Journal
MATERIALS
Volume 15, Issue 23, Pages -Publisher
MDPI
DOI: 10.3390/ma15238297
Keywords
chalcogenides; thermoelectrics; X-ray diffraction; Raman; intercalation
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Layered TiS2 intercalated with linear alkylamines has shown promising performance as a flexible n-type thermoelectric material, but its thermal and environmental stability remains a challenge. This study demonstrates that amine-intercalated TiS2 prepared by mechanochemical process is prone to chemical decomposition through sulfur exsolution, and molecular oxygen is likely to mediate this reaction. Computational analysis suggests the formation of Ti-N adducts as a result of amine groups substituting for sulfur vacancies.
Layered TiS2 intercalated with linear alkylamines has recently attracted significant interest as a model compound for flexible n-type thermoelectric applications, showing remarkably high power factors at room temperature. The thermal and, particularly, environmental stability of such materials is, however, a still an open challenge. In this paper, we show that amine-intercalated TiS2 prepared by a simple mechanochemical process is prone to chemical decomposition through sulfur exsolution, and that the presence of molecular oxygen is likely to mediate the decomposition reaction. Through computational analysis of the possible reaction pathways, we propose that Ti-N adducts are formed as a consequence of amine groups substituting for S vacancies on the internal surfaces of the S-Ti-S layers. These findings provide insights for possible future applications of similar hybrid compounds as devices operating in ambient conditions, and suggest isolating them from atmospheric oxygen.
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