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

Title: Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials

Abstract

Thermoelectric modules, consisting of multiple pairs of n- and p-type legs, enable converting heat into electricity and vice versa. However, the thermoelectric performance is often asymmetrical, in that one type outperforms the other. In this paper, we identified the relationship between the asymmetrical thermoelectric performance and the weighted mobility ratio, a correlation that can help predict the thermoelectric performance of unreported materials. Here, a reasonably high ZT for the n-type ZrCoBi-based half-Heuslers is first predicted and then experimentally verified. A high peak ZT of ~1 at 973 K can be realized by ZrCo0.9Ni0.1Bi0.85Sb0.15. The measured heat-to-electricity conversion efficiency for the unicouple of ZrCoBi-based materials can be as high as ~10% at the cold-side temperature of ~303 K and at the hot-side temperature of ~983 K. Our work demonstrates that the ZrCoBi-based half-Heuslers are highly promising for the application of mid- and high-temperature thermoelectric power generation.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [3];  [1];  [1]; ORCiD logo [3];  [4]; ORCiD logo [1]
  1. Univ. of Houston, TX (United States)
  2. Univ. of Missouri, Columbia, MO (United States); Chinese Academy of Sciences (CAS), Hefei (China); Univ. of Science and Technology of China, Hefei (China)
  3. Univ. of Missouri, Columbia, MO (United States)
  4. Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Research Org.:
Univ. of Missouri, Columbia, MO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1613120
Grant/Contract Number:  
SC0019114; 11474329
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 5; Journal Issue: 6; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zhu, Hangtian, Mao, Jun, Feng, Zhenzhen, Sun, Jifeng, Zhu, Qing, Liu, Zihang, Singh, David J., Wang, Yumei, and Ren, Zhifeng. Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials. United States: N. p., 2019. Web. doi:10.1126/sciadv.aav5813.
Zhu, Hangtian, Mao, Jun, Feng, Zhenzhen, Sun, Jifeng, Zhu, Qing, Liu, Zihang, Singh, David J., Wang, Yumei, & Ren, Zhifeng. Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials. United States. https://doi.org/10.1126/sciadv.aav5813
Zhu, Hangtian, Mao, Jun, Feng, Zhenzhen, Sun, Jifeng, Zhu, Qing, Liu, Zihang, Singh, David J., Wang, Yumei, and Ren, Zhifeng. Fri . "Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials". United States. https://doi.org/10.1126/sciadv.aav5813. https://www.osti.gov/servlets/purl/1613120.
@article{osti_1613120,
title = {Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials},
author = {Zhu, Hangtian and Mao, Jun and Feng, Zhenzhen and Sun, Jifeng and Zhu, Qing and Liu, Zihang and Singh, David J. and Wang, Yumei and Ren, Zhifeng},
abstractNote = {Thermoelectric modules, consisting of multiple pairs of n- and p-type legs, enable converting heat into electricity and vice versa. However, the thermoelectric performance is often asymmetrical, in that one type outperforms the other. In this paper, we identified the relationship between the asymmetrical thermoelectric performance and the weighted mobility ratio, a correlation that can help predict the thermoelectric performance of unreported materials. Here, a reasonably high ZT for the n-type ZrCoBi-based half-Heuslers is first predicted and then experimentally verified. A high peak ZT of ~1 at 973 K can be realized by ZrCo0.9Ni0.1Bi0.85Sb0.15. The measured heat-to-electricity conversion efficiency for the unicouple of ZrCoBi-based materials can be as high as ~10% at the cold-side temperature of ~303 K and at the hot-side temperature of ~983 K. Our work demonstrates that the ZrCoBi-based half-Heuslers are highly promising for the application of mid- and high-temperature thermoelectric power generation.},
doi = {10.1126/sciadv.aav5813},
journal = {Science Advances},
number = 6,
volume = 5,
place = {United States},
year = {Fri Jun 21 00:00:00 EDT 2019},
month = {Fri Jun 21 00:00:00 EDT 2019}
}

