Bonding Hierarchy Gives Rise to High Thermoelectric Performance in Layered Zintl Compound BaAu2P4
Abstract
The search for new thermoelectric materials has gained rapid progress in recent years as thermoelectric technology offers the potential for environmentally friendly and sustainable energy conversion methods from waste heat to electricity. In this work, we use first-principles calculations based on density functional theory to predict high thermoelectric performance in BaAu2P4, a layered Zintl compound with a small band gap. BaAu2P4 exhibits crystallographic heterogeneity in which rigid [Au2P4]2– units are separated by layers of Ba2+ cations, which are bonded relatively weakly to the lattice through electrostatic interactions. The phosphorus atoms are covalently bonded to each other and form infinite chains within the crystal. While the phosphorus chains facilitate large electrical conductivity, the presence of multiple bands near the Fermi level gives rise to an enhanced Seebeck coefficient. On the other hand, the loosely bound Ba along with Au strongly scatter the heat carrying acoustic phonons, significantly reducing the lattice thermal conduction along the stacking direction. As a consequence of this bonding hierarchy (i.e., coexisting rigid and fluctuating sublattices), BaAu2P4 exhibits a large power factor and low lattice thermal conductivity, which results in a high thermoelectric figure of merit ($zT$). Thus, our findings should encourage the exploration of new thermoelectric materialsmore »
- Authors:
-
- Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Northwestern Univ., Evanston, IL (United States); Citrine Informatics, Inc., Redwood City, CA (United States); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1543613
- Alternate Identifier(s):
- OSTI ID: 1775430
- Grant/Contract Number:
- SC0014520; SC0015106; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 21; 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; Chemistry; Materials Science; Thermal conductivity; Phonons; Gold; Lattices; Electrical conductivity
Citation Formats
Pal, Koushik, He, Jiangang, and Wolverton, C. Bonding Hierarchy Gives Rise to High Thermoelectric Performance in Layered Zintl Compound BaAu2P4. United States: N. p., 2018.
Web. doi:10.1021/acs.chemmater.8b03130.
Pal, Koushik, He, Jiangang, & Wolverton, C. Bonding Hierarchy Gives Rise to High Thermoelectric Performance in Layered Zintl Compound BaAu2P4. United States. https://doi.org/10.1021/acs.chemmater.8b03130
Pal, Koushik, He, Jiangang, and Wolverton, C. Fri .
"Bonding Hierarchy Gives Rise to High Thermoelectric Performance in Layered Zintl Compound BaAu2P4". United States. https://doi.org/10.1021/acs.chemmater.8b03130. https://www.osti.gov/servlets/purl/1543613.
@article{osti_1543613,
title = {Bonding Hierarchy Gives Rise to High Thermoelectric Performance in Layered Zintl Compound BaAu2P4},
author = {Pal, Koushik and He, Jiangang and Wolverton, C.},
abstractNote = {The search for new thermoelectric materials has gained rapid progress in recent years as thermoelectric technology offers the potential for environmentally friendly and sustainable energy conversion methods from waste heat to electricity. In this work, we use first-principles calculations based on density functional theory to predict high thermoelectric performance in BaAu2P4, a layered Zintl compound with a small band gap. BaAu2P4 exhibits crystallographic heterogeneity in which rigid [Au2P4]2– units are separated by layers of Ba2+ cations, which are bonded relatively weakly to the lattice through electrostatic interactions. The phosphorus atoms are covalently bonded to each other and form infinite chains within the crystal. While the phosphorus chains facilitate large electrical conductivity, the presence of multiple bands near the Fermi level gives rise to an enhanced Seebeck coefficient. On the other hand, the loosely bound Ba along with Au strongly scatter the heat carrying acoustic phonons, significantly reducing the lattice thermal conduction along the stacking direction. As a consequence of this bonding hierarchy (i.e., coexisting rigid and fluctuating sublattices), BaAu2P4 exhibits a large power factor and low lattice thermal conductivity, which results in a high thermoelectric figure of merit ($zT$). Thus, our findings should encourage the exploration of new thermoelectric materials in the family of layered compounds with small band gaps and crystallographic heterogeneity.},
doi = {10.1021/acs.chemmater.8b03130},
journal = {Chemistry of Materials},
number = 21,
volume = 30,
place = {United States},
year = {Fri Oct 12 00:00:00 EDT 2018},
month = {Fri Oct 12 00:00:00 EDT 2018}
}
Web of Science
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