Thermal conductivity in Bi0.5Sb1.5Te3+x and the role of dense dislocation arrays at grain boundaries
Abstract
Several prominent mechanisms for reduction in thermal conductivity have been shown in recent years to improve the figure of merit for thermoelectric materials. Such a mechanism is a hierarchical all-length-scale architecturing that recognizes the role of all microstructure elements, from atomic to nano to microscales, in reducing (lattice) thermal conductivity. In this context, there have been recent claims of remarkably low (lattice) thermal conductivity in Bi0.5Sb1.5Te3 that are attributed to seemingly ordinary grain boundary dislocation networks. These high densities of dislocation networks in Bi0.5Sb1.5Te3 were generated via unconventional materials processing with excess Te (which formed liquid phase, thereby facilitating sintering), followed by spark plasma sintering under pressure to squeeze out the liquid. We reproduced a practically identical microstructure, following practically identical processing strategies, but with noticeably different (higher) thermal conductivity than that claimed before. We show that the resultant microstructure is anisotropic, with notable difference of thermal and charge transport properties across and along two orthonormal directions, analogous to anisotropic crystals. Thus, we believe that grain boundary dislocation networks are not the primary cause of enhanced ZT through reduction in thermal conductivity. Instead, we can reproduce the purported high ZT through a favorable but impractical and incorrect combination of thermalmore »
- Authors:
-
- Wuhan University of Technology (China)
- Wuhan University of Technology (China); Northwestern Univ., Evanston, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1499916
- Alternate Identifier(s):
- OSTI ID: 1775291
- Grant/Contract Number:
- SC0014520
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 6; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Deng, Rigui, Su, Xianli, Zheng, Zheng, Liu, Wei, Yan, Yonggao, Zhang, Qingjie, Dravid, Vinayak P., Uher, Ctirad, Kanatzidis, Mercouri G., and Tang, Xinfeng. Thermal conductivity in Bi0.5Sb1.5Te3+x and the role of dense dislocation arrays at grain boundaries. United States: N. p., 2018.
Web. doi:10.1126/sciadv.aar5606.
Deng, Rigui, Su, Xianli, Zheng, Zheng, Liu, Wei, Yan, Yonggao, Zhang, Qingjie, Dravid, Vinayak P., Uher, Ctirad, Kanatzidis, Mercouri G., & Tang, Xinfeng. Thermal conductivity in Bi0.5Sb1.5Te3+x and the role of dense dislocation arrays at grain boundaries. United States. https://doi.org/10.1126/sciadv.aar5606
Deng, Rigui, Su, Xianli, Zheng, Zheng, Liu, Wei, Yan, Yonggao, Zhang, Qingjie, Dravid, Vinayak P., Uher, Ctirad, Kanatzidis, Mercouri G., and Tang, Xinfeng. Fri .
"Thermal conductivity in Bi0.5Sb1.5Te3+x and the role of dense dislocation arrays at grain boundaries". United States. https://doi.org/10.1126/sciadv.aar5606. https://www.osti.gov/servlets/purl/1499916.
@article{osti_1499916,
title = {Thermal conductivity in Bi0.5Sb1.5Te3+x and the role of dense dislocation arrays at grain boundaries},
author = {Deng, Rigui and Su, Xianli and Zheng, Zheng and Liu, Wei and Yan, Yonggao and Zhang, Qingjie and Dravid, Vinayak P. and Uher, Ctirad and Kanatzidis, Mercouri G. and Tang, Xinfeng},
abstractNote = {Several prominent mechanisms for reduction in thermal conductivity have been shown in recent years to improve the figure of merit for thermoelectric materials. Such a mechanism is a hierarchical all-length-scale architecturing that recognizes the role of all microstructure elements, from atomic to nano to microscales, in reducing (lattice) thermal conductivity. In this context, there have been recent claims of remarkably low (lattice) thermal conductivity in Bi0.5Sb1.5Te3 that are attributed to seemingly ordinary grain boundary dislocation networks. These high densities of dislocation networks in Bi0.5Sb1.5Te3 were generated via unconventional materials processing