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Title: Revelation of Inherently High Mobility Enables Mg3Sb2 as a Sustainable Alternative to n-Bi2Te3 Thermoelectrics

Abstract

Over the past years, thermoelectric Mg3Sb2 alloys particularly in n-type conduction, have attracted increasing attentions for thermoelectric applications, due to the multivalley conduction band, abundance of constituents, and less toxicity. However, the high vapor pressure, causticity of Mg, and the high melting point of Mg3Sb2 tend to cause the inclusion in the materials of boundary phases and defects that affect the transport properties. In this work, a utilization of tantalum-sealing for melting enables n-type Mg3Sb2 alloys to show a substantially higher mobility than ever reported, which can be attributed to the purification of phases and to the coarse grains. Importantly, the inherently high mobility successfully enables the thermoelectric figure of merit in optimal compositions to be highly competitive to that of commercially available n-type Bi2Te3 alloys and to be higher than that of other known n-type thermoelectrics at 300-500 K. This work reveals Mg3Sb2 alloys as a top candidate for near-room-temperature thermoelectric applications.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2]; ORCiD logo [1]
  1. Interdisciplinary Materials Research CenterSchool of Materials Science and EngineeringTongji University 4800 Caoan Road Shanghai 201804 China
  2. Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley CA 94720 USA
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1560221
Alternate Identifier(s):
OSTI ID: 1560224; OSTI ID: 1560607
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Name: Advanced Science Journal Volume: 6 Journal Issue: 16; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
Germany
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Shi, Xuemin, Sun, Cheng, Bu, Zhonglin, Zhang, Xinyue, Wu, Yixuan, Lin, Siqi, Li, Wen, Faghaninia, Alireza, Jain, Anubhav, and Pei, Yanzhong. Revelation of Inherently High Mobility Enables Mg3Sb2 as a Sustainable Alternative to n-Bi2Te3 Thermoelectrics. Germany: N. p., 2019. Web. doi:10.1002/advs.201802286.
Shi, Xuemin, Sun, Cheng, Bu, Zhonglin, Zhang, Xinyue, Wu, Yixuan, Lin, Siqi, Li, Wen, Faghaninia, Alireza, Jain, Anubhav, & Pei, Yanzhong. Revelation of Inherently High Mobility Enables Mg3Sb2 as a Sustainable Alternative to n-Bi2Te3 Thermoelectrics. Germany. doi:10.1002/advs.201802286.
Shi, Xuemin, Sun, Cheng, Bu, Zhonglin, Zhang, Xinyue, Wu, Yixuan, Lin, Siqi, Li, Wen, Faghaninia, Alireza, Jain, Anubhav, and Pei, Yanzhong. Tue . "Revelation of Inherently High Mobility Enables Mg3Sb2 as a Sustainable Alternative to n-Bi2Te3 Thermoelectrics". Germany. doi:10.1002/advs.201802286.
@article{osti_1560221,
title = {Revelation of Inherently High Mobility Enables Mg3Sb2 as a Sustainable Alternative to n-Bi2Te3 Thermoelectrics},
author = {Shi, Xuemin and Sun, Cheng and Bu, Zhonglin and Zhang, Xinyue and Wu, Yixuan and Lin, Siqi and Li, Wen and Faghaninia, Alireza and Jain, Anubhav and Pei, Yanzhong},
abstractNote = {Over the past years, thermoelectric Mg3Sb2 alloys particularly in n-type conduction, have attracted increasing attentions for thermoelectric applications, due to the multivalley conduction band, abundance of constituents, and less toxicity. However, the high vapor pressure, causticity of Mg, and the high melting point of Mg3Sb2 tend to cause the inclusion in the materials of boundary phases and defects that affect the transport properties. In this work, a utilization of tantalum-sealing for melting enables n-type Mg3Sb2 alloys to show a substantially higher mobility than ever reported, which can be attributed to the purification of phases and to the coarse grains. Importantly, the inherently high mobility successfully enables the thermoelectric figure of merit in optimal compositions to be highly competitive to that of commercially available n-type Bi2Te3 alloys and to be higher than that of other known n-type thermoelectrics at 300-500 K. This work reveals Mg3Sb2 alloys as a top candidate for near-room-temperature thermoelectric applications.},
doi = {10.1002/advs.201802286},
journal = {Advanced Science},
number = 16,
volume = 6,
place = {Germany},
year = {2019},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1002/advs.201802286

Citation Metrics:
Cited by: 10 works
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Figures / Tables:

Figure 1 Figure 1: SEM images and the corresponding composition mappings by EDS taken from the polished surface (with and without HNO3-etching) of Mg3.05SbBi0.97Te0.03 pellets hot pressed using a) big pieces, and hand-ground powders b) in argon-filled glovebox and c) in air, showing an increase in oxidation but a decrease in averagemore » grain size from (a) to (c).« less

