Co-precipitation synthesis of nanostructured Cu<sub>3</sub>SbSe<sub>4</sub>and its Sn-doped sample with high thermoelectric performance

Li, Di; Li, Rui; Qin, Xiaoying; Song, Caixia; Xin, Hongxing; Zhang, Jian; Guo, Genmiao; Zou, Tianhua; Liu, Yong-Fei; Zhu, Xiaoguang

doi:10.1039/c3dt52447g

Cited by 54 publications

(41 citation statements)

References 22 publications

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“…7 shows the carrier density dependence of the Seebeck coefficient and Hall mobility at room temperature, together with the data previously reported for this system. 23,33,42 We found that the SPB model with acoustic phonon scattering assumption could well explain both properties. From the carrier density dependence of the Seebeck coefficient (the Pisarenko relation), it seems that all the measured S are consistent with a constant density-of-state (DOS) effective mass, m* ¼ 1.5 m e .…”

Section: Resultsmentioning

confidence: 83%

Thermoelectric properties of Sn-doped p-type Cu₃SbSe₄: a compound with large effective mass and small band gap

et al. 2014

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Cu 3 SbSe 4 -based compounds composed of earth-abundant elements have been found to exhibit good thermoelectric performance at medium temperatures. High zT values were achieved in previous studies, but further insight into the transport mechanism as well as some key material parameters is still needed. In this work, we studied the electrical and thermal transport properties of Sn-doped Cu 3 SbSe 4 between 300 K and 673 K. It was found that the single parabolic band model explains the electrical transport very well.Experimentally, we determined the band gap to be around 0.29 eV. The density-of-state effective mass was found to be about 1.5 m e for the doped samples. The transport properties suggested degeneracy splitting near the valence band maximum that was not captured by previous band structure calculations.The maximum zT $ 0.70 was obtained at 673 K, and the optimized carrier density was $1.8 Â 10 20 cm À3, and the potential for further improvement of zT via material engineering is briefly discussed.

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Section: Resultsmentioning

confidence: 83%

Thermoelectric properties of Sn-doped p-type Cu₃SbSe₄: a compound with large effective mass and small band gap

et al. 2014

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“…The finite-temperature structural characteristics of Cu 3 SbSe 3 , a new type of TE material, could further demonstrate the deviation from the static and small-vibration picture. Cu-Sb-Se systems have been shown to possess a ZT value about unity (31,32), and Cu 3 SbSe 3 manifests anomalously low lattice thermal conductivity (0.7-1.0 Wm -1 ·K −1 ) with an unusual temperature dependence (33, 34) (see An Effective Approach for the Thermal Transport in Part-Crystalline Part-Liquid Materials) and has also been expected to possess a ZT value about unity (35). In the compound, certain type of constituent atoms weakly bond to the rest of lattice with relatively strong rigidity.…”

Section: Resultsmentioning

confidence: 99%

Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy

Qiu

Wei

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

239

209

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Understanding thermal and phonon transport in solids has been of great importance in many disciplines such as thermoelectric materials, which usually requires an extremely low lattice thermal conductivity (LTC). By analyzing the finite-temperature structural and vibrational characteristics of typical thermoelectric compounds such as filled skutterudites and Cu 3 SbSe 3 , we demonstrate a concept of part-crystalline part-liquid state in the compounds with chemicalbond hierarchy, in which certain constituent species weakly bond to other part of the crystal. Such a material could intrinsically manifest the coexistence of rigid crystalline sublattices and other fluctuating noncrystalline sublattices with thermally induced largeamplitude vibrations and even flow of the group of species atoms, leading to atomic-level heterogeneity, mixed part-crystalline partliquid structure, and thus rattling-like thermal damping due to the collective soft-mode vibrations similar to the Boson peak in amorphous materials. The observed abnormal LTC close to the amorphous limit in these materials can only be described by an effective approach that approximately treats the rattling-like damping as a "resonant" phonon scattering.sublattice melting | partial Grüneisen parameter | first principles | anharmonicity U nderstanding thermal and phonon transport in solids has been of great importance in many disciplines such as thermoelectrics (1-3), phononic materials (4), and thermal management composites (5). The interplay among chemical bonds, lattice dynamics, and thermal transport in materials is also an attractive topic in condensed matter physics (6) and materials science (7). Thermal transport is a key issue in thermoelectric (TE) energy-conversion materials, which are regarded among the potential candidates for revolutionizing waste-heat recovery (2, 7-9). The dimensionless figure of merit of a TE material is defined as ZT = TS 2 σ=κ, where T, S, σ, and κ are the absolute temperature, Seebeck coefficient, electrical conductivity, and thermal conductivity, respectively. To improve the efficiency of TE conversion, many approaches aim at reducing the thermal conductivity, especially the lattice part, to a minimum level, namely the realization of phonon-glass-like thermal transport (1, 7).TE materials research primarily focuses on solid and crystalline thermoelectrics. It has been long viewed that all solids contain strong interatomic interactions without even an exception, and thus the established approaches to describe thermal transports in crystalline solids, including TE solids, are solely based on the perturbative "small-parameter" approximation to lattice dynamics of atoms around their equilibrium positions, i.e., phonons and phonon-phonon interactions (10, 11). As a result, crystallographic homogeneity at the atomic level in solid materials has overwhelmingly been accepted. However, recent work on exploring novel TE materials went noticeably beyond the conventional knowledge of solid TE compounds being ideally crystalline, atomically...

