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SnS and SnSe are layered materials with similar crystal structures, of which SnSe has attracted attention as a high-performance thermoelectric material thanks to its high phonon anharmonicity. However, sulfur is less toxic and more abundant than selenium, making SnS an environmentally friendly and sustainable thermoelectric material, although its thermoelectric conversion efficiency is very low (dimensionless figure of merit, ZT, ~ 0.01). Attempts to improve the ZT of SnS are ongoing, with doping of impurity elements such as Na, Ag and Se being the main methods used. However, the effects have been inconsistent and controversial. In this study, SnS nanoparticles (NPs), Ag-doped SnS NPs and Ag-doped SnS1−xSex NPs with S partially replaced by Se were chemically synthesized. These NPs were then sintered by hot-pressing and the correlation between the electronic and thermal transport properties and structure of the sintered pellets was investigated in detail. As a result, it was found that when Ag-doped SnS NPs were sintered, two types of Ag were present in the sintered pellets: one in the form of segregated Ag-rich nanoprecipitates, and the other in the form of interlayer intercalated Ag ions. On the other hand, when Ag-doped SnS1−xSex NPs were sintered, Se was found to form a homogeneous solid solution. The effects of these three impurity-derived structures (Ag-rich nanoprecipitates, intercalated Ag+ and Se in solid solution in SnS) on the electronic and thermal conduction properties were investigated. The ZT values were improved by Ag-doping and Se-doping, and the ZT values for SnS doped with 1.5 at% Ag (SnS:Ag) and SnS0.9Se0.1:Ag, in which SnS:Ag was further doped with Se (10 at% with respect to S), were 0.09 at 666 K and 0.14 at 667 K, respectively.

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  This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Energy Materials, copyright © 2024 The Authors. Published by American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsaem.4c00487

Keyword: thermoelectric materials, electron microscopy

Date published: 2024-05-27

Publisher: American Chemical Society (ACS)

Journal:

• ACS Applied Energy Materials (ISSN: 25740962) vol. 7 issue. 10 p. 4484-4493

Funding:

• Thermal and Electric Energy Technology Foundation
• Japan Society for the Promotion of Science 19H02440

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4688

First published URL: https://doi.org/10.1021/acsaem.4c00487

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Updated at: 2025-05-16 08:30:14 +0900

Published on MDR: 2025-05-16 08:20:26 +0900