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Works referenced in this record:

Concerted Rattling in CsAg 5 Te 3 Leading to Ultralow Thermal Conductivity and High Thermoelectric Performance
journal, August 2016

  • Lin, Hua; Tan, Gangjian; Shen, Jin-Ni
  • Angewandte Chemie International Edition, Vol. 55, Issue 38
  • DOI: 10.1002/anie.201605015

Synthesis and properties of CaCd2Sb2 and EuCd2Sb2
journal, January 2010


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

Optimum Carrier Concentration in n-Type PbTe Thermoelectrics
journal, May 2014

  • Pei, Yanzhong; Gibbs, Zachary M.; Gloskovskii, Andrei
  • Advanced Energy Materials, Vol. 4, Issue 13
  • DOI: 10.1002/aenm.201400486

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

Lattice Thermal Conductivity of Disordered Semiconductor Alloys at High Temperatures
journal, September 1963


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

Enhanced thermoelectric properties of Bi2(Te1−xSex)3-based compounds as n-type legs for low-temperature power generation
journal, January 2012

  • Wang, Shanyu; Tan, Gangjian; Xie, Wenjie
  • Journal of Materials Chemistry, Vol. 22, Issue 39
  • DOI: 10.1039/c2jm34608g

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

Electronic and transport properties of zintl phase Ae Mg 2 Pn 2 , Ae  = Ca,Sr,Ba, Pn  = As,Sb,Bi in relation to Mg 3 Sb 2
journal, October 2013

  • Singh, David J.; Parker, David
  • Journal of Applied Physics, Vol. 114, Issue 14
  • DOI: 10.1063/1.4824465

Tuning bands of PbSe for better thermoelectric efficiency
journal, January 2014

  • Wang, Heng; Gibbs, Zachary M.; Takagiwa, Yoshiki
  • Energy Environ. Sci., Vol. 7, Issue 2
  • DOI: 10.1039/C3EE43438A

Designing high-performance layered thermoelectric materials through orbital engineering
journal, March 2016

  • Zhang, Jiawei; Song, Lirong; Madsen, Georg K. H.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10892

Rationalizing phonon dispersion for lattice thermal conductivity of solids
journal, September 2018

  • Chen, Zhiwei; Zhang, Xinyue; Lin, Siqi
  • National Science Review, Vol. 5, Issue 6
  • DOI: 10.1093/nsr/nwy097

Computational prediction of a high ZT of n-type Mg 3 Sb 2 -based compounds with isotropic thermoelectric conduction performance
journal, January 2018

  • Li, Juan; Zheng, Shuqi; Fang, Teng
  • Physical Chemistry Chemical Physics, Vol. 20, Issue 11
  • DOI: 10.1039/C7CP08680F

Tuning Multiscale Microstructures to Enhance Thermoelectric Performance of n-Type Bismuth-Telluride-Based Solid Solutions
journal, June 2015


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

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

Improved Thermoelectric Performance of Silver Nanoparticles-Dispersed Bi 2 Te 3 Composites Deriving from Hierarchical Two-Phased Heterostructure
journal, December 2014

  • Zhang, Qihao; Ai, Xin; Wang, Lianjun
  • Advanced Functional Materials, Vol. 25, Issue 6
  • DOI: 10.1002/adfm.201402663

Lattice Dislocations Enhancing Thermoelectric PbTe in Addition to Band Convergence
journal, April 2017


Optimizations of Pulsed Plated p and n-type Bi 2 Te 3 -Based Ternary Compounds by Annealing in Different Ambient Atmospheres
journal, August 2012

  • Schumacher, Christian; Reinsberg, Klaus G.; Rostek, Raimar
  • Advanced Energy Materials, Vol. 3, Issue 1
  • DOI: 10.1002/aenm.201200417

Simultaneous Optimization of Carrier Concentration and Alloy Scattering for Ultrahigh Performance GeTe Thermoelectrics
journal, September 2017


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


Exceptional thermoelectric performance in Mg 3 Sb 0.6 Bi 1.4 for low-grade waste heat recovery
journal, January 2019

  • Imasato, Kazuki; Kang, Stephen Dongmin; Snyder, G. Jeffrey
  • Energy & Environmental Science, Vol. 12, Issue 3
  • DOI: 10.1039/C8EE03374A

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


High thermoelectric performance in Te-free (Bi,Sb) 2 Se 3 via structural transition induced band convergence and chemical bond softening
journal, January 2016

  • Wang, Shanyu; Sun, Yongxing; Yang, Jiong
  • Energy & Environmental Science, Vol. 9, Issue 11
  • DOI: 10.1039/C6EE02674E

Single parabolic band transport in p-type EuZn 2 Sb 2 thermoelectrics
journal, January 2017

