The impact of manganese substitution on the structure and properties of tetrahedrite

Guélou, Gabin; Powell, Anthony V.; Smith, Ronald I.; Vaqueiro, Paz

doi:10.1063/1.5110696

Cited by 11 publications

(12 citation statements)

References 34 publications

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“…This phenomenon could also be connected with the liquid-like nature of copper ions, which is more probable in Cu-rich tetrahedrite phases. As is often reported for the superionic argyrodites [24,60], as well as tetrahedrites [48,61,62], the migration of Cu ions can strongly disturb phonon propagation. To verify the TE performance of the investigated samples, the density of the state effective mass m * was calculated using the Kane band model.…”

Section: Samplementioning

confidence: 83%

Phase Analysis and Thermoelectric Properties of Cu-Rich Tetrahedrite Prepared by Solvothermal Synthesis

et al. 2022

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Because of the large Seebeck coefficient, low thermal conductivity, and earth-abundant nature of components, tetrahedrites are promising thermoelectric materials. DFT calculations reveal that the additional copper atoms in Cu-rich Cu14Sb4S13 tetrahedrite can effectively engineer the chemical potential towards high thermoelectric performance. Here, the Cu-rich tetrahedrite phase was prepared using a novel approach, which is based on the solvothermal method and piperazine serving both as solvent and reagent. As only pure elements were used for the synthesis, the offered method allows us to avoid the typically observed inorganic salt contaminations in products. Prepared in such a way, Cu14Sb4S13 tetrahedrite materials possess a very high Seebeck coefficient (above 400 μVK−1) and low thermal conductivity (below 0.3 Wm−1K−1), yielding to an excellent dimensionless thermoelectric figure of merit ZT ≈ 0.65 at 723 K. The further enhancement of the thermoelectric performance is expected after attuning the carrier concentration to the optimal value for achieving the highest possible power factor in this system.

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Section: Samplementioning

confidence: 83%

Phase Analysis and Thermoelectric Properties of Cu-Rich Tetrahedrite Prepared by Solvothermal Synthesis

et al. 2022

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“…The dimensionless figure of merit (ZT) of Cu performed long-term and careful melting processes; raw elements were heated to 923 K, maintained for 12 h, cooled to room temperature, and then annealed at 723 K for two weeks. Guélou et al [18] also conducted long-term and multi-step processes; samples were mechanically alloyed for 6 h, annealed at 973 K for 3 h, and cooled to 823 K for 30 h. The furnace was then cooled to room temperature, and finally, the ingot was crushed and subjected to a second annealing at 823 K for 30 h. In the present study, however, a single tetrahedrite phase exhibiting a high level of ZT was obtained by MA within 24 h without post-annealing.…”

Section: Resultsmentioning

confidence: 99%

“…In our previous study [10], undoped Cu 12 Sb 4 S 13 exhibited a ZT of 0.66 at 723 K. In this study, as the Mn content increased, both the thermal conductivity and PF increased. As a result, Cu 11.7 Mn 0.3 Sb 4 S 13 exhibited the highest ZT of 0.75 at 723 K. Wang et al [17] reported a ZT of 0.89 at 700 K for Cu 11.5 Mn 0.5 Sb 4 S 13 prepared by encapsulated melting and HP.Guélou et al[18] obtained a ZT of 0.56 at 573 K for Cu 11 MnSb 4 S 13 produced by MA and HP. Wang et al[17]…”

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confidence: 99%

Charge Transport and Thermoelectric Properties of Mn-Doped Tetrahedrites Cu12-xMnxSb4S13

Kim¹,

Lee²,

Kim³

2021

Korean J. Met. Mater.

