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Wang, W.; Bo, L.; Zhu, J.; Zhao, D. Copper-Based Diamond-like Thermoelectric Compounds. Encyclopedia. Available online: (accessed on 14 June 2024).
Wang W, Bo L, Zhu J, Zhao D. Copper-Based Diamond-like Thermoelectric Compounds. Encyclopedia. Available at: Accessed June 14, 2024.
Wang, Wenying, Lin Bo, Junliang Zhu, Degang Zhao. "Copper-Based Diamond-like Thermoelectric Compounds" Encyclopedia, (accessed June 14, 2024).
Wang, W., Bo, L., Zhu, J., & Zhao, D. (2023, May 10). Copper-Based Diamond-like Thermoelectric Compounds. In Encyclopedia.
Wang, Wenying, et al. "Copper-Based Diamond-like Thermoelectric Compounds." Encyclopedia. Web. 10 May, 2023.
Copper-Based Diamond-like Thermoelectric Compounds

Copper-based diamond-like compounds (CBDL) compounds contain a large number of family members, which include ternary I–III–VI2 chalcopyrites, I3–V–VI4 stannites, I2–IV–VI3 stannites, quaternary I2–II–IV–VI4 compounds, and even large-cell Cu10B2C4D13 tetrahedrites and Cu26P2Q6S32 colusites.

thermoelectric copper-based diamond-like compounds zT

1. Introduction

The attractive capability of thermoelectric (TE) materials in actualizing the conversion between temperature gradient and electrical power makes them strong candidates for waste-heat recovery as well as solid-state refrigeration [1][2][3]. The practical and widespread application of TE technology strongly relies on the development of high-performance TE materials, where the TE performance of materials is evaluated by a dimensionless figure of merit, zT = α2σT/κ. The TE parameters α and σ are the Seebeck coefficient and electrical conductivity which, respectively, constitute the power factor, PF = α2σ, used to evaluate electrical conductivity characteristics. Parameter T is the Kelvin thermodynamic temperature, while κ refers to the total thermal conductivity, which is composed of two major contributions from the charge carriers (κE) and the lattice (κL), respectively. From a computational perspective, the most ideal high-performance TE material should have a large α, high σ as well as a low κ value. What cannot be avoided is the strong coupling between thermoelectric parameters regarding carrier concentration, such as when a high σ means low α and a high κE, limiting the improvement of zT [4][5][6]. In order to achieve high zT in traditional or emerging TE materials, various methods and approaches have been adopted to reduce the correlation between thermal and electrical properties [7][8][9], including defect engineering, size effects, alloying effect and high-entropy engineering, etc. In addition to achieving high performance, the exploration of alternative materials consists of earth-abundant and eco-friendly components to meet the sake of clean and environmental protection is also considered as one of the most popular approaches in TE field [10][11][12][13]. In recent years, diverse bulk TE materials have been widely researched, including liquid-like Cu2(S, Se, Te), silver-based chalcogenides, Sn(Te, S, Se), half-heuslers, etc. [14][15][16].
As an environmentally friendly and promising TE material without precious elements, the performance advantages of copper-based diamond-like TE compounds lie in their high Seebeck coefficient and low thermal conductivity [17][18][19][20][21]. Typical compounds include: Cu3SbSe4, with a high zT of 0.89 at 650 K [19]; Cu2SnSe3, with α of ~250 μV·K−1 in the temperature range of 300–700 K [22]; and CuInTe2, with a κL value as low as 0.3 W·m−1·K−1 [23], etc. Copper-based diamond-like TE compounds are a type of material that conforms to the concept of “phonon-glass electron-crystal” (PGEC) [17] materials, and their crystal structures are usually composed of two sublattices [23][24][25], in which one sublattice constitutes a conductive network, while the other acts as a thermal barrier and is sometimes also known as a charge reservoir. In 2011, Skoug et al. [24] summarized the significance of lone-pair electrons in the Cu-Sb-Se diamond-like system and demonstrated that the low intrinsic κL in compounds came from the interaction of lone-pair electrons with neighboring atoms. Moreover, Skoug et al. [25] also confirmed that the dominant Cu-Se network controlled the electric transport while the Sn orbitals only compensated the system for electrons. Several diamond-like crystal structures evolved from thecubic zincblende structure. Simultaneously, a series of advanced CBDL compounds have been discovered since 2009, most of which have presented outstanding TE properties. The timeline of maximum zTs and the temperature dependence of zTs for selected CBDL compounds. Taking the typical diamond-like compounds of Cu(In, Ga)Te2, Cu3SbSe4, and Cu2SnSe3 as examples, long-term efforts have shown that they all apparently have superior TE transport properties with high zTs that exceed one. For instance, Liu et al. [23] devised a pseudocubic crystal structure in CuInTe2 compounds; thus the highest zT of 1.24 was obtained in Ag-doped CuInTe2 compounds. A peak zT of 1.14 was attained in a Cu2Sn0.90In0.10Se3 compound at 850 K by replacing Sn sites with In. It is also worth noting that a high average zT (zTave) value is desirable for overall TE conversion efficiency. For instance, a high zTmax of 1.67 at 873 K, and a zTave of 0.73, were realized in Cu0.7Ag0.3Ga0.4In0.6Te2 [26]. In the latest research of Zhou’s group [27][28], record-high zTave values of 0.73 and 0.77 were achieved in Cu3SbSe4–based and Cu3SbS4–based materials, respectively, which were also comparable to other state-of-the-art TE compounds. Hence one can see that CBDL compounds are expected to become environmentally friendly candidates for TE applications and to achieve excellent performances.

