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      Copper Chalcogenide–Copper Tetrahedrite Composites—A New Concept for Stable Thermoelectric Materials Based on the Chalcogenide System

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          Abstract

          For the first time, an alternative way of improving the stability of Cu-based thermoelectric materials is proposed, with the investigation of two different copper chalcogenide–copper tetrahedrite composites, rich in sulfur and selenium anions, respectively. Based on the preliminary DFT results, which indicate the instability of Sb-doped copper chalcogenide, the Cu 1.97S–Cu 12Sb 4S 13 and Cu 2−xSe–Cu 3SbSe 3 composites are obtained using melt-solidification techniques, with the tetrahedrite phase concentration varying from 1 to 10 wt.%. Room temperature structural analysis (XRD, SEM) indicates the two-phase structure of the materials, with ternary phase precipitates embed within the copper chalcogenide matrix. The proposed solution allows for successful blocking of excessive Cu migration, with stable electrical conductivity and Seebeck coefficient values over subsequent thermal cycles. The materials exhibit a p-type, semimetallic character with high stability, represented by a near-constant power factor (PF)—temperature dependences between individual cycles. Finally, the thermoelectric figure-of-merit ZT parameter reaches about 0.26 (623 K) for the Cu 1.97S–Cu 12Sb 4S 13 system, in which case increasing content of tetrahedrite is a beneficial effect, and about 0.44 (623 K) for the Cu 2−xSe–Cu 3SbSe 3 system, where increasing the content of Cu 3SbSe 3 negatively influences the thermoelectric performance.

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          Complex thermoelectric materials.

          Thermoelectric materials, which can generate electricity from waste heat or be used as solid-state Peltier coolers, could play an important role in a global sustainable energy solution. Such a development is contingent on identifying materials with higher thermoelectric efficiency than available at present, which is a challenge owing to the conflicting combination of material traits that are required. Nevertheless, because of modern synthesis and characterization techniques, particularly for nanoscale materials, a new era of complex thermoelectric materials is approaching. We review recent advances in the field, highlighting the strategies used to improve the thermopower and reduce the thermal conductivity.
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            Restoring the density-gradient expansion for exchange in solids and surfaces.

            Popular modern generalized gradient approximations are biased toward the description of free-atom energies. Restoration of the first-principles gradient expansion for exchange over a wide range of density gradients eliminates this bias. We introduce a revised Perdew-Burke-Ernzerhof generalized gradient approximation that improves equilibrium properties of densely packed solids and their surfaces.
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              Copper ion liquid-like thermoelectrics.

              Advanced thermoelectric technology offers a potential for converting waste industrial heat into useful electricity, and an emission-free method for solid state cooling. Worldwide efforts to find materials with thermoelectric figure of merit, zT values significantly above unity, are frequently focused on crystalline semiconductors with low thermal conductivity. Here we report on Cu(2-x)Se, which reaches a zT of 1.5 at 1,000 K, among the highest values for any bulk materials. Whereas the Se atoms in Cu(2-x)Se form a rigid face-centred cubic lattice, providing a crystalline pathway for semiconducting electrons (or more precisely holes), the copper ions are highly disordered around the Se sublattice and are superionic with liquid-like mobility. This extraordinary 'liquid-like' behaviour of copper ions around a crystalline sublattice of Se in Cu(2-x)Se results in an intrinsically very low lattice thermal conductivity which enables high zT in this otherwise simple semiconductor. This unusual combination of properties leads to an ideal thermoelectric material. The results indicate a new strategy and direction for high-efficiency thermoelectric materials by exploring systems where there exists a crystalline sublattice for electronic conduction surrounded by liquid-like ions.
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                Author and article information

                Contributors
                Role: Academic Editor
                Journal
                Materials (Basel)
                Materials (Basel)
                materials
                Materials
                MDPI
                1996-1944
                18 May 2021
                May 2021
                : 14
                : 10
                : 2635
                Affiliations
                Faculty of Materials Science and Ceramics, AGH University of Science and Technology, Al. Mickiewicza 30, 30-059 Krakow, Poland; kmars@ 123456agh.edu.pl (K.M.); pnieroda@ 123456agh.edu.pl (P.N.); pawelr@ 123456agh.edu.pl (P.R.)
                Author notes
                [* ]Correspondence: amikula@ 123456agh.edu.pl
                Author information
                https://orcid.org/0000-0002-8067-996X
                Article
                materials-14-02635
                10.3390/ma14102635
                8157852
                3440ec20-3876-43a3-a68f-6ee988eded3a
                © 2021 by the authors.

                Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 13 April 2021
                : 14 May 2021
                Categories
                Article

                composite,copper chalcogenide,tetrahedrite,thermoelectrics

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