with excess Te (which formed liquid phase, thereby facilitating sintering), followed by spark plasma sintering under pressure to squeeze out the liquid. We reproduced a practically identical microstructure, following practically identical processing strategies, but with noticeably different (higher) thermal conductivity than that claimed before. We show that the resultant microstructure is anisotropic, with notable difference of thermal and charge transport properties across and along two orthonormal directions, analogous to anisotropic crystals. Thus, we believe that grain boundary dislocation networks are not the primary cause of enhanced ZT through reduction in thermal conductivity. Instead, we can reproduce the purported high ZT through a favorable but impractical and incorrect combination of thermal conductivity measured along the pressing direction of anisotropy while charge transport measured in the direction perpendicular to the anisotropic direction. We believe that our work underscores the need for consistency in charge and thermal transport measurements for unified and verifiable measurements of thermoelectric (and related) properties and phenomena.},
doi = {10.1126/sciadv.aar5606},
journal = {Science Advances},
number = 6,
volume = 4,
place = {United States},
year = {Fri Jun 01 00:00:00 EDT 2018},
month = {Fri Jun 01 00:00:00 EDT 2018}
}
Web of Science
Figures / Tables:
Works referenced in this record:
Mechanically Robust BiSbTe Alloys with Superior Thermoelectric Performance: A Case Study of Stable Hierarchical Nanostructured Thermoelectric Materials
journal, November 2014
- Zheng, Yun; Zhang, Qiang; Su, Xianli
- Advanced Energy Materials, Vol. 5, Issue 5
Enhanced thermoelectric figure of merit in p-type β-Zn 4 Sb 3 /Bi 0.4 Sb 1.6 Te 3 nanocomposites
journal, January 2016
- Li, Yuanyue; Dou, Yunchen; Qin, Xiaoying
- RSC Advances, Vol. 6, Issue 15
Thermoelectric Devices for Power Generation: Recent Progress and Future Challenges : Thermoelectric Devices for Power Generation
journal, September 2015
- Zhang, Qi Hao; Huang, Xiang Yang; Bai, Sheng Qiang
- Advanced Engineering Materials, Vol. 18, Issue 2
Simultaneous improvement in electrical and thermal properties of interface-engineered BiSbTe nanostructured thermoelectric materials
journal, December 2016
- Jo, Seungki; Park, Sung Hoon; Ban, Hyeong Woo
- Journal of Alloys and Compounds, Vol. 689
The texture related anisotropy of thermoelectric properties in bismuth telluride based polycrystalline alloys
journal, September 2011
- Shen, J. J.; Hu, L. P.; Zhu, T. J.
- Applied Physics Letters, Vol. 99, Issue 12
Multi-Scale Microstructural Thermoelectric Materials: Transport Behavior, Non-Equilibrium Preparation, and Applications
journal, January 2017
- Su, Xianli; Wei, Ping; Li, Han
- Advanced Materials, Vol. 29, Issue 20
Active thermal cloak
journal, September 2015
- Nguyen, Dang Minh; Xu, Hongyi; Zhang, Youming
- Applied Physics Letters, Vol. 107, Issue 12
The Thermoelectric Figure of Merit and its Relation to Thermoelectric Generators†
journal, July 1959
- Chasmar, R. P.; Stratton, R.
- Journal of Electronics and Control, Vol. 7, Issue 1
Practical doping principles
journal, July 2003
- Zunger, Alex
- Applied Physics Letters, Vol. 83, Issue 1
Thermoelectric Efficiency and Compatibility
journal, October 2003
- Snyder, G. Jeffrey; Ursell, Tristan S.
- Physical Review Letters, Vol. 91, Issue 14
Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics
journal, April 2015
- Kim, Sang Il; Lee, Kyu Hyoung; Mun, Hyeon A.
- Science, Vol. 348, Issue 6230
Thermoelectric properties and extremely low lattice thermal conductivity in p-type Bismuth Tellurides by Pb-doping and PbTe precipitation
journal, June 2016
- Lin, Chan-Chieh; Ginting, Dianta; Lydia, R.
- Journal of Alloys and Compounds, Vol. 671
Transport properties and valence band feature of high-performance (GeTe) 85 (AgSbTe 2 ) 15 thermoelectric materials
journal, January 2014
- Chen, Y.; Jaworski, C. M.; Gao, Y. B.