2. Copper-Based Diamond-like Thermoelectric Compounds

Copper-based diamond-like compounds (CBDL) compounds contain a large number of family members, which include ternary I–III–VI2 chalcopyrites, I3–V–VI4 stannites, I2–IV–VI3 stannites, quaternary I2–II–IV–VI4 compounds, and even large-cell Cu10B2C4D13 tetrahedrites and Cu26P2Q6S32 colusites. The TE properties of selected typical CBDL compounds including zTave, zTmax, α2σ, κL, and carrier concentration (n) at room temperature.
Among CBDL compounds, CuGaTe2 and CuInTe2 are typical Cu–III–VI2 (III = In, Ga; VI = Se, S, Te) chalcopyrites structural compounds which have exhibited excellent thermoelectric properties at higher temperatures. In 2012, Plirdpring et al. [29] achieved a record zT of 1.4 in CuGaTe2 compound at 950 K, which indicated that it was a potential material in the field of TE applications. Comparatively, it was found that CuInTe2 possessed a high zT of 1.18 at 850 K [20]. A large number of studies were conducted to optimize the TE transport behaviors of chalcopyrite-based materials in the following years. Through defect engineering, Pei’s team obtained a maximum zT of 1.0 at 750 K in the Ag-doped CuGaTe2 compound [30] and identified that vacancy scattering was an active approach to improve TE transport behaviors [31]. Zhang et al. [26] synthesized a quinary alloy compound Cu0.7Ag0.3Ga0.4In0.6Te2 with a complex nanosized strain domain structure, which presented excellent TE properties with a peak zT of 1.64 at 873 K and an average zT (zTave) of 0.73. Through compositing TiO2 nanofibers, Yang et al. [32] achieved a maximum zT of 1.47 at 823 K in a CuInTe2–based TE compound. Moreover, Chen et al. [23] obtained a maximum zT of 1.24 in the Cu0.75Ag0.2InTe2 compound. The above shows that Cu(In, Ga)Te2 diamond-like TE materials have a higher zTs, comparable to other advanced thermoelectric materials such as PbTe [33][34][35][36] and SnTe [37][38][39]. In addition, a natural chalcopyrite mineral, CuFeS2 [40][41][42][43], was also recognized as an advanced CBDL thermoelectric material. It is noteworthy that the CuFeS2 compound is a rare typical n-type TE compound among CBDL thermoelectric materials [44][45].
Cu3–V–VI4 (V = Sb, P, As; VI = Se, S, Te) compounds with a tetragonal diamond-like crystal structure can be approximately regarded as the superposition of four equivalent zincblendes, wherein Cu3SbSe4 is considered as a promising TE candidate owing to its narrow band gap of ~0.3 eV [19][27][46][47]. For improving the TE performance of Cu3SbSe4–based materials, Li et al. [48] coordinately regulated electrical and thermal transport behaviors through the incorporation of Sn-doping and AgSb0.98Ge0.02Se2 inclusion, and the highest zT of 1.23 was eventually achieved at 675 K. Bo et al. [47] successfully applied the concept of configuration entropy to optimize the TE performance of Cu3SbSe4, and the zT increased by about four times, compared to the initial phase, with the increase of entropy. In their latest report, Zhou’s group [27] attained a superior average power factor (PFave) of 19 µW·cm−1·K−2 in 300–723 K by using a small amount of foreign Al atoms as “stabilizers” to supply the high hole concentration, with almost no effect on carrier mobility. Consequently, combined with the reduced κ, a record-high zT of 1.4 and a zTave of 0.72 were obtained within the Cu3SbSe4–based compounds. A new unconventional doping process that can coordinate the TE properties of materials was also presented. Apart from Cu3SbSe4, Cu3SbS4 is also a promising Cu3–V–VI4–type of TE material [28][49][50], and it has been demonstrated that its PFave can reach up to 16.1 µW·cm−1·K−2 and the zTave up to 0.77 between 400 and 773 K via its optimization [28].