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Mn-doped tetrahedrites Cu12-xMnxSb4S13 (0.1 ≤ x ≤ 0.4) were synthesized by mechanical alloying (MA) and sintered by hot pressing (HP). A single tetrahedrite phase was synthesized by MA without post-annealing, and it was stable without any phase changes after HP. The hot-pressed specimens had a relative density higher than 98.6%. The lattice constant of the Mn-doped samples increased compared to that of undoped Cu12Sb4S13, but no significant change in the lattice constant was observed with a change in Mn content. All Mn-doped tetrahedrites acted as p-type semiconductors, as confirmed from positive Hall and Seebeck coefficient values. The Seebeck coefficient increased with increasing temperature but decreased with increasing Mn content; maximum Seebeck coefficient values of 200−219 μVK-1 were obtained at 323−723 K for x = 0.1. Electrical conductivity increased with increasing temperature and Mn content; the highest electrical conductivity values of (1.76−2.45) × 104 Sm-1 were obtained at 323−723 K for x = 0.4. As a result, Cu11.6Mn0.4Sb4S13 exhibited a maximum power factor of 0.80 mWm-1K-2 at 723 K. As the Mn content increased, both the electronic and lattice thermal conductivities increased, and thus, the total thermal conductivity was the lowest at 0.48–0.63Wm-1K-1 at 323–723 K for x = 0.1. A maximum dimensionless figure of merit of 0.75 was obtained at 723 K for Cu11.7Mn0.3Sb4S13. The MA-HP process is suitable for preparing doped tetrahedrites exhibiting excellent thermoelectric performance.

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“…Considering the valence and coordination of each element, the charge balance of tetrahedrite can be expressed as [6,7]. To improve the dimensionless figure of merit (ZT), partial substitutions at the Cu, Sb, or S sites have been made with doping elements, including transition metals such as Ni, Co, Fe, and Mn at the Cu site [8][9][10][11], Te or As at the Sb site [12,13], and Se at the S site [14].…”

Section: Introductionmentioning

confidence: 99%

Charge Transport and Thermoelectric Properties of Sn-Doped Tetrahedrites Cu12Sb4-ySnyS13

Ahn¹,

Kim²

2021

Korean J. Met. Mater.

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In this study, tetrahedrite compounds doped with Sn were prepared by mechanical alloying and hot pressing, and their charge transport and thermoelectric properties were analyzed. X-ray diffraction analysis revealed that both the synthetic powders and sintered bodies were synthesized as a single tetrahedrite phase without secondary phases. Densely sintered specimens were obtained with relatively high densities of 99.5%-100.0% of the theoretical density, and the component elements were distributed uniformly. Sn was successfully substituted at the Sb site, and the lattice constant increased from 1.0348 to 1.0364 nm. Positive signs of the Hall and Seebeck coefficients confirmed that the Sn-doped tetrahedrites were p-type semiconductors. The carrier concentration decreased from 1.28 × 1019 to 1.57 × 1018 cm-3 as the Sn content decreased because excess electrons were supplied by doping with Sn4+ at the Sb3+ site of the tetrahedrite. The Seebeck coefficient increased with increasing Sn content, and Cu12Sb3.6Sn0.4S13 exhibited maximum values of 238-270 µVK-1 at temperatures of 323-723 K. However, the electrical conductivity decreased as the amount of Sn doping increased. Thus, Cu12Sb3.9Sn0.1S13 exhibited the highest electrical conductivity of (2.24-2.40) × 104 Sm-1 at temperatures of 323-723 K. A maximum power factor of 0.73 mWm-1K-2 was achieved at 723 K for Cu12Sb3.9Sn0.1S13. Sn substitution reduced both the electronic and lattice thermal conductivities. The lowest thermal conductivity of 0.49-0.60 Wm-1K-1 was obtained at temperatures of 323-723 K for Cu12Sb3.6Sn0.4S13, where the lattice thermal conductivity was dominant at 0.49-0.57 Wm-1K-1. As a result, a maximum dimensionless figure of merit of 0.66 was achieved at 723 K for Cu12Sb3.9Sn0.1S13.

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The impact of manganese substitution on the structure and properties of tetrahedrite

Cited by 11 publications

References 34 publications

Phase Analysis and Thermoelectric Properties of Cu-Rich Tetrahedrite Prepared by Solvothermal Synthesis

Phase Analysis and Thermoelectric Properties of Cu-Rich Tetrahedrite Prepared by Solvothermal Synthesis

Charge Transport and Thermoelectric Properties of Mn-Doped Tetrahedrites Cu12-xMnxSb4S13

Charge Transport and Thermoelectric Properties of Sn-Doped Tetrahedrites Cu12Sb4-ySnyS13

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