- New Journal of Physics, Vol. 16, Issue 1
High Thermoelectric Performance via Hierarchical Compositionally Alloyed Nanostructures
journal, May 2013
- Zhao, Li-Dong; Hao, Shiqiang; Lo, Shih-Han
- Journal of the American Chemical Society, Vol. 135, Issue 19
Improvement of Thermoelectric Properties of Bi0.4Sb1.6Te3 with Addition of Nanoscale Zinc Oxide Particles
journal, August 2015
- Xiao, Ye; Yang, Junyou; Jiang, Qinghui
- Journal of Electronic Materials, Vol. 45, Issue 3
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
Thermoelectric performance enhancement in n-type Bi2(TeSe)3 alloys owing to nanoscale inhomogeneity combined with a spark plasma-textured microstructure
journal, June 2016
- Pan, Yu; Li, Jing-Feng
- NPG Asia Materials, Vol. 8, Issue 6
Convergence of Conduction Bands as a Means of Enhancing Thermoelectric Performance of -Type Solid Solutions
journal, April 2012
- Liu, Wei; Tan, Xiaojian; Yin, Kang
- Physical Review Letters, Vol. 108, Issue 16
High Performance Thermoelectrics from Earth-Abundant Materials: Enhanced Figure of Merit in PbS by Second Phase Nanostructures
journal, December 2011
- Zhao, Li-Dong; Lo, Shih-Han; He, Jiaqing
- Journal of the American Chemical Society, Vol. 133, Issue 50
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
Unique nanostructures and enhanced thermoelectric performance of melt-spun BiSbTe alloys
journal, March 2009
- Xie, Wenjie; Tang, Xinfeng; Yan, Yonggao
- Applied Physics Letters, Vol. 94, Issue 10
Preparation and thermoelectric transport properties of high-performance p-type Bi2Te3 with layered nanostructure
journal, January 2007
- Tang, Xinfeng; Xie, Wenjie; Li, Han
- Applied Physics Letters, Vol. 90, Issue 1
Enhanced Thermoelectric Properties in the Counter-Doped SnTe System with Strained Endotaxial SrTe
journal, February 2016
- Zhao, Li-Dong; Zhang, Xiao; Wu, Haijun
- Journal of the American Chemical Society, Vol. 138, Issue 7
Enhanced thermoelectric performance in p-type BiSbTe bulk alloy with nanoinclusion of ZnAlO
journal, January 2011
- Zhang, Ting; Zhang, Qiushi; Jiang, Jun
- Applied Physics Letters, Vol. 98, Issue 2
A simultaneous increase in the ZT and the corresponding critical temperature of p-type Bi 0.4 Sb 1.6 Te 3 by a combined strategy of dual nanoinclusions and carrier engineering
journal, January 2014
- Xiao, Ye; Yang, Jun-you; Jiang, Qing-hui
- J. Mater. Chem. A, Vol. 2, Issue 47
Recent Developments in Semiconductor Thermoelectric Physics and Materials
journal, August 2011
- Shakouri, Ali
- Annual Review of Materials Research, Vol. 41, Issue 1
Advances in Thermal Conductivity
journal, August 2012
- Toberer, Eric S.; Baranowski, Lauryn L.; Dames, Chris
- Annual Review of Materials Research, Vol. 42, Issue 1
High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys
journal, May 2008
- Poudel, B.; Hao, Q.; Ma, Y.
- Science, Vol. 320, Issue 5876, p. 634-638
Enhanced thermoelectric figure of merit in p-type BiSbTeSe alloy with ZnSb addition
journal, January 2013
- Zhang, Ting; Jiang, Jun; Xiao, Yukun
- J. Mater. Chem. A, Vol. 1, Issue 3
Ultrahigh power factor and thermoelectric performance in hole-doped single-crystal SnSe
journal, November 2015
- Zhao, L.-D.; Tan, G.; Hao, S.
- Science, Vol. 351, Issue 6269, p. 141-144
Improvement of the Thermoelectric Figure-of-Merit of a Doped Telluride Nanocomposite by Combining Phonon Scattering with Grain Boundary-Modifying Zn-Containing Nanostructures
journal, October 2014
- Rowe, Michael P.; Zhou, Li Qin; Banerjee, Debasish
- Journal of Electronic Materials, Vol. 44, Issue 1
High-performance nanostructured thermoelectric materials
journal, October 2010
- Li, Jing-Feng; Liu, Wei-Shu; Zhao, Li-Dong
- NPG Asia Materials, Vol. 2, Issue 4
Advances in thermoelectric materials research: Looking back and moving forward
journal, September 2017
- He, Jian; Tritt, Terry M.