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

Citation Metrics:
Cited by: 43 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Realizing high figure of merit in heavy-band p-type half-Heusler thermoelectric materials
journal, September 2015

  • Fu, Chenguang; Bai, Shengqiang; Liu, Yintu
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9144

Thermoelectric properties of materials near the band crossing line in Mg2Sn–Mg2Ge–Mg2Si system
journal, January 2016


Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe
journal, August 2015

  • Tan, Gangjian; Shi, Fengyuan; Hao, Shiqiang
  • Journal of the American Chemical Society, Vol. 137, Issue 35
  • DOI: 10.1021/jacs.5b07284

Low effective mass leading to high thermoelectric performance
journal, January 2012

  • Pei, Yanzhong; LaLonde, Aaron D.; Wang, Heng
  • Energy & Environmental Science, Vol. 5, Issue 7
  • DOI: 10.1039/c2ee21536e

Manipulation of ionized impurity scattering for achieving high thermoelectric performance in n-type Mg 3 Sb 2 -based materials
journal, September 2017

  • Mao, Jun; Shuai, Jing; Song, Shaowei
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 40
  • DOI: 10.1073/pnas.1711725114

Enhanced Thermoelectric Figure-of-Merit in Nanostructured p-type Silicon Germanium Bulk Alloys
journal, December 2008

  • Joshi, Giri; Lee, Hohyun; Lan, Yucheng
  • Nano Letters, Vol. 8, Issue 12
  • DOI: 10.1021/nl8026795

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

Low-Symmetry Rhombohedral GeTe Thermoelectrics
journal, May 2018


Multiple-Filled Skutterudites: High Thermoelectric Figure of Merit through Separately Optimizing Electrical and Thermal Transports
journal, May 2011

  • Shi, Xun; Yang, Jiong; Salvador, James R.
  • Journal of the American Chemical Society, Vol. 133, Issue 20
  • DOI: 10.1021/ja111199y

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

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

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

Achieving high power factor and output power density in p-type half-Heuslers Nb 1-x Ti x FeSb
journal, November 2016

  • He, Ran; Kraemer, Daniel; Mao, Jun
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 48
  • DOI: 10.1073/pnas.1617663113

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


New trends, strategies and opportunities in thermoelectric materials: A perspective
journal, June 2017


Material Design Considerations Based on Thermoelectric Quality Factor
book, January 2013


Discovery of ZrCoBi based half Heuslers with high thermoelectric conversion efficiency
journal, June 2018


Enhanced thermoelectric figure of merit in nanostructured n-type silicon germanium bulk alloy
journal, November 2008

  • Wang, X. W.; Lee, H.; Lan, Y. C.
  • Applied Physics Letters, Vol. 93, Issue 19
  • DOI: 10.1063/1.3027060

Improved thermoelectric performance of n-type half-Heusler MCo1-xNixSb (M = Hf, Zr)
journal, June 2017


Filled Skutterudite Antimonides: A New Class of Thermoelectric Materials
journal, May 1996


Discovery of TaFeSb-based half-Heuslers with high thermoelectric performance
journal, January 2019


Advances in thermoelectrics
journal, April 2018


Effect of Hf Concentration on Thermoelectric Properties of Nanostructured N-Type Half-Heusler Materials Hf x Zr 1-x NiSn 0.99 Sb 0.01
journal, May 2013

  • Chen, Shuo; Lukas, Kevin C.; Liu, Weishu
  • Advanced Energy Materials, Vol. 3, Issue 9
  • DOI: 10.1002/aenm.201300336

Thermoelectrics with Earth Abundant Elements: High Performance p-type PbS Nanostructured with SrS and CaS
journal, April 2012

  • Zhao, Li-Dong; He, Jiaqing; Wu, Chun-I
  • Journal of the American Chemical Society, Vol. 134, Issue 18
  • DOI: 10.1021/ja301772w

