Band Engineering Through Pb-Doping of Nanocrystal Building Blocks to Enhance Thermoelectric Performance in Cu3SbSe4
Article
Wan, Shanhong, Xiao, Shanshan, Li, Mingquan, Wang, Xin, Lim, Khak Ho, Hong, Min, Ibanez, Maria, Cabot, Andreu and Liu, Yu. 2024. "Band Engineering Through Pb-Doping of Nanocrystal Building Blocks to Enhance Thermoelectric Performance in Cu3SbSe4." Small Methods. 8 (8). https://doi.org/10.1002/smtd.202301377
Article Title | Band Engineering Through Pb-Doping of Nanocrystal Building Blocks to Enhance Thermoelectric Performance in Cu3SbSe4 |
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ERA Journal ID | 214172 |
Article Category | Article |
Authors | Wan, Shanhong, Xiao, Shanshan, Li, Mingquan, Wang, Xin, Lim, Khak Ho, Hong, Min, Ibanez, Maria, Cabot, Andreu and Liu, Yu |
Journal Title | Small Methods |
Journal Citation | 8 (8) |
Article Number | 2301377 |
Number of Pages | 10 |
Year | 2024 |
Publisher | Wiley-VCH Verlag GmbH & Co. KGaA |
Place of Publication | Germany |
ISSN | 2366-9608 |
Digital Object Identifier (DOI) | https://doi.org/10.1002/smtd.202301377 |
Web Address (URL) | https://onlinelibrary.wiley.com/doi/10.1002/smtd.202301377 |
Abstract | Developing cost-effective and high-performance thermoelectric (TE) materials to assemble efficient TE devices presents a multitude of challenges and opportunities. Cu3SbSe4 is a promising p-type TE material based on relatively earth abundant elements. However, the challenge lies in its poor electrical conductivity. Herein, an efficient and scalable solution-based approach is developed to synthesize high-quality Cu3SbSe4 nanocrystals doped with Pb at the Sb site. After ligand displacement and annealing treatments, the dried powders are consolidated into dense pellets, and their TE properties are investigated. Pb doping effectively increases the charge carrier concentration, resulting in a significant increase in electrical conductivity, while the Seebeck coefficients remain consistently high. The calculated band structure shows that Pb doping induces band convergence, thereby increasing the effective mass. Furthermore, the large ionic radius of Pb2+ results in the generation of additional point and plane defects and interphases, dramatically enhancing phonon scattering, which significantly decreases the lattice thermal conductivity at high temperatures. Overall, a maximum figure of merit (zTmax) ≈ 0.85 at 653 K is obtained in Cu3Sb0.97Pb0.03Se4. This represents a 1.6-fold increase compared to the undoped sample and exceeds most doped Cu3SbSe4-based materials produced by solid-state, demonstrating advantages of versatility and cost-effectiveness using a solution-based technology. |
Keywords | band engineering |
Contains Sensitive Content | Does not contain sensitive content |
ANZSRC Field of Research 2020 | 401605. Functional materials |
Public Notes | The accessible file is the accepted version of the paper. Please refer to the URL for the published version. |
Byline Affiliations | Hefei University of Technology, China |
Jiangsu Normal University, China | |
Zhejiang University, China | |
School of Engineering | |
Centre for Future Materials | |
Institute of Science and Technology Austria, Austria | |
Catalonia Institute for Energy Research (IREC), Spain |
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Under embargo until 28 Dec 2024
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