Different from Cu–III–VI2 and Cu3–V–VI4 compounds, ternary Cu2–IV–VI3 (IV = Sn, Ge, Pb; VI = Se, Te, S) compounds crystallize in more distorted structures that are far from tetragonal. Cu2SnSe3 is a kind of CBDL compound with diverse structural phases, which has been found and synthesized successfully, including in cubic, tetragonal, orthogonal, and monoclinic phases involving three variants [22]. Hu et al. [51] improved the TE transport behaviors of Cu2SnSe3 by enhancing the crystal symmetry of it via Mg-doping and intensifying the phonon scattering through the introduction of dislocations and nanoprecipitates. Similarly, Ming et al. [52] obtained a peak zT of 1.51 at 858 K in the Cu2Sn0.82In0.18Se2.7S0.3 compound through regulating the band structure and introducing multi-scale defects. In addition, a record-high zT of 1.61 was obtained at 848 K by Qin et al. [53] by constructing the intrinsic point defects, including high-dense stacking faults and endo-grown nanoneedles, to obstruct mid- as well as low-frequency phonons in Cu2SnSe3 compounds. Except for Cu2SnSe3, Cu5A2B7 (A = Si, Ge, Sn; B = S, Se, Te), with a centrosymmetric space group C2/m, is also a kind of distorted CBDL compound which has been considered to possess a non-centrosymmetric cubic structure, with the phase crystallized as C-centered [54][55][56]. An undesirable characteristic of Cu5A2B7 compounds is that they represent metal-like behaviors, such as the carrier concentration and κ of Cu5Sn2Te7 at 300 K are 1.39×1021 cm−3 and 15.1 W·m−1·K−1, respectively [55]. Simultaneously, zinc atoms have been proven to be effective dopants for strengthening the semiconductor properties of Cu5Sn2Te7 compounds; Sturm et al. [56] introduced a zinc dopant into Cu5Sn2Se7 and Cu5Sn2Te7 compounds, which also supports this conclusion. Especially noteworthy is that the effect of zinc doping is not optimal, and the TE performance of the compound still needs further improvement.
Quaternary Cu2–II–IV–VI4 (II = Co, Mn, Hg, Mg, Zn, Cd, Fe; IV = Sn, Ge; VI = Se, S, Te) compounds with more complex tetragonal structures have also been widely studied. The distinguishing features of quaternary CBDL compounds are they possess a wider bandgap and a relatively lower carrier mobility compared with the ternary CBDL compounds [57][58][59][60][61][62][63][64][65]. Taking the orthorhombic enargite-type Cu2MnGeS4 as an example [61], the bandgap of it is ~1.0 eV in the initial phase while it only converts to 0.9 eV in the Cu2.5Mn0.5GeS4 by adjusting the ratio of Mn and Cu atoms. The large-cell Cu10B2C4D13 [66][67][68][69]  (B = Ag, Cu; C = Co, Ni, Zn, Cu, Mn, Fe, Hg, Cd; Q = Sb, Bi, As; Q = Se, S) tetrahedrites have even more complex crystal structures. The featured“PGEC” framework is also displayed in the Cu12Sb4S13 tetrahedrite, where the electric transmission is controlled by a CuS4 network and the thermal transmission is governed by a cavity polyhedral consisting of CuS3 and SbS3 groups [66]. In 2013, Lu et al. [68] achieved an enhanced zT of 0.95 at 720 K in Cu12Sb4S13 utilizing Zn-doping. Moreover, Li et al. [69] attained a high zT of 1.15 at 723 K in a porous Cu12Sb4S13–based material; a segmented single-leg device based on the material was successfully fabricated which realized a high conversion efficiency of 6% when the ΔT reached up to 419 K. Cu26P2Q6S32 [70][71][72][73][74](P = V, Ta, Nb, W, Mo; Q = Ge, Sn, As, Sb) colusites are other large-cell examples, which possess 66 atoms in a crystal cell while the tetrahedrites possess 58 atoms. Therefore, the common characteristic of both is their inherent low κ derived from high structural inhomogeneity [74][75]. For instance, Guilmeau’s group [71] obtained the lowest κ of 0.4 W·m−1·K−1 at 300 K in the Cu26V2Sn6S32 colusite, which was attributed to the structural complexity of colusite and mass fluctuations among the Cu, V and Sn atoms. In 2018, they further elucidated the potential mechanism related to the fountainhead of intrinsically low κ for a colusite along with the influence of antisite defects and S-vacancies on carrier concentration [71][72].


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