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“…Few reports have also detailed the production of bulk nanostructured CASe. [32][33][34] However bottom-up strategies to cost-effectively produce efficient CASe NCs, nanomaterials and CASe-based devices remain to be demonstrated. Here, we report a solution-based scalable synthesis approach to produce several grams of monodisperse CASe NCs doped with controlled amounts of Sn and Bi.…”

Section: Introductionmentioning

confidence: 99%

Solution-based synthesis and processing of Sn- and Bi-doped Cu₃SbSe₄nanocrystals, nanomaterials and ring-shaped thermoelectric generators

et al. 2017

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Copper-based chalcogenides that comprise abundant, low-cost, and environmental friendly elements are excellent materials for a number of energy conversion applications, including photovoltaics, photocatalysis, and thermoelectrics (TE). In such applications, the use of solution-processed nanocrystal (NC) to produce thin films or bulk nanomaterials has associated several potential advantages, such as high material yield and throughput, and composition control with unmatched spatial resolution and cost. Here we report on the production of Cu3SbSe4 (CASe) NCs with tuned amounts of Sn and Bi dopants. After proper ligand removal, as monitored by nuclear magnetic resonance and infrared spectroscopies, these NCs were used to produce dense CASe bulk nanomaterials for solid state TE energy conversion. By adjusting the amount of extrinsic dopants, dimensionless TE figures of merit (ZT) up to 1.26 at 673 K were reached. Such high ZT values are related to an optimized carrier concentration by Sn doping, a minimized lattice thermal conductivity due to efficient phonon scattering at point defects and grain boundaries, and to an increase of the Seebeck coefficient obtained by a modification of the electronic band structure with the Bi doping. Nanomaterials were further employed to fabricate ring-shaped TE generators to be coupled to hot pipes and which provided 20 mV and 1 mW per TE element when exposed to a 160 °C temperature gradient. The simple design and good thermal contact associated with the ring geometry and the potential low cost of the material solution processing may allow the fabrication of TE generators with short payback times.Peer ReviewedPostprint (author's final draft

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Co-precipitation synthesis of nanostructured Cu₃SbSe₄and its Sn-doped sample with high thermoelectric performance

Cited by 54 publications

References 22 publications

Thermoelectric properties of Sn-doped p-type Cu₃SbSe₄: a compound with large effective mass and small band gap

Thermoelectric properties of Sn-doped p-type Cu₃SbSe₄: a compound with large effective mass and small band gap

Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy

Solution-based synthesis and processing of Sn- and Bi-doped Cu₃SbSe₄nanocrystals, nanomaterials and ring-shaped thermoelectric generators

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Co-precipitation synthesis of nanostructured Cu3SbSe4and its Sn-doped sample with high thermoelectric performance

Cited by 54 publications

References 22 publications

Thermoelectric properties of Sn-doped p-type Cu3SbSe4: a compound with large effective mass and small band gap

Thermoelectric properties of Sn-doped p-type Cu3SbSe4: a compound with large effective mass and small band gap

Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy

Solution-based synthesis and processing of Sn- and Bi-doped Cu3SbSe4nanocrystals, nanomaterials and ring-shaped thermoelectric generators

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Co-precipitation synthesis of nanostructured Cu₃SbSe₄and its Sn-doped sample with high thermoelectric performance

Thermoelectric properties of Sn-doped p-type Cu₃SbSe₄: a compound with large effective mass and small band gap

Thermoelectric properties of Sn-doped p-type Cu₃SbSe₄: a compound with large effective mass and small band gap

Solution-based synthesis and processing of Sn- and Bi-doped Cu₃SbSe₄nanocrystals, nanomaterials and ring-shaped thermoelectric generators