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Title: Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb4

Abstract

The rise of high-throughput calculations has accelerated the discovery of promising classes of thermoelectric materials. In prior work, we identified the n-type Zintl pnictides as one such material class. To date, however, a lack of detailed defect calculations and chemical intuition has led the community to investigate p-type Zintls almost exclusively. Here, we investigate the synthesis, thermoelectric properties, and defect structure of the complex Zintl KGaSb4. We find that KGaSb4 is successfully doped n-type with Ba and has the potential for p-type doping with Zn. Our calculations reveal the fundamental defect structure in KGaSb4 that enables n-type and p-type doping. We find that Ba doped KGaSb4 exhibits high electronic mobility (~50 cm2V-1s-1) and near minimum lattice thermal conductivity (<0.5 Wm-1K-1) at 400 °C. Samples doped with 1.5% Ba achieve zT > 0.9 at 400 °C, promising for a previously unstudied material. Here, we also briefly investigate the series of alloys between KGaSb4 and KAlSb4, finding that a full solid solution exists. Altogether our work reinforces motivation for the exploration of n-type Zintl materials, especially in tandem with high-throughput defect calculations to inform selection of effective dopants and systems amenable to n-type transport.

Authors:
ORCiD logo [1];  [2];  [3];  [4]
+ Show Author Affiliations
  1. Colorado School of Mines, Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
  4. Colorado School of Mines, Golden, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)
OSTI Identifier:
1365699
Report Number(s):
NREL/JA-5K00-68728
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 10; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; synthesis; thermoelectric properties; defect structure

Citation Formats

Ortiz, Brenden R., Gorai, Prashun, Stevanovic, Vladan, and Toberer, Eric S. Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb4. United States: N. p., 2017. Web. doi:10.1021/acs.chemmater.7b01217.
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Ortiz, Brenden R., Gorai, Prashun, Stevanovic, Vladan, & Toberer, Eric S. Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb4. United States. https://doi.org/10.1021/acs.chemmater.7b01217
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Ortiz, Brenden R., Gorai, Prashun, Stevanovic, Vladan, and Toberer, Eric S. Mon . "Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb4". United States. https://doi.org/10.1021/acs.chemmater.7b01217. https://www.osti.gov/servlets/purl/1365699.
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@article{osti_1365699,
title = {Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb4},
author = {Ortiz, Brenden R. and Gorai, Prashun and Stevanovic, Vladan and Toberer, Eric S.},
abstractNote = {The rise of high-throughput calculations has accelerated the discovery of promising classes of thermoelectric materials. In prior work, we identified the n-type Zintl pnictides as one such material class. To date, however, a lack of detailed defect calculations and chemical intuition has led the community to investigate p-type Zintls almost exclusively. Here, we investigate the synthesis, thermoelectric properties, and defect structure of the complex Zintl KGaSb4. We find that KGaSb4 is successfully doped n-type with Ba and has the potential for p-type doping with Zn. Our calculations reveal the fundamental defect structure in KGaSb4 that enables n-type and p-type doping. We find that Ba doped KGaSb4 exhibits high electronic mobility (~50 cm2V-1s-1) and near minimum lattice thermal conductivity (<0.5 Wm-1K-1) at 400 °C. Samples doped with 1.5% Ba achieve zT > 0.9 at 400 °C, promising for a previously unstudied material. Here, we also briefly investigate the series of alloys between KGaSb4 and KAlSb4, finding that a full solid solution exists. Altogether our work reinforces motivation for the exploration of n-type Zintl materials, especially in tandem with high-throughput defect calculations to inform selection of effective dopants and systems amenable to n-type transport.},
doi = {10.1021/acs.chemmater.7b01217},
journal = {Chemistry of Materials},
number = 10,
volume = 29,
place = {United States},
year = {Mon May 08 00:00:00 EDT 2017},
month = {Mon May 08 00:00:00 EDT 2017}
}
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https://doi.org/10.1021/acs.chemmater.7b01217
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