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Title: Distinct Impact of Alkali-Ion Doping on Electrical Transport Properties of Thermoelectric p-Type Polycrystalline SnSe

Abstract

Recent findings about ultrahigh thermoelectric performance in SnSe single crystals have stimulated related research on this simple binary compound, which is focused mostly on its polycrystalline counterparts, and particularly on electrical property enhancement by effective doping. The work reported here systematically investigated the thermoelectric properties of polycrystalline SnSe doped with three alkali metals (Li, Na, and K). It is found that Na has the best doping efficiency, leading to an increase in hole concentration from 3.2 × 1017 to 4.4 × 1019 cm–3 at room temperature, accompanied by a drop in Seebeck coefficient from 480 to 142 μV/K. An equivalent single parabolic band model was found adequate to capture the variation tendency of Seebeck coefficient with doping levels within a wide range. A mixed scattering of carriers by acoustic phonons and grain boundaries is suitable for numerically understanding the temperature-dependence of carrier mobility. A maximum ZT of ~0.8 was achieved in 1% Na- or K-doped SnSe at 800 K. Possible strategies to improve the mobility and ZT of polycrystals were also proposed.

Authors:
 [1];  [2];  [2];  [1];  [1];  [2];  [2];  [2]
+ Show Author Affiliations
  1. Tsinghua Univ., Beijing (China)
  2. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC); Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); National Basic Research Program of China; National Science Foundation (NSF); International Institute for Nanotechnology (IIN); Keck Foundation; State of Illinois
OSTI Identifier:
1388415
Grant/Contract Number:  
SC0001299; FG02-09ER46577; 2013CB632503; SC0014520
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 28; Related Information: S3TEC partners with Massachusetts Institute of Technology (lead); Boston College; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute; 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; solar (photovoltaic); solar (thermal); solid state lighting; phonons; thermal conductivity; thermoelectric; defects; mechanical behavior; charge transport; spin dynamics; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); impurities; crystal structure; scattering; carrier dynamics; doping

Citation Formats

Wei, Tian-Ran, Tan, Gangjian, Zhang, Xiaomi, Wu, Chao-Feng, Li, Jing-Feng, Dravid, Vinayak P., Snyder, G. Jeffrey, and Kanatzidis, Mercouri G. Distinct Impact of Alkali-Ion Doping on Electrical Transport Properties of Thermoelectric p-Type Polycrystalline SnSe. United States: N. p., 2016. Web. doi:10.1021/jacs.6b04181.
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Wei, Tian-Ran, Tan, Gangjian, Zhang, Xiaomi, Wu, Chao-Feng, Li, Jing-Feng, Dravid, Vinayak P., Snyder, G. Jeffrey, & Kanatzidis, Mercouri G. Distinct Impact of Alkali-Ion Doping on Electrical Transport Properties of Thermoelectric p-Type Polycrystalline SnSe. United States. https://doi.org/10.1021/jacs.6b04181
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Wei, Tian-Ran, Tan, Gangjian, Zhang, Xiaomi, Wu, Chao-Feng, Li, Jing-Feng, Dravid, Vinayak P., Snyder, G. Jeffrey, and Kanatzidis, Mercouri G. Mon . "Distinct Impact of Alkali-Ion Doping on Electrical Transport Properties of Thermoelectric p-Type Polycrystalline SnSe". United States. https://doi.org/10.1021/jacs.6b04181. https://www.osti.gov/servlets/purl/1388415.
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@article{osti_1388415,
title = {Distinct Impact of Alkali-Ion Doping on Electrical Transport Properties of Thermoelectric p-Type Polycrystalline SnSe},
author = {Wei, Tian-Ran and Tan, Gangjian and Zhang, Xiaomi and Wu, Chao-Feng and Li, Jing-Feng and Dravid, Vinayak P. and Snyder, G. Jeffrey and Kanatzidis, Mercouri G.},
abstractNote = {Recent findings about ultrahigh thermoelectric performance in SnSe single crystals have stimulated related research on this simple binary compound, which is focused mostly on its polycrystalline counterparts, and particularly on electrical property enhancement by effective doping. The work reported here systematically investigated the thermoelectric properties of polycrystalline SnSe doped with three alkali metals (Li, Na, and K). It is found that Na has the best doping efficiency, leading to an increase in hole concentration from 3.2 × 1017 to 4.4 × 1019 cm–3 at room temperature, accompanied by a drop in Seebeck coefficient from 480 to 142 μV/K. An equivalent single parabolic band model was found adequate to capture the variation tendency of Seebeck coefficient with doping levels within a wide range. A mixed scattering of carriers by acoustic phonons and grain boundaries is suitable for numerically understanding the temperature-dependence of carrier mobility. A maximum ZT of ~0.8 was achieved in 1% Na- or K-doped SnSe at 800 K. Possible strategies to improve the mobility and ZT of polycrystals were also proposed.},
doi = {10.1021/jacs.6b04181},
journal = {Journal of the American Chemical Society},
number = 28,
volume = 138,
place = {United States},
year = {Mon Jun 27 00:00:00 EDT 2016},
month = {Mon Jun 27 00:00:00 EDT 2016}
}
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Figures / Tables:

Figure 1 Figure 1: XRD patterns of (a) SnSe-based materials and (b) a Na-doped sample along two different directions; obvious difference in the relative peak intensity of (400) and (111) is seen, indicating strong anisotropy of the bulk samples. (c) High-resolution XPS spectra of Na (1s) and K (2p3/2); one or amore » series of Se LMM Auger electron bonding energy peak(s) was (were) detected near the K 2p3/2 signal. (d) Optical absorption spectra for SnSe-based materials; arrow 1 in shows the Burstein−Moss shift and arrow 2 indicates enhanced free-carrier absorption.« less
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