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Title: Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe

Abstract

Herein we demonstrate a high solubility limit of >9 mol% for MnTe alloying in SnTe. The electrical conductivity of SnTe decreases gradually while the Seebeck coefficient increases remarkably with increasing MnTe content, leading to enhanced power factors. The room-temperature Seebeck coefficients of Mn-doped SnTe are significantly higher than those predicted by theoretical Pisarenko plots for pure SnTe, indicating a modified band structure. The high-temperature Hall data of Sn1–xMnxTe show strong temperature dependence, suggestive of a two-valence-band conduction behavior. Moreover, the peak temperature of the Hall plot of Sn1–xMnxTe shifts toward lower temperature as MnTe content is increased, which is clear evidence of decreased energy separation (band convergence) between the two valence bands. The first-principles electronic structure calculations based on density functional theory also support this point. The higher doping fraction (>9%) of Mn in comparison with ~3% for Cd and Hg in SnTe gives rise to a much better valence band convergence that is responsible for the observed highest Seebeck coefficient of ~230 μV/K at 900 K. The high doping fraction of Mn in SnTe also creates stronger point defect scattering, which when combined with ubiquitous endotaxial MnTe nanostructures when the solubility of Mn is exceeded scatters a wide spectrummore » of phonons for a low lattice thermal conductivity of 0.9 W m–1 K–1 at 800 K. The synergistic role that Mn plays in regulating the electron and phonon transport of SnTe yields a high thermoelectric figure of merit of 1.3 at 900 K.« less

Authors:
 [1];  [1];  [1];  [2];  [2];  [3];  [2];  [1];  [1];  [4]
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  1. Northwestern Univ., Evanston, IL (United States)
  2. Univ. of Michigan, Ann Arbor, MI (United States)
  3. Beihang Univ., Beijing (China)
  4. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC); Michigan State Univ., East Lansing, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1370358
Grant/Contract Number:  
SC0001054
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 35; Related Information: RMSSEC partners with Michigan State University (lead); University of California, Los Angeles; University of Michigan; Northwestern University; Oak Ridge National Laboratory; Ohio State University; Wayne State University; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thermal conductivity; Alloying; Thermodynamic modeling; Lattices; Transition metals

Citation Formats

Tan, Gangjian, Shi, Fengyuan, Hao, Shiqiang, Chi, Hang, Bailey, Trevor P., Zhao, Li-Dong, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., and Kanatzidis, Mercouri G. Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe. United States: N. p., 2015. Web. doi:10.1021/jacs.5b07284.
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Tan, Gangjian, Shi, Fengyuan, Hao, Shiqiang, Chi, Hang, Bailey, Trevor P., Zhao, Li-Dong, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., & Kanatzidis, Mercouri G. Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe. United States. https://doi.org/10.1021/jacs.5b07284
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Tan, Gangjian, Shi, Fengyuan, Hao, Shiqiang, Chi, Hang, Bailey, Trevor P., Zhao, Li-Dong, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., and Kanatzidis, Mercouri G. Wed . "Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe". United States. https://doi.org/10.1021/jacs.5b07284. https://www.osti.gov/servlets/purl/1370358.
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@article{osti_1370358,
title = {Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe},
author = {Tan, Gangjian and Shi, Fengyuan and Hao, Shiqiang and Chi, Hang and Bailey, Trevor P. and Zhao, Li-Dong and Uher, Ctirad and Wolverton, Chris and Dravid, Vinayak P. and Kanatzidis, Mercouri G.},
abstractNote = {Herein we demonstrate a high solubility limit of >9 mol% for MnTe alloying in SnTe. The electrical conductivity of SnTe decreases gradually while the Seebeck coefficient increases remarkably with increasing MnTe content, leading to enhanced power factors. The room-temperature Seebeck coefficients of Mn-doped SnTe are significantly higher than those predicted by theoretical Pisarenko plots for pure SnTe, indicating a modified band structure. The high-temperature Hall data of Sn1–xMnxTe show strong temperature dependence, suggestive of a two-valence-band conduction behavior. Moreover, the peak temperature of the Hall plot of Sn1–xMnxTe shifts toward lower temperature as MnTe content is increased, which is clear evidence of decreased energy separation (band convergence) between the two valence bands. The first-principles electronic structure calculations based on density functional theory also support this point. The higher doping fraction (>9%) of Mn in comparison with ~3% for Cd and Hg in SnTe gives rise to a much better valence band convergence that is responsible for the observed highest Seebeck coefficient of ~230 μV/K at 900 K. The high doping fraction of Mn in SnTe also creates stronger point defect scattering, which when combined with ubiquitous endotaxial MnTe nanostructures when the solubility of Mn is exceeded scatters a wide spectrum of phonons for a low lattice thermal conductivity of 0.9 W m–1 K–1 at 800 K. The synergistic role that Mn plays in regulating the electron and phonon transport of SnTe yields a high thermoelectric figure of merit of 1.3 at 900 K.},
doi = {10.1021/jacs.5b07284},
journal = {Journal of the American Chemical Society},
number = 35,
volume = 137,
place = {United States},
year = {Wed Aug 26 00:00:00 EDT 2015},
month = {Wed Aug 26 00:00:00 EDT 2015}
}
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https://doi.org/10.1021/jacs.5b07284
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    Eco-Friendly SnTe Thermoelectric Materials: Progress and Future Challenges
    journal, September 2017

