Preparation and properties of ZnSb thermoelectric material through mechanical-alloying and Spark Plasma Sintering

Pothin, R.; Ayral, R.M.; Berche, Alexandre; Granier, Dominique; Rouessac, Florence Bosc; Jund, Philippe

doi:10.1016/j.cej.2016.04.063

Cited by 35 publications

(34 citation statements)

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“…The intermetallic Zn-Sb system has recently attracted research interest, as it shows promising thermoelectric performance at intermediate temperatures [1][2][3][4][5]. Unlike other state-of-the-art thermoelectric materials, zinc antimonides consist of neither toxic nor expensive elements [6].…”

Section: Introductionmentioning

confidence: 99%

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Zn vacancy formation, Zn evaporation and decomposition of ZnSb at elevated temperatures: Influence on the microstructure and the electrical properties

Song

Schrade

Masó

et al. 2017

Journal of Alloys and Compounds

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The influence of annealing on the microstructure and electrical properties of undoped polycrystalline ZnSb samples has been investigated by different experimental techniques. In situ XRD in an argon atmosphere showed that ZnSb powders decompose at 300 °C, which is attributed to Zn evaporation. In situ SEM in a moist atmosphere showed fast surface deterioration at 450 °C and above, reflecting decomposition of ZnSb and the formation of metallic Sb precipitates. The rate of Zn loss in a reducing atmosphere was determined by thermogravimetry and related to the Zn partial vapor pressure. The increase of the hole carrier concentration of ZnSb measured at room temperature after heat treatment was correlated with Zn evaporation at elevated temperature. The carrier concentration after annealing at 400 °C is consistent with an activation energy for Zn vacancy formation of 0.4 eV and a maximum Zn deficiency x of Zn 1-x Sb of 1 × 10-3 .

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Section: Introductionmentioning

confidence: 99%

“…In this paper, we establish the combined occurrence of Eqs. (1) and (2), and study the decomposition of ZnSb as a function of time and temperature in different surrounding atmospheres. We finally relate our measurements of weight loss to Zn vacancy concentrations and changes in electrical properties.…”

Section: Introductionmentioning

confidence: 99%

Zn vacancy formation, Zn evaporation and decomposition of ZnSb at elevated temperatures: Influence on the microstructure and the electrical properties

Song

Schrade

Masó

et al. 2017

Journal of Alloys and Compounds

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“…Considering that one of the favourable aspects of ZnSb from a commercial point of view is the low materials cost, there have been several efforts where the cost efficiency of the synthesis technique is important [92][93][94].…”

Section: Thermoelectrics For Power Generation -A Look At Trends In Thmentioning

confidence: 99%

Review of Research on the Thermoelectric Material ZnSb

Song¹,

Finstad²

2016

Thermoelectrics for Power Generation - A Look at Trends in the Technology

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The thermoelectric material ZnSb has been studied intensively in recent years and has shown promising features. The other zinc-antimonide compound, Zn 4 Sb 3 has remarkable low thermal conductivity, but it is accompanied with phase transitions at moderate temperature and has inherent stability problems. Compared to that, ZnSb is relatively phase stable and has a relative high charge carrier mobility and Seebeck coefficient, thus yielding a decent power factor. Meanwhile, its thermal conductivity can be reduced by means of nanostructuring, thus giving a good figure of merit at moderate temperatures, 400-600K. Many researchers have dedicated their efforts to study and improve ZnSb properties, and the figure of merit has been reported to be above one. Still, ZnSb as a thermoelectric material has features and behaviours that are not well-understood. The behaviour and properties of its intrinsic defects are not understood, but have interested researchers in recent years. This chapter intends to offer a comprehensive review on ZnSb to the readers. By combining own experiences from research on thermoelectric materials, the authors address the prospect for improving the thermoelectric properties of ZnSb and the concerns of transferring lab results to manufacturing.

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“…[29][30][31][32][33][34][35] A computationally derived convex hull of formation enthalpies for various binary zinc antimonides predicts ZnSb to have the most negative formation enthalpy. 36 Low-temperature, soft chemistry techniques may provide a reproducible means to observe and isolate many of these compounds.…”

Section: Introductionmentioning

confidence: 99%

Expanding the I–II–V Phase Space: Soft Synthesis of Polytypic Ternary and Binary Zinc Antimonides

et al. 2018

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Soft chemistry methods offer the possibility of synthesizing metastable and kinetic products that are unobtainable through thermodynamically-controlled, high-temperature reactions. A recent solution-phase exploration of Li-Zn-Sb phase space revealed a previously unknown cubic half-Heusler MgAgAs-type LiZnSb polytype. Interestingly, this new cubic phase was calculated to be the most thermodynamically stable, despite prior literature reporting only two other ternary phases (the hexagonal half-Heusler LiGaGe-type LiZnSb, and the full-Heusler Li2ZnSb). This surprising discovery, coupled with the intriguing optoelectronic and transport properties of many antimony containing Zintl phases, required a thorough exploration of syn-thetic parameters. Here, we systematically study the effects that different precursor concentrations, injection order, nucleation and growth temperatures, and reaction time have on the solution-phase synthesis of these materials. By doing so, we identify conditions that selectively yield several unique ternary (c-LiZnSb vs. h*-LiZnSb), binary (ZnSb vs. Zn8Sb7), and metallic (Zn, Sb) products. Further, we find one of the ternary phases adopts a variant of the previously observed hexagonal LiZnSb struc-ture. Our results demonstrate the utility of low temperature solution phase-soft synthesis-methods in accessing and mining a rich phase space. We anticipate that this work will motivate further exploration of multinary I-II-V compounds, as well as encourage similarly thorough investigations of related Zintl systems by solution phase methods. Disciplines Materials ChemistryComments "This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in Chemistry of Materials, copyright © American Chemical Society after peer review. To access the final edited and published work see http://dx.doi.org/10.1021/acs.chemmater.8b02910. ABSTRACT: Soft chemistry methods offer the possibility of synthesizing metastable and kinetic products that are unobtainable through thermodynamically-controlled, high-temperature reactions. A recent solution-phase exploration of Li-Zn-Sb phase space revealed a previously unknown cubic half-Heusler MgAgAs-type LiZnSb polytype. Interestingly, this new cubic phase was calculated to be the most thermodynamically stable, despite prior literature reporting only two other ternary phases (the hexagonal half-Heusler LiGaGe-type LiZnSb, and the full-Heusler Li2ZnSb). This surprising discovery, coupled with the intriguing optoelectronic and transport properties of many antimony containing Zintl phases, required a thorough exploration of synthetic parameters. Here, we systematically study the effects that different precursor concentrations, injection order, nucleation and growth temperatures, and reaction time have on the solution-phase synthesis of these materials. By doing so, we identify conditions that selectively yield several unique ternary (c-LiZnSb vs. h*-LiZnSb), binary (ZnSb vs. Zn8Sb7), and metallic (Zn, Sb) products. Furt...

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Preparation and properties of ZnSb thermoelectric material through mechanical-alloying and Spark Plasma Sintering

Cited by 35 publications

References 35 publications

Zn vacancy formation, Zn evaporation and decomposition of ZnSb at elevated temperatures: Influence on the microstructure and the electrical properties

Zn vacancy formation, Zn evaporation and decomposition of ZnSb at elevated temperatures: Influence on the microstructure and the electrical properties

Review of Research on the Thermoelectric Material ZnSb

Expanding the I–II–V Phase Space: Soft Synthesis of Polytypic Ternary and Binary Zinc Antimonides

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