB-Group Elements for Sb
journal, December 2008

  • Liu, Wei-Shu; Zhang, Bo-Ping; Zhao, Li-Dong
  • Chemistry of Materials, Vol. 20, Issue 24
  • DOI: 10.1021/cm802367f

Raising the Thermoelectric Performance of p-Type PbS with Endotaxial Nanostructuring and Valence-Band Offset Engineering Using CdS and ZnS
journal, September 2012

  • Zhao, Li-Dong; He, Jiaqing; Hao, Shiqiang
  • Journal of the American Chemical Society, Vol. 134, Issue 39
  • DOI: 10.1021/ja306527n

Infrared Absorption of Magnesium Stannide
journal, February 1964


Effect of Silicon and Sodium on Thermoelectric Properties of Thallium-Doped Lead Telluride-Based Materials
journal, April 2012

  • Zhang, Qinyong; Wang, Hengzhi; Zhang, Qian
  • Nano Letters, Vol. 12, Issue 5
  • DOI: 10.1021/nl3002183

Highly effective Mg 2 Si 1 x Sn x thermoelectrics
journal, July 2006


Nanostructured Thermoelectrics: Big Efficiency Gains from Small Features
journal, July 2010

  • Vineis, Christopher J.; Shakouri, Ali; Majumdar, Arun
  • Advanced Materials, Vol. 22, Issue 36, p. 3970-3980
  • DOI: 10.1002/adma.201000839

Principles of thermoelectric devices
journal, June 1960


Low Electron Scattering Potentials in High Performance Mg 2 Si 0.45 Sn 0.55 Based Thermoelectric Solid Solutions with Band Convergence
journal, April 2013

  • Liu, Xiaohua; Zhu, Tiejun; Wang, Heng
  • Advanced Energy Materials, Vol. 3, Issue 9
  • DOI: 10.1002/aenm.201300174

Thermoelectric Property Studies on Cu-Doped n-type CuxBi2Te2.7Se0.3 Nanocomposites
journal, June 2011

  • Liu, Wei-Shu; Zhang, Qinyong; Lan, Yucheng
  • Advanced Energy Materials, Vol. 1, Issue 4, p. 577-587
  • DOI: 10.1002/aenm.201100149

The Thermoelectric Figure of Merit and its Relation to Thermoelectric Generators†
journal, July 1959


All-scale hierarchical thermoelectrics: MgTe in PbTe facilitates valence band convergence and suppresses bipolar thermal transport for high performance
journal, January 2013

  • Zhao, L. D.; Wu, H. J.; Hao, S. Q.
  • Energy & Environmental Science, Vol. 6, Issue 11
  • DOI: 10.1039/c3ee42187b

Enhanced Thermoelectric Figure of Merit of p-Type Half-Heuslers
journal, February 2011

  • Yan, Xiao; Joshi, Giri; Liu, Weishu
  • Nano Letters, Vol. 11, Issue 2
  • DOI: 10.1021/nl104138t

High thermoelectric performance by resonant dopant indium in nanostructured SnTe
journal, July 2013

  • Zhang, Q.; Liao, B.; Lan, Y.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 33, p. 13261-13266
  • DOI: 10.1073/pnas.1305735110

Estimation of the thermal band gap of a semiconductor from seebeck measurements
journal, July 1999


Recent advances in thermoelectric nanocomposites
journal, January 2012


Materials for thermoelectric energy conversion
journal, April 1988


Enhancement of thermoelectric figure-of-merit by resonant states of aluminium doping in lead selenide
journal, January 2012

  • Zhang, Qinyong; Wang, Hui; Liu, Weishu
  • Energy Environ. Sci., Vol. 5, Issue 1, p. 5246-5251
  • DOI: 10.1039/C1EE02465E

Thermoelectric Figure of Merit of Two‐Band Semiconductors
journal, May 1962


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

Synthesis of Mg2Si1−xSnx solid solutions as thermoelectric materials by bulk mechanical alloying and hot pressing
journal, January 2007


n-type thermoelectric material Mg 2 Sn 0.75 Ge 0.25 for high power generation
journal, March 2015

  • Liu, Weishu; Kim, Hee Seok; Chen, Shuo
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 11
  • DOI: 10.1073/pnas.1424388112

Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States
journal, July 2008

  • Heremans, J. P.; Jovovic, V.; Toberer, E. S.
  • Science, Vol. 321, Issue 5888, p. 554-557
  • DOI: 10.1126/science.1159725

Thermoelectric properties of highly efficient Bi-doped Mg 2 Si 1− x−y Sn x Ge y materials
journal, September 2014


Band engineering of high performance p-type FeNbSb based half-Heusler thermoelectric materials for figure of merit zT > 1
journal, January 2015

  • Fu, Chenguang; Zhu, Tiejun; Liu, Yintu
  • Energy & Environmental Science, Vol. 8, Issue 1
  • DOI: 10.1039/C4EE03042G

Convergence of Conduction Bands as a Means of Enhancing Thermoelectric Performance of n -Type Mg 2 Si 1 x Sn x Solid Solutions
journal, April 2012


First-principles simulation of electron mean-free-path spectra and thermoelectric properties in silicon
journal, March 2015


Kramers-Kronig analysis of reflection data
journal, August 1965


Optical Properties of Mg 2 Si, Mg 2 Ge, and Mg 2 Sn from 0.6 to 11.0 eV at 77°K
journal, February 1969


Enhanced thermoelectric properties in CoSb3-xTex alloys prepared by mechanical alloying and spark plasma sintering
journal, November 2007

  • Liu, Wei-Shu; Zhang, Bo-Ping; Li, Jing-Feng
  • Journal of Applied Physics, Vol. 102, Issue 10
  • DOI: 10.1063/1.2815671

Suppressing the bipolar contribution to the thermoelectric properties of Mg 2 Si 0.4 Sn 0.6 by Ge substitution
journal, April 2015

  • Zhang, Libin; Xiao, Penghao; Shi, Li
  • Journal of Applied Physics, Vol. 117, Issue 15
  • DOI: 10.1063/1.4918311

In situ synthesis and thermoelectric properties of La-doped Mg 2 (Si, Sn) composites
journal, August 2008


Thermoelectricity
journal, January 1984

  • Tuomi, Donald
  • Journal of The Electrochemical Society, Vol. 131, Issue 9
  • DOI: 10.1149/1.2116027

Accurate Band Gaps of Semiconductors and Insulators with a Semilocal Exchange-Correlation Potential
journal, June 2009


Enhanced thermoelectric property originating from additional carrier pocket in skutterudite compounds
journal, July 2008

  • Liu, Wei-Shu; Zhao, Li-Dong; Zhang, Bo-Ping
  • Applied Physics Letters, Vol. 93, Issue 4
  • DOI: 10.1063/1.2965123

Phonon conduction in PbSe, PbTe, and PbTe 1 x Se x from first-principles calculations
journal, May 2012


Figure of merit for thermoelectrics
journal, February 1989

  • Mahan, G. D.
  • Journal of Applied Physics, Vol. 65, Issue 4
  • DOI: 10.1063/1.342976

High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys
journal, May 2008


Doping and temperature dependence of thermoelectric properties in Mg 2 (Si,Sn)
journal, October 2012


High-performance nanostructured thermoelectric materials
journal, October 2010


Importance of relativistic effects in electronic structure and thermopower calculations for Mg 2 Si , Mg 2 Ge , and Mg 2 Sn
journal, March 2014