    • Moshwan, Raza; Yang, Lei; Zou, Jin
    • Advanced Functional Materials, Vol. 27, Issue 43
    • DOI: 10.1002/adfm.201703278

    Promoting SnTe as an Eco-Friendly Solution for p-PbTe Thermoelectric via Band Convergence and Interstitial Defects
    journal, March 2017

    High-entropy functional materials
    journal, September 2018

    • Gao, Michael C.; Miracle, Daniel B.; Maurice, David
    • Journal of Materials Research, Vol. 33, Issue 19
    • DOI: 10.1557/jmr.2018.323

    Eutectoid nano-precipitates inducing remarkably enhanced thermoelectric performance in (Sn 1−x Cd x Te) 1−y (Cu 2 Te) y
    journal, January 2020

    • Qi, Xia; Huang, Yi; Wu, Di
    • Journal of Materials Chemistry A, Vol. 8, Issue 5
    • DOI: 10.1039/c9ta11180h

    Seeing atomic-scale structural origins and foreseeing new pathways to improved thermoelectric materials
    journal, January 2019

    • Wu, Haijun; Zhang, Yang; Ning, Shoucong
    • Materials Horizons, Vol. 6, Issue 8
    • DOI: 10.1039/c9mh00543a

    Discordant nature of Cd in GeTe enhances phonon scattering and improves band convergence for high thermoelectric performance
    journal, January 2020

    • Nshimyimana, Evariste; Hao, Shiqiang; Su, Xianli
    • Journal of Materials Chemistry A, Vol. 8, Issue 3
    • DOI: 10.1039/c9ta10436d

    SnTe@MnO 2 ‐SP Nanosheet–Based Intelligent Nanoplatform for Second Near‐Infrared Light–Mediated Cancer Theranostics
    journal, July 2019

    • Zhang, Hanjie; Zeng, Weiwei; Pan, Chao
    • Advanced Functional Materials, Vol. 29, Issue 37
    • DOI: 10.1002/adfm.201903791

    High thermoelectric performance of Ag doped SnTe polycrystalline bulks via the synergistic manipulation of electrical and thermal transport
    journal, January 2019

    • Zhao, Lanling; Wang, Jun; Li, Jichao
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 32
    • DOI: 10.1039/c9cp03534f

    Eco-friendly high-performance silicide thermoelectric materials
    journal, February 2017

    • Liu, Wei; Yin, Kang; Zhang, Qingjie
    • National Science Review, Vol. 4, Issue 4
    • DOI: 10.1093/nsr/nwx011

    Subtle Roles of Sb and S in Regulating the Thermoelectric Properties of N-Type PbTe to High Performance
    journal, May 2017

    • Tan, Gangjian; Stoumpos, Constantinos C.; Wang, Si
    • Advanced Energy Materials, Vol. 7, Issue 18
    • DOI: 10.1002/aenm.201700099

    Arrays of Planar Vacancies in Superior Thermoelectric Ge 1− x − y Cd x Bi y Te with Band Convergence
    journal, September 2018

    Effect of single metal doping on the thermoelectric properties of SnTe
    journal, January 2019

    • Aminzare, Masoud; Tseng, Yu-Chih; Ramakrishnan, Anbalagan
    • Sustainable Energy & Fuels, Vol. 3, Issue 1
    • DOI: 10.1039/c8se00385h

    Hydrothermal synthesis of SnQ ( Q = Te, Se, S) and their thermoelectric properties
    journal, October 2017

    Optimization of thermoelectric properties of n-type Ti, Pb co-doped SnSe
    journal, January 2017

    • Li, Fu; Wang, Wenting; Qiu, Xincheng
    • Inorganic Chemistry Frontiers, Vol. 4, Issue 10
    • DOI: 10.1039/c7qi00436b

    Band structure engineering in Sn 1.03 Te through an In-induced resonant level
    journal, January 2020

    • Misra, Shantanu; Wiendlocha, Bartlomiej; Tobola, Janusz
    • Journal of Materials Chemistry C, Vol. 8, Issue 3
    • DOI: 10.1039/c9tc04407h

    Band engineering, carrier density control, and enhanced thermoelectric performance in multi-doped SnTe
    journal, September 2019

    • Doi, A.; Shimano, S.; Inoue, D.
    • APL Materials, Vol. 7, Issue 9
    • DOI: 10.1063/1.5116882

    Improved Thermoelectric Properties in Melt-Spun SnTe
    journal, October 2017

    • Ibrahim, Dorra; Ohorodniichuk, Viktoriia; Candolfi, Christophe
    • ACS Omega, Vol. 2, Issue 10
    • DOI: 10.1021/acsomega.7b01397

    Si2Ge: A New VII-Type Clathrate with Ultralow Thermal Conductivity and High Thermoelectric Property
    journal, February 2020

    Negative-pressure polymorphs made by heterostructural alloying
    journal, April 2018

    • Siol, Sebastian; Holder, Aaron; Steffes, James
    • Science Advances, Vol. 4, Issue 4
    • DOI: 10.1126/sciadv.aaq1442

    Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials
    journal, June 2019

    BiCuSeO Thermoelectrics: An Update on Recent Progress and Perspective
    journal, February 2017

    • Zhang, Xiaoxuan; Chang, Cheng; Zhou, Yiming
    • Materials, Vol. 10, Issue 2
    • DOI: 10.3390/ma10020198
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