Weak electron-phonon coupling contributing to high thermoelectric performance in n-type PbSe
journal, May 2012

  • Wang, H.; Pei, Y.; LaLonde, A. D.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 25
  • DOI: 10.1073/pnas.1111419109

Enhanced thermoelectric properties of n-type NbCoSn half-Heusler by improving phase purity
journal, October 2016

  • He, Ran; Huang, Lihong; Wang, Yumei
  • APL Materials, Vol. 4, Issue 10
  • DOI: 10.1063/1.4952994

Stabilizing the Optimal Carrier Concentration for High Thermoelectric Efficiency
journal, November 2011

  • Pei, Yanzhong; LaLonde, Aaron D.; Heinz, Nicholas A.
  • Advanced Materials, Vol. 23, Issue 47
  • DOI: 10.1002/adma.201103153

Discovery of high-performance low-cost n-type Mg3Sb2-based thermoelectric materials with multi-valley conduction bands
journal, January 2017

  • Zhang, Jiawei; Song, Lirong; Pedersen, Steffen Hindborg
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms13901

Lanthanide Contraction as a Design Factor for High-Performance Half-Heusler Thermoelectric Materials
journal, June 2018


Cooling, Heating, Generating Power, and Recovering Waste Heat with Thermoelectric Systems
journal, September 2008


Controlling Metallurgical Phase Separation Reactions of the Ge 0.87 Pb 0.13 Te Alloy for High Thermoelectric Performance
journal, March 2013

  • Gelbstein, Yaniv; Davidow, Joseph; Girard, Steven N.
  • Advanced Energy Materials, Vol. 3, Issue 6
  • DOI: 10.1002/aenm.201200970

Preparation and thermoelectric properties of semiconducting Zn4Sb3
journal, July 1997

  • Caillat, T.; Fleurial, J. -P.; Borshchevsky, A.
  • Journal of Physics and Chemistry of Solids, Vol. 58, Issue 7
  • DOI: 10.1016/S0022-3697(96)00228-4

Deep defect level engineering: a strategy of optimizing the carrier concentration for high thermoelectric performance
journal, January 2018

  • Zhang, Qian; Song, Qichen; Wang, Xinyu
  • Energy & Environmental Science, Vol. 11, Issue 4
  • DOI: 10.1039/C8EE00112J

High thermoelectric performance of MgAgSb-based materials
journal, July 2014


Isotropic Conduction Network and Defect Chemistry in Mg 3+ δ Sb 2 -Based Layered Zintl Compounds with High Thermoelectric Performance
journal, September 2016

  • Tamaki, Hiromasa; Sato, Hiroki K.; Kanno, Tsutomu
  • Advanced Materials, Vol. 28, Issue 46
  • DOI: 10.1002/adma.201603955

Phase-transition temperature suppression to achieve cubic GeTe and high thermoelectric performance by Bi and Mn codoping
journal, May 2018

  • Liu, Zihang; Sun, Jifeng; Mao, Jun
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 21
  • DOI: 10.1073/pnas.1802020115

Defect-Controlled Electronic Properties in A Zn 2 Sb 2 Zintl Phases
journal, February 2014

  • Pomrehn, Gregory S.; Zevalkink, Alex; Zeier, Wolfgang G.
  • Angewandte Chemie International Edition, Vol. 53, Issue 13
  • DOI: 10.1002/anie.201311125

High thermoelectric performance of α-MgAgSb for power generation
journal, January 2018

  • Liu, Zihang; Mao, Jun; Sui, Jiehe
  • Energy & Environmental Science, Vol. 11, Issue 1
  • DOI: 10.1039/C7EE02504A

Defect Engineering for Realizing High Thermoelectric Performance in n-Type Mg 3 Sb 2 -Based Materials
journal, September 2017


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


Low effective mass and carrier concentration optimization for high performance p-type Mg 2(1−x) Li 2x Si 0.3 Sn 0.7 solid solutions
journal, January 2014

