Non-equilibrium processing leads to record high thermoelectric figure of merit in PbTe–SrTe

Tan, Gangjian; Shi, Fengyuan; Hao, Shiqiang; Zhao, Li-Dong; Chi, Hang; Zhang, Xiaomi; Uher, Ctirad; Wolverton, Chris; Dravid, Vinayak P.; Kanatzidis, Mercouri G.

doi:10.1038/ncomms12167

Title: Non-equilibrium processing leads to record high thermoelectric figure of merit in PbTe–SrTe

Journal Article · Tue Jul 26 00:00:00 EDT 2016 · Nature Communications

DOI:https://doi.org/10.1038/ncomms12167· OSTI ID:1326596

^[1]; Shi, Fengyuan ^[2]; Hao, Shiqiang ^[2]; Zhao, Li-Dong ^[3];

^[4]; Zhang, Xiaomi ^[2]; Uher, Ctirad ^[4]; Wolverton, Chris ^[2]; Dravid, Vinayak P. ^[2]; Kanatzidis, Mercouri G. ^[5]

Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Beihang Univ., Beijing (China). School of Materials Science and Engineering
Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

The broad-based implementation of thermoelectric materials in converting heat to electricity hinges on the achievement of high conversion efficiency. Here we demonstrate a thermoelectric figure of merit ZT of 2.5 at 923 K by the cumulative integration of several performance-enhancing concepts in a single material system. Using non-equilibrium processing we show that hole-doped samples of PbTe can be heavily alloyed with SrTe well beyond its thermodynamic solubility limit of <1 mol%. The much higher levels of Sr alloyed into the PbTe matrix widen the bandgap and create convergence of the two valence bands of PbTe, greatly boosting the power factors with maximal values over 30 μWcm ^-1 K ^-2. Exceeding the 5 mol% solubility limit leads to endotaxial SrTe nanostructures which produce extremely low lattice thermal conductivity of 0.5 Wm ^-1 K ^-1 but preserve high hole mobilities because of the matrix/precipitate valence band alignment. The best composition is hole-doped PbTe-8% SrTe.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences and Engineering Division

Grant/Contract Number:: AC02-06CH11357; SC0014520

OSTI ID:: 1326596

Journal Information:: Nature Communications, Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 448 works

