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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null (Ed.)In the past decade, great efforts have been devoted to the development of organic–inorganic hybrid perovskites for achieving efficient photovoltaics, but less attention has been paid to their thermoelectric applications. In this study, for the first time, we report the thermoelectric performance of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4-TCNQ) doped NH 2 CHNH 2 SnI 3 (FASnI 3 ) thin films. It is found that the electrical conductivities of the F4-TCNQ doped FASnI 3 thin films increase and then decrease along with increased doping levels of F4-TCNQ. Systematic studies indicate that enhanced electrical conductivities are attributed to the increased charge carrier concentrations and mobilities and superior film morphologies of the F4-TCNQ doped FASnI 3 thin films, and decreased electrical conductivities originate from the cracks and poor film morphology of the F4-TCNQ doped FASnI 3 thin films induced by excess F4-TCNQ dopants. The quantitative thermal conductivity scanning thermal microscopy studies reveal that the F4-TCNQ doped FASnI 3 thin films exhibit ultralow thermal conductivities. Moreover, the thermoelectric performance of the F4-TCNQ doped FASnI 3 thin films is investigated. It is found that the F4-TCNQ doped FASnI 3 thin films exhibit a Seebeck coefficient of ∼310 μV K −1 , a power factor of ∼130 μW m −1 K −2 and a ZT value of ∼0.19 at room temperature. All these results demonstrate that our studies open a door for exploring cost-effective less-toxic organic–inorganic hybrid perovskites in heat-to-electricity conversion applications at room temperature.more » « less
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/C9NA00605B
