Achieving zT > 1 in Inexpensive Zintl Phase Ca 9Zn4+xSb9 by Phase Boundary Mapping
Abstract
Complex multinary compounds (ternary, quaternary, and higher) offer countless opportunities for discovering new semiconductors for applications such as photovoltaics and thermoelectrics. However, controlling doping has been a major challenge in complex semiconductors as there are many possibilities for charged intrinsic defects (e.g., vacancies, interstitials, antisite defects) whose energy depends on competing impurity phases. Even with compounds with no apparent deviation from a stoichiometric nominal composition, such defects commonly lead to free carrier concentrations in excess of 1020 cm-3. Nevertheless, by slightly altering the nominal composition, these defect concentrations can be tuned with small variation of the chemical potentials (composition) of each element. While the variation of chemical composition is undetectable, it is shown that the changes can be inferred by mapping (in nominal composition space) the boundaries where different competing impurity phases form. In the inexpensive Zintl compound Ca9Zn4+xSb9, the carrier concentrations can be finely tuned within three different three-phase regions by altering the nominal composition (x = 0.2–0.8), enabling the doubling of thermoelectric performance (zT). Because of the low thermal conductivity, the zT can reach as high as 1.1 at 875 K, which is one of the highest among the earth abundant p-type thermoelectrics with no ion conducting.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States); California Institute of Technology (CalTech), Pasadena, CA (United States)
- Northwestern Univ., Evanston, IL (United States)
- Dalhousie Univ., Halifax, NS (Canada)
- California Institute of Technology (CalTech), Pasadena, CA (United States). Jet Propulsion Lab. (JPL)
- Michigan State Univ., East Lansing, MI (United States)
- California Institute of Technology (CalTech), Pasadena, CA (United States); Northwestern Univ., Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1533015
- Alternate Identifier(s):
- OSTI ID: 1401530
- Grant/Contract Number:
- FG02-07ER46433; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Volume: 27; Journal Issue: 20; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; chemistry; science & technology; materials science; physics; energy conversion; phase boundary mapping; semiconductors; thermoelectrics; Zintl phases
Citation Formats
Ohno, Saneyuki, Aydemir, Umut, Amsler, Maximilian, Pöhls, Jan-Hendrik, Chanakian, Sevan, Zevalkink, Alex, White, Mary Anne, Bux, Sabah K., Wolverton, Chris, and Snyder, G. Jeffrey. Achieving zT > 1 in Inexpensive Zintl Phase Ca 9Zn4+xSb9 by Phase Boundary Mapping. United States: N. p., 2017.
Web. doi:10.1002/adfm.201606361.
Ohno, Saneyuki, Aydemir, Umut, Amsler, Maximilian, Pöhls, Jan-Hendrik, Chanakian, Sevan, Zevalkink, Alex, White, Mary Anne, Bux, Sabah K., Wolverton, Chris, & Snyder, G. Jeffrey. Achieving zT > 1 in Inexpensive Zintl Phase Ca 9Zn4+xSb9 by Phase Boundary Mapping. United States. https://doi.org/10.1002/adfm.201606361
Ohno, Saneyuki, Aydemir, Umut, Amsler, Maximilian, Pöhls, Jan-Hendrik, Chanakian, Sevan, Zevalkink, Alex, White, Mary Anne, Bux, Sabah K., Wolverton, Chris, and Snyder, G. Jeffrey. Wed .
"Achieving zT > 1 in Inexpensive Zintl Phase Ca 9Zn4+xSb9 by Phase Boundary Mapping". United States. https://doi.org/10.1002/adfm.201606361. https://www.osti.gov/servlets/purl/1533015.
@article{osti_1533015,
title = {Achieving zT > 1 in Inexpensive Zintl Phase Ca 9Zn4+xSb9 by Phase Boundary Mapping},
author = {Ohno, Saneyuki and Aydemir, Umut and Amsler, Maximilian and Pöhls, Jan-Hendrik and Chanakian, Sevan and Zevalkink, Alex and White, Mary Anne and Bux, Sabah K. and Wolverton, Chris and Snyder, G. Jeffrey},
abstractNote = {Complex multinary compounds (ternary, quaternary, and higher) offer countless opportunities for discovering new semiconductors for applications such as photovoltaics and thermoelectrics. However, controlling doping has been a major challenge in complex semiconductors as there are many possibilities for charged intrinsic defects (e.g., vacancies, interstitials, antisite defects) whose energy depends on competing impurity phases. Even with compounds with no apparent deviation from a stoichiometric nominal composition, such defects commonly lead to free carrier concentrations in excess of 1020 cm-3. Nevertheless, by slightly altering the nominal composition, these defect concentrations can be tuned with small variation of the chemical potentials (composition) of each element. While the variation of chemical composition is undetectable, it is shown that the changes can be inferred by mapping (in nominal composition space) the boundaries where different competing impurity phases form. In the inexpensive Zintl compound Ca9Zn4+xSb9, the carrier concentrations can be finely tuned within three different three-phase regions by altering the nominal composition (x = 0.2–0.8), enabling the doubling of thermoelectric performance (zT). Because of the low thermal conductivity, the zT can reach as high as 1.1 at 875 K, which is one of the highest among the earth abundant p-type thermoelectrics with no ion conducting.},
doi = {10.1002/adfm.201606361},
journal = {Advanced Functional Materials},
number = 20,
volume = 27,
place = {United States},
year = {Wed Mar 29 00:00:00 EDT 2017},
month = {Wed Mar 29 00:00:00 EDT 2017}
}
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