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Article Dans Une Revue Chemistry of Materials Année : 2023

Pseudobinary approach to the discovery and design of copper-based sulfides

Koichiro Suekuni
  • Fonction : Auteur correspondant
Erik Elkaim
Rabih Al Rahal Al Orabi
Marco Fornari
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Hikaru Saito
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Michihiro Ohta
Yui Kanemori
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Résumé

Copper-based sulfide semiconductors with the structure based on a sphalerite-like network can provide environmentally sound solutions to thermoelectric and photovoltaic energy conversion at a low cost. In this study, we report the synthesis and characterization of a copper-based sulfide, Cu$_{30}$Ti$_6$Sb$_2$S$_{32}$, discovered within the pseudobinary Cu$_3$SbS$_4$-Cu$_4$TiS$_4$ system. This new compound crystallizes in a colusite-like cubic structure, which is characterized by "interstitial" Ti atoms forming tetrahedral-octahedral [TiS$_4$]Cu$_6$ complexes linearly arranged within the Cu-S corner-sharing matrix. The [TiS$_4$]Cu$_6$ unit arrangement distinguishes the crystal structures of Cu$_{26}$Ti$_2$Sb$_6$S$_{32}$ (isolated units, 0D linkage), Cu$_{30}$Ti$_6$Sb$_2$S$_{32}$ (chain of linked units, 1D), and Cu$_4$TiS$_4$ (plane of linked units, 2D). We emphasize the semiconducting nature and the low thermal conductivity. The electronic structure and vibrational properties are investigated by the combination of experiments and first-principles calculations. We demonstrate that a design approach based on the pseudobinary composition, here, with the generic formula (Cu$_3$SbS$_4$)$_{1-x}$) (Cu$_4$TiS$_4$)$_x$, is a fruitful direction for the discovery of new copper-based sulfides with tunable transport properties.

Domaines

Matériaux
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Dates et versions

hal-04237383 , version 1 (18-11-2023)

Identifiants

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Takashi Hagiwara, Koichiro Suekuni, Pierric Lemoine, Carmelo Prestipino, Erik Elkaim, et al.. Pseudobinary approach to the discovery and design of copper-based sulfides. Chemistry of Materials, 2023, 35 (18), pp.7554-7563. ⟨10.1021/acs.chemmater.3c01135⟩. ⟨hal-04237383⟩
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