Solubility design leading to high figure of merit in low-cost Ce-CoSb₃ skutterudites
Abstract
CoSb₃-based filled skutterudite has emerged as one of the most viable candidates for thermoelectric applications in automotive industry. However, the scale-up commercialization of such materials is still a challenge due to the scarcity and cost of constituent elements. Here we study Ce, the most earth abundant and low-cost rare earth element as a single-filling element and demonstrate that, by solubility design using a phase diagram approach, the filling fraction limit (FFL) x in CeₓCo4Sb₁₂ can be increased more than twice the amount reported previously (x=0.09). This ultra-high FFL (x=0.20) enables the optimization of carrier concentration such that no additional filling elements are needed to produce a state of the art n-type skutterudite material with a zT value of 1.3 at 850 K before nano-structuring. The earth abundance and low cost of Ce would potentially facilitate a widespread application of skutterudites.
Additional Information
© 2015 Macmillan Publishers Limited. This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. Received 16 March 2015; Accepted 21 May 2015; Published 20 July 2015. We acknowledge the financial support of Solid-State Solar-Thermal Energy Conversion Center (S3TEC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0001299. We also acknowledge the financial support of National Science Council of Taiwan (NSC101-3113-P-008-001). We thank Yulong Li, Xun Shi, Lidong Chen of Shanghai Institute of Ceramics, Chinese Academy of Sciences for ZEM-3 measurements. This work made use of the EPIC facility (NUANCE Center-Northwestern University), which has received support from the MRSEC program (NSF DMR-1121262) at the Materials Research Center; the Nanoscale Science and Engineering Center (NSF EEC–0647560) at the International Institute for Nanotechnology; and the State of Illinois, through the International Institute for Nanotechnology. The LEAP at the Northwestern University Center for Atom-Probe Tomography (NUCAPT) was acquired and upgraded with equipment grants from the MRI program of the National Science Foundation (grant number DMR-0420532) and the DURIP program of the Office of Naval Research (grant numbers N00014-0400798, N00014-0610539, N00014-0910781). NUCAPT is supported by the National Science Foundation's MRSEC program (grant number DMR-1121262). Additional instrumentation at NUCAPT was supported by the Initiative for Sustainability and Energy at Northwestern (ISEN). We acknowledge further support from the International S&T Cooperation Program of China (2015DFA51050). Thank you to Dieter Isheim for critical conversations regarding experimental set-up and data analysis. Author contributions: Y.T. and G.J.S. contributed equally to design the study and write the manuscript. Y.T. contributed to sample synthesis, structure characterization and property measurements. R.H. contributed to APT analysis and manuscript refinement. S.W.C. contributed to the discussion of phase diagram results. Y.T., R.H. and G.J.S. contributed to the thumbnail figure design.Attached Files
Published - ncomms8584.pdf
Supplemental Material - ncomms8584-s1.pdf
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Additional details
Additional titles
- Alternative title
- Solubility design leading to high figure of merit in low-cost Ce-CoSb3 skutterudites
Identifiers
- PMCID
- PMC4518255
- Eprint ID
- 59942
- Resolver ID
- CaltechAUTHORS:20150828-084633086
Funding
- Department of Energy (DOE)
- DE-SC0001299
- National Science Council (Taipei)
- NSC101-3113-P-008-001
- NSF
- DMR-1121262
- NSF
- EEC-0647560
- State of Illinois
- NSF
- DMR-0420532
- Office of Naval Research (ONR)
- N00014-0400798
- Office of Naval Research (ONR)
- N00014-0610539
- Office of Naval Research (ONR)
- N00014-0910781
- Northwestern University
- International Science and Technology Cooperation Program of China
- 2015DFA51050
Dates
- Created
-
2015-09-11Created from EPrint's datestamp field
- Updated
-
2022-05-26Created from EPrint's last_modified field