Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.125
Publication date: 22nd December 2022
Ternary alkali-metal dichalcogenides {AMeE (A = Li, Na, K, Rb, Cs, Cu, Ag, Tl; Me= Metals E = S, Se, Te} are an intriguing class of semiconductors with tremendous technological potential.[1,2] For more than a decade, the compounds of these structural types have been explored as potent thermoelectric materials.[3] High-temperature solid-state synthesis is typically employed to synthesize alkali metal-based chemicals. However, it naturally forms highly aggregated, polydisperse particles with little control over different phases and understanding in terms of mechanistic insights. In this case, solution phase synthesis can be advantageous to form uniform nanocrystals. Herein, we develop a facile colloidal hot-injection strategy to synthesize shape and size-tunable caesium copper selenide nanocrystals comprising earth-abundant and non-toxic elements. Ex-situ mechanistic investigation reveals that the NCs formation is driven by the dissolution of binary Cu2-xSe, followed by the incorporation of Cs+ to form the ternary CsCu5Se3. A thorough case study on the addition of alkyl acid and amine ligands indicates that the involvement of both acid and amine functionality is required to synthesize pure-phase NCs. The current study also reveals that variation in the alkyl chain length of amines influences the size, shape, and formation of distinct phases. Furthermore, the nanocrystals were consolidated as pellets to study thermoelectric transport properties showing ultra-low thermal conductivity of 0.65 W/mK at 728 K, promising for improved thermoelectric applications. Altogether, the present study provides a mechanistic understanding of the factors that impact the synthesis of materials based on alkali metal chalcogenides and exhibit their promising thermoelectric properties.
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