  • Wang, Xiao; Li, Wen; Wang, Chen
  • Journal of Materials Chemistry A, Vol. 5, Issue 46
  • DOI: 10.1039/C7TA08869H

Recent progress and future challenges on thermoelectric Zintl materials
journal, June 2017


Observation of room-temperature ballistic thermal conduction persisting over 8.3 µm in SiGe nanowires
journal, June 2013

  • Hsiao, Tzu-Kan; Chang, Hsu-Kai; Liou, Sz-Chian
  • Nature Nanotechnology, Vol. 8, Issue 7
  • DOI: 10.1038/nnano.2013.121

Investigation of n-type doping strategies for Mg 3 Sb 2
journal, January 2018

  • Gorai, Prashun; Ortiz, Brenden R.; Toberer, Eric S.
  • Journal of Materials Chemistry A, Vol. 6, Issue 28
  • DOI: 10.1039/C8TA03344G

Atomic Disorders Induced by Silver and Magnesium Ion Migrations Favor High Thermoelectric Performance in α-MgAgSb-Based Materials
journal, September 2015

  • Li, Dandan; Zhao, Huaizhou; Li, Shanming
  • Advanced Functional Materials, Vol. 25, Issue 41
  • DOI: 10.1002/adfm.201503022

Thermoelectric Bi 2 Te 3 -improved charge collection for high-performance dye-sensitized solar cells
journal, January 2012

  • Chen, Tao; Guai, Guan Hong; Gong, Cheng
  • Energy Environ. Sci., Vol. 5, Issue 4
  • DOI: 10.1039/C1EE02385C

Tellurium as a high-performance elemental thermoelectric
journal, January 2016

  • Lin, Siqi; Li, Wen; Chen, Zhiwei
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10287

On the electronic structure of the semiconducting compounds Mg 3 Bi 2 and Mg 3 Sb 2
journal, January 1984

  • Watson, L. M.; Marshall, C. A. W.; Cardoso, C. P.
  • Journal of Physics F: Metal Physics, Vol. 14, Issue 1
  • DOI: 10.1088/0305-4608/14/1/014

Tuning the carrier scattering mechanism to effectively improve the thermoelectric properties
journal, January 2017

  • Shuai, Jing; Mao, Jun; Song, Shaowei
  • Energy & Environmental Science, Vol. 10, Issue 3
  • DOI: 10.1039/C7EE00098G

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

Wet chemical synthesis and thermoelectric properties of V-VI one- and two-dimensional nanostructures
journal, January 2010

  • Zhang, Genqiang; Yu, Qingxuan; Li, Xiaoguang
  • Dalton Trans., Vol. 39, Issue 4
  • DOI: 10.1039/B913462J

Advanced thermoelectrics governed by a single parabolic band: Mg 2 Si 0.3 Sn 0.7 , a canonical example
journal, January 2014

  • Liu, Wei; Chi, Hang; Sun, Hui
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 15
  • DOI: 10.1039/C4CP00641K

Mg 3+ δ Sb x Bi 2− x Family: A Promising Substitute for the State-of-the-Art n-Type Thermoelectric Materials near Room Temperature
journal, December 2018

  • Shu, Rui; Zhou, Yecheng; Wang, Qi
  • Advanced Functional Materials, Vol. 29, Issue 4
  • DOI: 10.1002/adfm.201807235

High Lattice Thermal Conductivity Solids
book, January 2006

  • Morelli, Donald T.; Slack, Glen A.; Shindé, Subhash L.
  • High Thermal Conductivity Materials, p. 37-68
  • DOI: 10.1007/0-387-25100-6_2

Enhanced thermoelectric performance of Mg 2 Si 0.4 Sn 0.6 solid solutions by in nanostructures and minute Bi-doping
journal, August 2013

  • Zhang, Xin; Liu, Hongliang; Lu, Qingmei
  • Applied Physics Letters, Vol. 103, Issue 6
  • DOI: 10.1063/1.4816971

Mg Alloying in SnTe Facilitates Valence Band Convergence and Optimizes Thermoelectric Properties
journal, January 2015

  • Banik, Ananya; Shenoy, U. Sandhya; Anand, Shashwat
  • Chemistry of Materials, Vol. 27, Issue 2
  • DOI: 10.1021/cm504112m

Band engineering in Mg 3 Sb 2 by alloying with Mg 3 Bi 2 for enhanced thermoelectric performance
journal, January 2018

  • Imasato, Kazuki; Kang, Stephen Dongmin; Ohno, Saneyuki
  • Materials Horizons, Vol. 5, Issue 1
  • DOI: 10.1039/C7MH00865A

Anomalous electrical conductivity of n-type Te-doped Mg3.2Sb1.5Bi0.5
journal, December 2017


Band Degeneracy, Low Thermal Conductivity, and High Thermoelectric Figure of Merit in SnTe–CaTe Alloys
journal, December 2015