  • Zhang, Qiang; Cheng, Long; Liu, Wei
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 43
  • DOI: 10.1039/C4CP03468F

Lithium Doping to Enhance Thermoelectric Performance of MgAgSb with Weak Electron-Phonon Coupling
journal, January 2016


Point Defect Engineering of High-Performance Bismuth-Telluride-Based Thermoelectric Materials
journal, June 2014

  • Hu, Lipeng; Zhu, Tiejun; Liu, Xiaohua
  • Advanced Functional Materials, Vol. 24, Issue 33
  • DOI: 10.1002/adfm.201400474

Electronic fitness function for screening semiconductors as thermoelectric materials
journal, November 2017


Electronic structure calculations of solids using the WIEN2k package for material sciences
journal, August 2002


Defect-Controlled Electronic Properties in A Zn 2 Sb 2 Zintl Phases
journal, February 2014

  • Pomrehn, Gregory S.; Zevalkink, Alex; Zeier, Wolfgang G.
  • Angewandte Chemie, Vol. 126, Issue 13
  • DOI: 10.1002/ange.201311125

Multiple-Filled Skutterudites: High Thermoelectric Figure of Merit through Separately Optimizing Electrical and Thermal Transports
journal, January 2012

  • Shi, Xun; Yang, Jiong; Salvador, James R.
  • Journal of the American Chemical Society, Vol. 134, Issue 5
  • DOI: 10.1021/ja211185w

Complex thermoelectric materials
book, October 2010


Stabilizing the Optimal Carrier Concentration for High Thermoelectric Efficiency
journal, November 2011

  • Pei, Yanzhong; LaLonde, Aaron D.; Heinz, Nicholas A.
  • Advanced Materials, Vol. 23, Issue 47
  • DOI: 10.1002/adma.201103153

Multiple-Filled Skutterudites: High Thermoelectric Figure of Merit through Separately Optimizing Electrical and Thermal Transports
journal, January 2012

  • Shi, Xun; Yang, Jiong; Salvador, James R.
  • Journal of the American Chemical Society, Vol. 134, Issue 5
  • DOI: 10.1021/ja211185w

Thermoelectrics with Earth Abundant Elements: High Performance p-type PbS Nanostructured with SrS and CaS
journal, April 2012

  • Zhao, Li-Dong; He, Jiaqing; Wu, Chun-I
  • Journal of the American Chemical Society, Vol. 134, Issue 18
  • DOI: 10.1021/ja301772w

Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe
journal, August 2015

  • Tan, Gangjian; Shi, Fengyuan; Hao, Shiqiang
  • Journal of the American Chemical Society, Vol. 137, Issue 35
  • DOI: 10.1021/jacs.5b07284

Enhanced Thermoelectric Figure-of-Merit in Nanostructured p-type Silicon Germanium Bulk Alloys
journal, December 2008

  • Joshi, Giri; Lee, Hohyun; Lan, Yucheng
  • Nano Letters, Vol. 8, Issue 12
  • DOI: 10.1021/nl8026795

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

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

Discovery of ZrCoBi based half Heuslers with high thermoelectric conversion efficiency
journal, June 2018


Discovery of TaFeSb-based half-Heuslers with high thermoelectric performance
journal, January 2019


Weak electron-phonon coupling contributing to high thermoelectric performance in n-type PbSe
journal, May 2012

  • Wang, H.; Pei, Y.; LaLonde, A. D.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 25
  • DOI: 10.1073/pnas.1111419109

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

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

Phase-transition temperature suppression to achieve cubic GeTe and high thermoelectric performance by Bi and Mn codoping
journal, May 2018

  • Liu, Zihang; Sun, Jifeng; Mao, Jun
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 21
  • DOI: 10.1073/pnas.1802020115

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


Filled Skutterudite Antimonides: A New Class of Thermoelectric Materials
journal, May 1996


Works referencing / citing this record:

Characterization of rattling in relation to thermal conductivity: Ordered half-Heusler semiconductors
journal, February 2020