Recent Progress on Diamondoid Cu2SnSe3 Thermoelectric Materials: A Review

doi:10.1007/s40195-024-01798-7

摘要/Abstract

Abstract:

Due to its unique electronic and thermal transport properties, diamondoid Cu₂SnSe₃ has garnered significant attention as a promising thermoelectric material. Over the past decade, numerous reports have demonstrated ZT exceeding 1.0 in this system, a benchmark for thermoelectric performance. In this paper, we summarize recent progress in Cu₂SnSe₃ thermoelectrics and introduce various strategies for optimizing its electrical and thermal transport properties. We review recent discoveries concerning crystal symmetry and electronic structure, and present a collection of reports on enhancing electronic transport properties through band structure modification. Additionally, we provide insights into how lattice dynamics and microstructure influence phonon transport behaviors and highlight the thermal conductivity reduction achieved through comprehensive phonon scattering mechanisms. Lastly, we outline the current challenges facing by Cu₂SnSe₃ and propose innovative ideas for future research.

Key words: Thermoelectric performance, Crystal structure, Carrier concentration, Band convergence, Lattice thermal conductivity, Scattering mechanism

. [J]. 金属学报英文版, 2025, 38(5): 707-719.

Pengpeng Chen, Hongyao Xie, Li-Dong Zhao. Recent Progress on Diamondoid Cu₂SnSe₃ Thermoelectric Materials: A Review[J]. Acta Metallurgica Sinica (English Letters), 2025, 38(5): 707-719.

图/表 8

Fig. 1 Structure evolution and thermoelectric performance of Cu2SnSe3 compounds. A Lattice structures of Cu2SnSe3, Cu5Sn2Se7 and Cu2SnSe4. B The ZT value of different Cu2SnSe3 compounds varies as the function of reported years, showing the gradual development for Cu2SnSe3 thermoelectrics [82,86,88]

Table 1 Physical properties of Cu2SnSe3 semiconductor at 300 K

Properties	Results
Density (g cm⁻³)	5.7
Melting point (K)	960
Molecular mass (g mol⁻¹)	482.7
Crystal structure	Monoclinic or cubic
Space group	Cc (No. 9) or $F\overline{4}3m$ (No. 216)
Lattice parameters	Monoclinic: a = 6.97 Å, b = 12.05 Å, c = 6.95 Å, β = 109.2°, α = γ = 90° Cubic: a = b = c = 5.67 Å, α = β = γ = 90°
Conduction type	p
Effective carrier mass	1.2m₀
Carrier concentration (cm⁻³)	10¹⁸-10¹⁹
Carrier mobility (cm² V⁻¹ s⁻¹)	4-870
Bandgap energy (eV)	0.85
Thermal conductivity (W m⁻¹ K⁻¹)	2.7
Debye temperature (K)	190
Sound velocity (m s⁻¹)	1600

Fig. 2 Improvement of electrical properties due to acceptor doping in Cu2SnSe3. Temperature dependence of A electrical conductivity, B Seebeck coefficient for different doped materials. C The Pisarenko plot, the solid curve is the theoretical value calculated via SPB model with m* = 1.3m0. D The carrier concentration dependence of carrier mobility. Temperature dependence of E power factor and F ZT values for different Cu2SnSe3 compounds [28,33,37,51,52,53,54,55,56,57,58]

Fig. 3 Triply degenerate electronic bands due to pseudocubic supercell in the tetragonal chalcopyrite and the impact on the Cu2-xAgxSn1-yMgySe3 samples due to band degeneracy. Crystal and electronic band structure of A cubic sphalerite and B I-III-VI2 ternary chalcopyrite. Γ4v is a non-degenerate band and Γ5v is a doubly degenerate band. ∆CF is the energy split on the top of Γ4v and Γ5v bands. C The ZT value as a function of ∆CF at 700 K. D The band structure of monoclinic and cubic Cu2SnSe3, showing the band degeneracy at Γ points from monoclinic to cubic symmetry in Cu2SnSe3 [1]. E The Pisarenko plot of Cu2-xAgxSn1-yMgySe3(x = 0, 0.05, 0.15; y = 0, 0.04, 0.08) and temperature dependence of F Seebeck coefficient and G ZT values for Cu2-xAgxSn1-yMgySe3 [26]

Fig. 4 Gradually enhanced electrical performance and the band structure evolution of Cu2SnSe3 with S alloying and In doping [73]. Temperature dependence of A electrical conductivity and B Seebeck coefficient for Cu2Sn1-yInySe3-xSx. C Room temperature carrier concentration and carrier mobility as the function of In content in Cu2SnSe2.7S0.3. D Pisarenko plot of Cu2Sn1-yInySe3-xSx (x = 0, 0.03, 0.05; y = 0, 0.09, 0.18). E Temperature dependence of power factor for Cu2Sn1-yInySe3-xSx. The band structures of F Cu2SnSe3, G Cu2SnSe2.5S0.5, and H Cu2Sn1-yInySe2.6875S0.3125. The red dashed lines denote the Fermi levels with different doping (y = 0, 0.0625, 0.125, 0.1875). I Temperature dependence of ZT values for Cu2Sn1-yInySe3-xSx

Fig. 5 Lattice thermal conductivity reduction due to introduction of point defects, dislocations and nanostructures. A Temperature dependence of lattice thermal conductivity in Cu2SnSe3 with different acceptors. B Lattice thermal conductivity reduction in (Ag,Ga) and (Ag,Ga,Na) co-doped Cu2SnSe3 at 823 K. TEM images show that dislocation arrays and nanoprecipitates in the (Ag,Ga,Na) co-doped sample. C Temperature dependence of lattice thermal conductivity for Cu2SnSe3. The thermal conductivity reduces with increasing ball milling time, implying the effective of enhancing phonon scattering through grain refining. The experimental results are in good agreement with theoretical calculations. D SEM images show the variation of nanoparticle size as ball milling time [26,28,37,52,53,57,82,87]

Fig. 6 Lattice thermal conductivity reduction due to full-scale scattering mechanism in Cu2SnSe3 [88]. A The temperature-dependent thermal conductivity of Cu2Sn1-2xFexInxSe3-f wt%Ag2Se (x = 0, 0.02, 0.04, 0.06; f = 0–5). B The spectral lattice thermal conductivity calculated by Debye–Callaway model. Regions (I) to (V) represent the influence of different scattering mechanism. The purple dashed lines denote middle- and low-frequency phonons (MLFPs). C The spectral lattice thermal conductivity of Cu2Sn0.88Fe0.06In0.06Se3-5 wt%Ag2Se with different nanoinclusions. The ratio of volume to surface area of nanoinclusions is denoted as $\xi$. D and E TEM images show high-dense stacking faults and oriented nanoneedles with random distributions in Cu2Sn0.88Fe0.06In0.06Se3-5 wt%Ag2Se

Fig. 7 Thermoelectric performance of Cu2SnSe3 and other Cu-based diamond-like compounds. A Temperature dependence of ZT values for different optimized Cu2SnSe3. B A comparison of ZT values for different Cu-based diamond-like compounds [23,25,26,29,34,35,41,89,90]

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Recent Progress on Diamondoid Cu₂SnSe₃ Thermoelectric Materials: A Review

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