An Unlikely Route to Low Lattice Thermal Conductivity: Small Atoms in a Simple Layered Structure
journal, September 2018


Phase Boundary Mapping to Obtain n-type Mg3Sb2-Based Thermoelectrics
journal, January 2018


Advances in Thermoelectric Mg 3 Sb 2 and Its Derivatives
journal, July 2018


Effect of Point Imperfections on Lattice Thermal Conductivity
journal, November 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

Low Sound Velocity Contributing to the High Thermoelectric Performance of Ag 8 SnSe 6
journal, July 2016


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

Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics
journal, April 2015


Broad temperature plateau for thermoelectric figure of merit ZT>2 in phase-separated PbTe0.7S0.3
journal, July 2014

  • Wu, H. J.; Zhao, L. -D.; Zheng, F. S.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5515

Cubic AgPbmSbTe2+m: Bulk Thermoelectric Materials with High Figure of Merit
journal, February 2004


Band and scattering tuning for high performance thermoelectric Sn1−xMnxTe alloys
journal, December 2015


Enhancement of average thermoelectric figure of merit by increasing the grain-size of Mg 3.2 Sb 1.5 Bi 0.49 Te 0.01
journal, January 2018

  • Kanno, Tsutomu; Tamaki, Hiromasa; Sato, Hiroki K.
  • Applied Physics Letters, Vol. 112, Issue 3
  • DOI: 10.1063/1.5016488

Intrinsically Minimal Thermal Conductivity in Cubic IVVI2 Semiconductors
journal, July 2008


Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics
journal, January 2017

  • Chen, Zhiwei; Ge, Binghui; Li, Wen
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms13828

Synthesis and characterization of the divalent samarium Zintl-phases SmMg2Bi2 and SmMg2Sb2
journal, November 2015


Significant Role of Mg Stoichiometry in Designing High Thermoelectric Performance for Mg 3 (Sb,Bi) 2 -Based n-Type Zintls
journal, January 2018

  • Shuai, Jing; Ge, Binghui; Mao, Jun
  • Journal of the American Chemical Society, Vol. 140, Issue 5
  • DOI: 10.1021/jacs.7b12767

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

Electronic origin of the high thermoelectric performance of GeTe among the p-type group IV monotellurides
journal, March 2017

  • Li, Juan; Chen, Zhiwei; Zhang, Xinyue
  • NPG Asia Materials, Vol. 9, Issue 3
  • DOI: 10.1038/am.2017.8

High-Performance Low-Cost n-Type Se-Doped Mg 3 Sb 2 -Based Zintl Compounds for Thermoelectric Application
journal, May 2017


Thermoelectric properties and microstructure of Mg3Sb2
journal, August 2006

  • Condron, Cathie L.; Kauzlarich, Susan M.; Gascoin, Franck
  • Journal of Solid State Chemistry, Vol. 179, Issue 8
  • DOI: 10.1016/j.jssc.2006.01.034

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


Effective dopants in p-type elementary Te thermoelectrics
journal, January 2017


Hierarchical Chemical Bonds Contributing to the Intrinsically Low Thermal Conductivity in α-MgAgSb Thermoelectric Materials
journal, October 2016

  • Ying, Pingjun; Li, Xin; Wang, Yancheng
  • Advanced Functional Materials, Vol. 27, Issue 1
  • DOI: 10.1002/adfm.201604145

Interstitial Defects Improving Thermoelectric SnTe in Addition to Band Convergence
journal, February 2017


Realizing the High Thermoelectric Performance of GeTe by Sb-Doping and Se-Alloying
journal, December 2016


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


Copper ion liquid-like thermoelectrics
journal, March 2012

  • Liu, Huili; Shi, Xun; Xu, Fangfang
  • Nature Materials, Vol. 11, Issue 5, p. 422-425
  • DOI: 10.1038/nmat3273

Boosting the thermoelectric performance of PbSe through dynamic doping and hierarchical phonon scattering
journal, January 2018

  • You, Li; Liu, Yefeng; Li, Xin
  • Energy & Environmental Science, Vol. 11, Issue 7
  • DOI: 10.1039/C8EE00418H

New Insight on Tuning Electrical Transport Properties via Chalcogen Doping in n-type Mg 3 Sb 2 -Based Thermoelectric Materials
journal, February 2018

  • Zhang, Jiawei; Song, Lirong; Borup, Kasper Andersen
  • Advanced Energy Materials, Vol. 8, Issue 16
  • DOI: 10.1002/aenm.201702776

Grain boundary dominated charge transport in Mg 3 Sb 2 -based compounds
journal, January 2018

  • Kuo, Jimmy Jiahong; Kang, Stephen Dongmin; Imasato, Kazuki
  • Energy & Environmental Science, Vol. 11, Issue 2
  • DOI: 10.1039/C7EE03326E

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

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