Interaction between Cu–S-Based Sphalerite-like Frameworks and Interstitial Cations in Colusite-Based Thermoelectric Materials

Cu–S-based multicomponent compounds with sphalerite-like frameworks have garnered attention as midtemperature p-type thermoelectric (TE) materials. Their valence bands, primarily comprising Cu–S hybridized orbitals, control electronic properties. Herein, for colusites Cu26Tr2M6S32 (Tr = V, Nb, and Ta; M = Ge and Sn), we investigate the distinctive interaction between the Cu–S-based sphalerite-like framework and Tr at the interstitial tetrahedral sites to improve the Seebeck coefficient (S). According to ab initio calculations, the d(t2) and d(e) orbitals of Tr interact with the valence band maxima at the Γ and M points, respectively. The hybridization between the Tr-t2 and S orbitals (under the presence of Tr), along with structural modifications, reduces the energy of the Γ band maximum toward the Fermi level, thereby increasing S. This understanding is expected to be a foundation for further advancements in the TE properties of Cu–S-based compounds.

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Publication Details

Journal
ACS Applied Energy Materials
Published
2025-03-08
DOI
https://doi.org/10.1021/acsaem.4c03142
Primary Topic
Advanced Thermoelectric Materials and Devices
Type
article
Field-Weighted Citation Impact
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article

Interaction between Cu–S-Based Sphalerite-like Frameworks and Interstitial Cations in Colusite-Based Thermoelectric Materials

Susumu Fujii, Seiya Takahashi, Koichiro Suekuni, M. Ohta et al.
ACS Applied Energy Materials
Advanced Thermoelectric Materials and Devices
article

Interaction between Cu–S-Based Sphalerite-like Frameworks and Interstitial Cations in Colusite-Based Thermoelectric Materials

Susumu Fujii, Seiya Takahashi, Koichiro Suekuni, M. Ohta, Hidetaka Kasai, Michitaka Ohtaki, Philipp Sauerschnig, Masato Yoshiya, Emmanuel Guilmeau, Eiji Nishibori, S. Ochi, Takashi Hagiwara, Kosuke Naemura
article en

Abstract

Cu–S-based multicomponent compounds with sphalerite-like frameworks have garnered attention as midtemperature p-type thermoelectric (TE) materials. Their valence bands, primarily comprising Cu–S hybridized orbitals, control electronic properties. Herein, for colusites Cu26Tr2M6S32 (Tr = V, Nb, and Ta; M = Ge and Sn), we investigate the distinctive interaction between the Cu–S-based sphalerite-like framework and Tr at the interstitial tetrahedral sites to improve the Seebeck coefficient (S). According to ab initio calculations, the d(t2) and d(e) orbitals of Tr interact with the valence band maxima at the Γ and M points, respectively. The hybridization between the Tr-t2 and S orbitals (under the presence of Tr), along with structural modifications, reduces the energy of the Γ band maximum toward the Fermi level, thereby increasing S. This understanding is expected to be a foundation for further advancements in the TE properties of Cu–S-based compounds.

ACS Applied Energy MaterialsVol. 8(6)
Kyushu University (JP), University of Tsukuba (JP), École Nationale Supérieure d'Ingénieurs de Caen (FR), Green Tech Labs (United States) (US), Normandie Université (FR), Zero Emissions Resource Organisation (NO), National Institute of Advanced Industrial Science and Technology (JP), The University of Osaka (JP), Université de Caen Normandie (FR)
Openalex Percentile: Top 97%
Advanced Thermoelectric Materials and Devices
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