Research Update: Cu–S based synthetic minerals as efficient thermoelectric materials at medium temperatures

Suekuni, Koichiro; Takabatake, Toshiro

doi:10.1063/1.4955398

Cited by 108 publications

(65 citation statements)

References 109 publications

(157 reference statements)

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“…This study demonstrates that other s-block elements may be worth considering to determine whether they can be beneficial for optimizing the thermoelectric performance of tetrahedrites. 9 List of Figures Fig. 1: (a…”

Section: Resultsmentioning

confidence: 99%

“…[3] Tetrahedrites can be described by the general chemical composition Cu10(Zn,Fe,Cu,…)2(Sb,As)4S13 which is a multicomponent variant of the ternary tetrahedrite Cu12Sb4S13. [4] While naturally occurring tetrahedrite minerals are not directly suitable for TE applications because of their nearly intrinsic semiconducting electrical properties synonymous with high electrical resistivity values, [5] synthetic tetrahedrites with optimized chemical composition have been shown to reach peak ZT values close to unity near 700 K. [6,7,8] Such good thermoelectric performance is mainly due to their extremely low lattice thermal conductivity with values as low as 0.5 W m-1 K-1 at 700 K. [9] These low values along with 3 the glass-like temperature dependence have been shown to originate from strongly anharmonic, low-energy optical modes associated with unconventional thermal vibrations of some of the Cu atoms. [10,11,12] Partial substitutions by transition metals or chalcogenides on the Cu, Sb or S sites help to drive the metallic properties of Cu12Sb4S13 towards a heavilydoped semiconducting state more favorable for thermoelectric performance.…”

Section: Introductionmentioning

confidence: 99%

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Thermoelectric Properties of Magnesium-Doped Tetrahedrite Cu12−xMgxSb4S13

Levinský

Candolfi

Dauscher

et al. 2019

Journal of Elec Materi

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Tetrahedrites, naturally occurring sulfosalt minerals, have been shown to exhibit peak ZT values close to unity near 700 K due to the combination of semiconducting-like properties and extremely low lattice thermal conductivity. A wide range of elements can be substituted into tetrahedrites, each of them affecting the thermoelectric properties. Interestingly, all tetrahedrites reported to date contain exclusively d-and p-block elements of the periodic table. Here, we demonstrate that magnesium, an s-block element, can be successfully introduced in Cu12Sb4S13. We successfully prepared a series of polycrystalline samples Cu12-xMgxSb4S13 with nominal compositions x = 0.5, 1.0, 1.5. Powder X-ray diffraction and chemical mapping confirmed that approximately half of the Mg atoms were incorporated into the tetrahedrite unit cell, while the other half forms electrically insulating MgS precipitates.Thermoelectric properties, measured between 5 and 673 K, show that the effect of Mg2+ is similar to that of other aliovalent elements substituting for either Cu or Sb. In particular, 2 increasing the Mg content drives the system closer to a semiconducting behavior, leading to a concomitant increase in the thermopower and electrical resistivity and a decrease in the electronic part of the thermal conductivity. Because these two trends counterbalance each other, the overall effect of Mg on the ZT of Cu12Sb4S13 is found to be marginal with a peak ZT of 0.55 at 673 K.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Thermoelectric Properties of Magnesium-Doped Tetrahedrite Cu12−xMgxSb4S13

Levinský

Candolfi

Dauscher

et al. 2019

Journal of Elec Materi

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“…Many spinels consisting of well‐abundant and environmental‐friendly elements (which is crucial for a possible thermoelectric application) became the object of numerous studies. Among these compounds, indium‐based thiospinels are a rare case of n ‐type sulfide semiconductors …”

Section: Introductionmentioning

confidence: 99%

Structural Peculiarities and Thermoelectric Study of Iron Indium Thiospinel

Wyżga

Veremchuk²,

Bobnar³

et al. 2020

Chemistry A European J

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The homogeneity range of ternary iron indium thiospinela t8 73 Kw as investigated. Ad etailed study was focused on two distinct series (y = z): 1) ap reviously reported charge-balanced (In 0.67 + 0.33y & 0.33À0.33y ) tetr [In 2Àz Fe z ] oct S 4 (A1series; & stands for vacancy;t he abbreviations "tetr" and "oct" indicate atoms occupying tetrahedral 8a and octahedral 16d sites, respectively)a nd 2) an ew charge-unbalanced (In 0.67 + y & 0.33Ày ) tetr [In 2Àz Fe z ] oct S 4 (A2-series). Fe atoms were confirmed to exclusively occupy an octahedral positioni nb oth series. An unusualr eduction of the unit cell parameter with increasing Fe contenti se xplained by differences in the ionic radii between Fe and In, as well as by an additional electrostatic attraction originating from charge imbalance( latter only in A2-series). The studiedc ompound is an n-type semiconductor,a nd its charge carrier concentration increases or decreases for larger Fe content withint he A1-and A2-series, respectively.T he thermal conductivity k tot is significantly reducedu pon increasing vacancy concentration, whereas the changeo fp ower factor is insufficientt od rastically improve the thermoelectric figure of merit.

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“…Among them, we have focused on sulfide systems because of the low toxicity and abundance of sulfur. [102][103][104] The electronegativity of sulfur is lower than that of oxygen; therefore, sulfides typically show lower ρ than oxides, leading to higher S 2 /ρ.…”

Section: Alternative To Pbtementioning

confidence: 99%

An Integrated Approach to Thermoelectrics: Combining Phonon Dynamics, Nanoengineering, Novel Materials Development, Module Fabrication, and Metrology

Ohta

Jood

Murata

et al. 2018

Advanced Energy Materials

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This review discusses the longstanding efforts to develop advanced thermoelectrics through a multidisciplinary approach by combining condensed matter physics, nanotechnology, solid‐state chemistry, electrical engineering, mechanical engineering, and metrology. The phonon dynamics of skutterudites, clathrates, tetrahedrites, and layered LaOBiSSe are investigated through inelastic neutron scattering, allowing insights into their low lattice thermal conductivity due to rattling in a cage as well as under planar coordination. The electrical resistivity, Seebeck coefficient, and Hall coefficient of Bi‐nanowires are successfully measured with a home‐made system, demonstrating a size effect in thermoelectric and galvanomagnetic phenomena. For PbTe‐based bulk thermoelectrics, an exceptionally high figure of merit ZT (≈1.8 at 800 K) is achieved through nanostructuring. Moreover, correspondingly high conversion efficiency (≈11% for a temperature difference of 590 K) is demonstrated in nanostructured PbTe‐based modules. Sulfides (tetrahedrite, colusite, and CdI2‐type layered systems) and arsenides (LnFeAsO and BaZn2As2) are developed as environmentally friendly and emerging thermoelectric materials, respectively. The output power and efficiency of modules with novel materials, including nanostructured PbTe, Zn4Sb3, and clathrates, are measured with the highly accurate self‐made system. Future opportunities and challenges for the widespread use of thermoelectric waste heat recovery and energy harvesting are also discussed.

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Research Update: Cu–S based synthetic minerals as efficient thermoelectric materials at medium temperatures

Cited by 108 publications

References 109 publications

Thermoelectric Properties of Magnesium-Doped Tetrahedrite Cu12−xMgxSb4S13

Thermoelectric Properties of Magnesium-Doped Tetrahedrite Cu12−xMgxSb4S13

Structural Peculiarities and Thermoelectric Study of Iron Indium Thiospinel

An Integrated Approach to Thermoelectrics: Combining Phonon Dynamics, Nanoengineering, Novel Materials Development, Module Fabrication, and Metrology

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