High Figure of Merit in Gallium-Doped Nanostructured n-Type PbTe-xGeTe with Midgap States
Abstract
PbTe-based thermoelectric materials are some of the most promising for converting heat into electricity, but their ntype versions still lag in performance the p-type ones. Here, we introduce midgap states and nanoscale precipitates using Gadoping and GeTe-alloying to considerably improve the performance of n-type PbTe. The GeTe alloying significantly enlarges the energy band gap of PbTe and subsequent Ga doping introduces special midgap states that lead to an increased density of states (DOS) effective mass and enhanced Seebeck coefficients. Moreover, the nucleated Ga2Te3 nanoscale precipitates and off-center discordant Ge atoms in the PbTe matrix cause intense phonon scattering, strongly reducing the thermal conductivity (~0.65 W m-1 K-1 at 623 K). As a result, a high room-temperature thermoelectric figure of merit ZT ~ 0.59 and a peak ZTmax of ~1.47 at 673 K were obtained for the Pb0.98Ga0.02Te-5%GeTe. The ZTavg value that is most relevant for devices is ~1.27 from 400 to 773 K, the highest recorded value for n-type PbTe.
- Authors:
-
- Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Wuhan Univ. of Technology, Wuhan (China)
- Agency for Science, Technology and Research (A*STAR), Innovis (Singapore). Institute of Materials Research and Engineering
- Nanyang Technological Univ. (Singapore)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1776870
- Grant/Contract Number:
- SC0014520; AC02-06CH11357; AC02-05CH11231; 2018-T2-1-010
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 40; 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
Citation Formats
Luo, Zhong-Zhen, Cai, Songting, Hao, Shiqiang, Bailey, Trevor P., Su, Xianli, Spanopoulos, Ioannis, Hadar, Ido, Tan, Gangjian, Luo, Yubo, Xu, Jianwei, Uher, Ctirad, Wolverton, Christopher, Dravid, Vinayak P., Yan, Qingyu, and Kanatzidis, Mercouri G. High Figure of Merit in Gallium-Doped Nanostructured n-Type PbTe-xGeTe with Midgap States. United States: N. p., 2019.
Web. doi:10.1021/jacs.9b09249.
Luo, Zhong-Zhen, Cai, Songting, Hao, Shiqiang, Bailey, Trevor P., Su, Xianli, Spanopoulos, Ioannis, Hadar, Ido, Tan, Gangjian, Luo, Yubo, Xu, Jianwei, Uher, Ctirad, Wolverton, Christopher, Dravid, Vinayak P., Yan, Qingyu, & Kanatzidis, Mercouri G. High Figure of Merit in Gallium-Doped Nanostructured n-Type PbTe-xGeTe with Midgap States. United States. https://doi.org/10.1021/jacs.9b09249
Luo, Zhong-Zhen, Cai, Songting, Hao, Shiqiang, Bailey, Trevor P., Su, Xianli, Spanopoulos, Ioannis, Hadar, Ido, Tan, Gangjian, Luo, Yubo, Xu, Jianwei, Uher, Ctirad, Wolverton, Christopher, Dravid, Vinayak P., Yan, Qingyu, and Kanatzidis, Mercouri G. Wed .
"High Figure of Merit in Gallium-Doped Nanostructured n-Type PbTe-xGeTe with Midgap States". United States. https://doi.org/10.1021/jacs.9b09249. https://www.osti.gov/servlets/purl/1776870.
@article{osti_1776870,
title = {High Figure of Merit in Gallium-Doped Nanostructured n-Type PbTe-xGeTe with Midgap States},
author = {Luo, Zhong-Zhen and Cai, Songting and Hao, Shiqiang and Bailey, Trevor P. and Su, Xianli and Spanopoulos, Ioannis and Hadar, Ido and Tan, Gangjian and Luo, Yubo and Xu, Jianwei and Uher, Ctirad and Wolverton, Christopher and Dravid, Vinayak P. and Yan, Qingyu and Kanatzidis, Mercouri G.},
abstractNote = {PbTe-based thermoelectric materials are some of the most promising for converting heat into electricity, but their ntype versions still lag in performance the p-type ones. Here, we introduce midgap states and nanoscale precipitates using Gadoping and GeTe-alloying to considerably improve the performance of n-type PbTe. The GeTe alloying significantly enlarges the energy band gap of PbTe and subsequent Ga doping introduces special midgap states that lead to an increased density of states (DOS) effective mass and enhanced Seebeck coefficients. Moreover, the nucleated Ga2Te3 nanoscale precipitates and off-center discordant Ge atoms in the PbTe matrix cause intense phonon scattering, strongly reducing the thermal conductivity (~0.65 W m-1 K-1 at 623 K). As a result, a high room-temperature thermoelectric figure of merit ZT ~ 0.59 and a peak ZTmax of ~1.47 at 673 K were obtained for the Pb0.98Ga0.02Te-5%GeTe. The ZTavg value that is most relevant for devices is ~1.27 from 400 to 773 K, the highest recorded value for n-type PbTe.},
doi = {10.1021/jacs.9b09249},
journal = {Journal of the American Chemical Society},
number = 40,
volume = 141,
place = {United States},
year = {Wed Sep 11 00:00:00 EDT 2019},
month = {Wed Sep 11 00:00:00 EDT 2019}
}
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