- Science, Vol. 357, Issue 6358
Thermoelectrics
book, January 2001
- Nolas, George S.; Sharp, Jeffrey; Goldsmid, H. Julian
- Springer Series in Materials Science
Works referencing / citing this record:
High‐Performance Flexible Thermoelectric Devices Based on All‐Inorganic Hybrid Films for Harvesting Low‐Grade Heat
journal, April 2019
- Wu, Bo; Guo, Yang; Hou, Chengyi
- Advanced Functional Materials, Vol. 29, Issue 25
Nanoassembly Growth Model for Subdomain and Grain Boundary Formation in 1T′ Layered ReS 2
journal, September 2019
- Li, Xiaobo; Wang, Xiao; Hong, Jinhua
- Advanced Functional Materials, Vol. 29, Issue 49
Cu Intercalation and Br Doping to Thermoelectric SnSe 2 Lead to Ultrahigh Electron Mobility and Temperature‐Independent Power Factor
journal, December 2019
- Zhou, Chongjian; Yu, Yuan; Zhang, Xiangzhao
- Advanced Functional Materials, Vol. 30, Issue 6
The Thermoelectric Properties of Bismuth Telluride
journal, April 2019
- Witting, Ian T.; Chasapis, Thomas C.; Ricci, Francesco
- Advanced Electronic Materials, Vol. 5, Issue 6
High‐Efficiency Thermoelectric Power Generation Enabled by Homogeneous Incorporation of MXene in (Bi,Sb) 2 Te 3 Matrix
journal, November 2019
- Lu, Xiaofang; Zhang, Qihao; Liao, Jincheng
- Advanced Energy Materials, Vol. 10, Issue 2
Structural and transport properties of quenched and melt-spun BixSb2−xTe3 solid solutions (x = 0.40 and 0.48)
journal, October 2019
- Ohorodniichuk, Viktoriia; El-Oualid, Soufiane; Dauscher, Anne
- Journal of Materials Science, Vol. 55, Issue 3
Enhancement of thermoelectric performance through synergy of Pb acceptor doping and superstructure modulation for p-type Bi2Te3
journal, December 2019
- Wu, Wei; Liu, Wenxin; Yu, Fengrong
- Journal of Materials Science: Materials in Electronics, Vol. 31, Issue 2
Discovery of colossal Seebeck effect in metallic Cu2Se
journal, January 2019
- Byeon, Dogyun; Sobota, Robert; Delime-Codrin, Kévin
- Nature Communications, Vol. 10, Issue 1
Enhancement of thermoelectric properties over a wide temperature range by lattice disorder and chemical potential tuning in a (CuI) y (Bi 2 Te 3 ) 0.95−x (Bi 2 Se 3 ) x (Bi 2 S 3 ) 0.05 quaternary system
journal, January 2019
- Cho, Hyunyong; Back, Song Yi; Kim, Jin Hee
- RSC Advances, Vol. 9, Issue 8
Optimized orientation and enhanced thermoelectric performance in Sn 0.97 Na 0.03 Se with Te addition
journal, January 2019
- Zhang, Jiahua; Xu, Jingtao; Tan, Xiaojian
- Journal of Materials Chemistry C, Vol. 7, Issue 9
Magnetism-induced huge enhancement of the room-temperature thermoelectric and cooling performance of p-type BiSbTe alloys
journal, January 2020
- Li, Cuncheng; Ma, Shifang; Wei, Ping
- Energy & Environmental Science, Vol. 13, Issue 2
Thermoelectric (Bi,Sb) 2 Te 3 –Ge 0.5 Mn 0.5 Te composites with excellent mechanical properties
journal, January 2019
- Duan, Sichen; Man, Na; Xu, Jingtao
- Journal of Materials Chemistry A, Vol. 7, Issue 15
New insights into the role of dislocation engineering in N-type filled skutterudite CoSb 3
journal, January 2019
- Liu, Zihang; Meng, Xianfu; Qin, Dandan
- Journal of Materials Chemistry C, Vol. 7, Issue 43
Temperature dependent Raman of BiTe nanotubes
journal, December 2018
- Zhou, Fang; Zhao, Yujing; Zhou, Weichang
- AIP Advances, Vol. 8, Issue 12
Advances in thermoelectrics
journal, April 2018
- Mao, Jun; Liu, Zihang; Zhou, Jiawei
- Advances in Physics, Vol. 67, Issue 2
Pre-oxidation effects on properties of bismuth telluride thermoelectric composites compacted by spark plasma sintering
journal, January 2020
- Kim, Jinseo; Duy, Le Thai; Ahn, Byungmin
- Journal of Asian Ceramic Societies, Vol. 8, Issue 1
Synthesis of single crystalline BiTe nanobelts by catalyst-free vapor transport method
journal, December 2019
- Pillai, Krishnakumar
- Materials Research Express, Vol. 6, Issue 12
Thermoelectric power generation: from new materials to devices
journal, July 2019
- Tan, Gangjian; Ohta, Michihiro; Kanatzidis, Mercouri G.
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2152
Pre-oxidation effects on properties of bismuth telluride thermoelectric composites compacted by spark plasma sintering
text, January 2020
- Kim, Jinseo; Duy, Le Thai; Ahn, Byungmin
- Taylor & Francis
Figures / Tables found in this record: