There has been a growing interest in solution-phase routes to thermoelectric materials due to the decreased costs and novel device architectures that these methods enable. Many excellent thermoelectric materials are metal chalcogenide semiconductors and the ability to create soluble metal chalcogenide semiconductor precursors using thiol–amine solvent mixtures was recently demonstrated by others. In this paper, we report the first thermoelectric property measurements on metal chalcogenide thin films made in this manner. We create Cu 2−x Se y S 1−y and Ag-doped Cu 2−x Se y S 1−y thin films and study the interrelationship between their composition and room temperature thermoelectric properties. We find that the precursor annealing temperature affects the metal : chalcogen ratio, and leads to charge carrier concentration changes that affect the Seebeck coefficient and electrical conductivity. Increasing the Se : S ratio increases electrical conductivity and decreases the Seebeck coefficient. We also find that incorporating Ag into the Cu 2−x Se y S 1−y film leads to appreciable improvements in thermoelectric performance by increasing the Seebeck coefficient and decreasing thermal conductivity. Overall, we find that the room temperature thermoelectric properties of these solution-processed materials are comparable to measurements on Cu 2−x Se alloys made via conventional thermoelectric material processing methods. Achieving parity between solution-phase processing and conventional processing is an important milestone and demonstrates the promise of this binary solvent approach as a solution-phase route to thermoelectric materials.
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High-performance thermoelectric silver selenide thin films cation exchanged from a copper selenide template
Over the past decade, Ag 2 Se has attracted increasing attention due to its potentially excellent thermoelectric (TE) performance as an n-type semiconductor. It has been considered a promising alternative to Bi–Te alloys and other commonly used yet toxic and/or expensive TE materials. To optimize the TE performance of Ag 2 Se, recent research has focused on fabricating nanosized Ag 2 Se. However, synthesizing Ag 2 Se nanoparticles involves energy-intensive and time-consuming techniques with poor yield of final product. In this work, we report a low-cost, solution-processed approach that enables the formation of Ag 2 Se thin films from Cu 2−x Se template films via cation exchange at room temperature. Our simple two-step method involves fabricating Cu 2−x Se thin films by the thiol-amine dissolution of bulk Cu 2 Se, followed by soaking Cu 2−x Se films in AgNO 3 solution and annealing to form Ag 2 Se. We report an average power factor (PF) of 617 ± 82 μW m −1 K −2 and a corresponding ZT value of 0.35 at room temperature. We obtained a maximum PF of 825 μW m −1 K −2 and a ZT value of 0.46 at room temperature for our best-performing Ag 2 Se thin-film after soaking for 5 minutes. These high PFs have been achieved via full solution processing without hot-pressing.
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- NSF-PAR ID:
- 10164598
- Date Published:
- Journal Name:
- Nanoscale Advances
- Volume:
- 2
- Issue:
- 1
- ISSN:
- 2516-0230
- Page Range / eLocation ID:
- 368 to 376
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/C9NA00605B