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Power-Source-Free Analysis of Pyroelectric Energy Conversion Zhang, Chenbo; Song, Yintao; Wegner, Maike Physical Review Applied, Vol. 12, Issue 1 https://doi.org/10.1103/physrevapplied.12.014063	journal	July 2019
Enhancing Thermoelectric Performance Using Nonlinear Transport Effects Jiang, Jian-Hua; Imry, Yoseph Physical Review Applied, Vol. 7, Issue 6 https://doi.org/10.1103/physrevapplied.7.064001	journal	June 2017
Monte Carlo phonon transport simulations in hierarchically disordered silicon nanostructures Chakraborty, Dhritiman; Foster, Samuel; Neophytou, Neophytos Physical Review B, Vol. 98, Issue 11 https://doi.org/10.1103/physrevb.98.115435	journal	September 2018
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Microstructure Evolution of Ag-Alloyed PbTe-Based Compounds and Implications for Thermoelectric Performance Grossfeld, Tom; Sheskin, Ariel; Gelbstein, Yaniv Crystals, Vol. 7, Issue 9 https://doi.org/10.3390/cryst7090281	journal	September 2017
Influence of Nanostructuration on PbTe Alloys Synthesized by Arc-Melting Gainza, Javier; Serrano-Sánchez, Federico; Biskup, Neven Materials, Vol. 12, Issue 22 https://doi.org/10.3390/ma12223783	journal	November 2019
Highly Textured N-Type SnSe Polycrystals with Enhanced Thermoelectric Performance Shang, Peng-Peng; Dong, Jinfeng; Pei, Jun Research, Vol. 2019 https://doi.org/10.34133/2019/9253132	journal	November 2019
Compromise and Synergy in High-Efficiency Thermoelectric Materials Zhu, Tiejun; Liu, Yintu; Fu, Chenguang Advanced Materials, Vol. 29, Issue 14 https://doi.org/10.1002/adma.201605884	journal	March 2017
Design of Highly Efficient Thermoelectric Materials: Tailoring Reciprocal-Space Properties by Real-Space Modification Zhu, Hao; Xiao, Chong; Xie, Yi Advanced Materials, Vol. 30, Issue 48 https://doi.org/10.1002/adma.201802000	journal	September 2018
High‐Performance Thermoelectric SnSe: Aqueous Synthesis, Innovations, and Challenges Shi, Xiao‐Lei; Tao, Xinyong; Zou, Jin Advanced Science, Vol. 7, Issue 7 https://doi.org/10.1002/advs.201902923	journal	February 2020
High Thermoelectric Performance in PbSe–NaSbSe ₂ Alloys from Valence Band Convergence and Low Thermal Conductivity Slade, Tyler J.; Bailey, Trevor P.; Grovogui, Jann A. Advanced Energy Materials, Vol. 9, Issue 30 https://doi.org/10.1002/aenm.201901377	journal	July 2019
Discordant nature of Cd in PbSe: off-centering and core–shell nanoscale CdSe precipitates lead to high thermoelectric performance Cai, Songting; Hao, Shiqiang; Luo, Zhong-Zhen Energy & Environmental Science, Vol. 13, Issue 1 https://doi.org/10.1039/c9ee03087e	journal	January 2020
Core–shell nanostructures introduce multiple potential barriers to enhance energy filtering for the improvement of the thermoelectric properties of SnTe Ma, Zheng; Wang, Chao; Lei, Jingdan Nanoscale, Vol. 12, Issue 3 https://doi.org/10.1039/c9nr09331a	journal	January 2020
Enhanced thermoelectric transport properties of n-type InSe due to the emergence of the flat band by Si doping Lee, Kyu Hyoung; Oh, Min-Wook; Kim, Hyun-Sik Inorganic Chemistry Frontiers, Vol. 6, Issue 6 https://doi.org/10.1039/c9qi00210c	journal	January 2019
Discordant nature of Cd in GeTe enhances phonon scattering and improves band convergence for high thermoelectric performance Nshimyimana, Evariste; Hao, Shiqiang; Su, Xianli Journal of Materials Chemistry A, Vol. 8, Issue 3 https://doi.org/10.1039/c9ta10436d	journal	January 2020
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Tuning of Mg content to enhance the thermoelectric properties in binary Mg _{2+ δ} Si ( δ = 0, 0.1, 0.15, 0.2) Balasubramanian, Priyadarshini; Battabyal, Manjusha; Das, Dhruba Materials Research Express, Vol. 6, Issue 12 https://doi.org/10.1088/2053-1591/ab58fb	journal	November 2019
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Chalcogenide Thermoelectrics Empowered by an Unconventional Bonding Mechanism Yu, Yuan; Cagnoni, Matteo; Cojocaru-Mirédin, Oana RWTH Aachen University https://doi.org/10.18154/rwth-2019-07977	text	January 2019
BiCuSeO Thermoelectrics: An Update on Recent Progress and Perspective Zhang, Xiaoxuan; Chang, Cheng; Zhou, Yiming Materials, Vol. 10, Issue 2 https://doi.org/10.3390/ma10020198	journal	February 2017
A Practical Approach to Evaluate Lattice Thermal Conductivity in Two-Phase Thermoelectric Alloys for Energy Applications Amouyal, Yaron Materials, Vol. 10, Issue 4 https://doi.org/10.3390/ma10040386	journal	April 2017
Manipulation of Band Degeneracy and Lattice Strain for Extraordinary PbTe Thermoelectrics Wu, Yixuan; Nan, Pengfei; Chen, Zhiwei Research, Vol. 2020 https://doi.org/10.34133/2020/8151059	journal	January 2020
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2D Black Phosphorus for Energy Storage and Thermoelectric Applications Zhang, Yu; Zheng, Yun; Rui, Kun Small, Vol. 13, Issue 28 https://doi.org/10.1002/smll.201700661	journal	June 2017
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Unveiling a Novel, Cation-Rich Compound in a High-Pressure Pb–Te Binary System Yu, Hulei; Lin, Xiaohuan; Li, Kuo ACS Central Science, Vol. 5, Issue 4 https://doi.org/10.1021/acscentsci.9b00083	journal	April 2019
Thermal Stability of P-Type BiSbTe Alloys Prepared by Melt Spinning and Rapid Sintering Zheng, Yun; Tan, Gangjian; Luo, Yubo Materials, Vol. 10, Issue 6 https://doi.org/10.3390/ma10060617	journal	June 2017

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