Enhancing Thermoelectric Performance of PbTe-Based Compounds by Substituting Elements: A First Principles Study

Joseph, Elad; Amouyal, Yaron

doi:10.1007/s11664-014-3416-7

Cited by 22 publications

(21 citation statements)

References 43 publications

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“…Finally, the explicit expression for Seebeck coeicient tensor, S ij , is given by [70,71]: Figure 1c and d, respectively. A computational routine similar to aforementioned one is implemented with several diferences.…”

Section: The Base Agsbte 2 Phase-electronic Calculationsmentioning

confidence: 99%

Silver-Antimony-Telluride: From First-Principles Calculations to Thermoelectric Applications

Amouyal¹

2016

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

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Silver-antimony-telluride (AgSbTe 2 ) based compounds have emerged as a promising class of materials for thermoelectric (TE) power generation at the mid-temperature range. This Chapter demonstrates utilization of irst-principles calculations for predicting TE properties of AgSbTe 2 -based compounds and experimental validations. Predictive calculations of the efects of La-doping on vibrational and electronic properties of AgSbTe 2 compounds are performed applying the density functional theory (DFT), and temperature-dependent TE transport coeicients are evaluated applying the Bolzmann transport theory (BTE). Experimentally, model ternary (AgSbTe 2 ) and quaternary (3 at. % La-AgSbTe 2 ) compounds were synthesized, for which TE transport coeicients were measured, indicating that thermal conductivity decreases due to La-alloying. The later also reduces electrical conductivity and increases Seebeck coeicients. All trends correspond with those predicted from irst-principles. Thermal stability issues are essential for TE device operation at service conditions, e.g. changes of matrix composition and second-phase precipitation, and are also addressed in this study on both computational and experimental aspects. It is shown that La-alloying afects TE igure-of-merit positively, e.g., improving from 0.35 up to 0.50 at 260 °C. We highlight the universal aspects of this approach that can be applied for other TE compounds. This enables us screening their performance prior to synthesis in laboratory.Keywords: silver-antimony-telluride, irst-principles calculations, thermoelectric transport properties, Bolzmann transport theory, latice dynamics, thermal stability IntroductionIt is of utmost technological importance to develop predictive tools that will provide us with information about design of materials' functional properties. In this context, density functional theory (DFT) irst-principle calculations ofer us such possibilities [1][2][3][4] Despite of relatively high ZT values of AgSbTe 2 phase, it is still challenging to increase them to the range of 2-3. Reaching at this limit will enable us employing this material for energy conversion at power levels >500 W [34]. Reduction in latice thermal conductivity is a conventional way to enhance TE performance and is achieved by either doping with solute elements [35] or formation of second phases to stimulate phonon scatering [36][37][38]. These latice defects afect, of course, electronic properties, mainly electrical conductivity and Seebeck coeicient. Atempts to improve TE properties of AgSbTe 2 -based alloys by doping with diferent elements [19,25,[39][40][41][42][43][44][45][46][47] Notwithstanding the aforementioned successful experimental and computational atempts, a set of experimental routines, that is initiated and directed by predictions from irst principles for complete TE performance or any other computational procedure, is missing. Thermoelectrics for Power Generation -A Look at Trends in the Technology 148A signiicant step in this direction is introduced by o...

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Section: The Base Agsbte 2 Phase-electronic Calculationsmentioning

confidence: 99%

Silver-Antimony-Telluride: From First-Principles Calculations to Thermoelectric Applications

Amouyal¹

2016

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

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“…8 Herein, we assume that the relaxation time, s p , is independent of the lattice direction, solute concentration, and phonon frequency. We express the temperature-dependent phonon relaxation time, s p ðTÞ, employing Dugdale and McDonald's expression, 50 which considers Umklapp scattering processes for defect-free crystals at adequately high temperatures, 8 as follows:…”

Section: A Calculation Of Vibrational Propertiesmentioning

confidence: 99%

“…Further details are provided by us elsewhere. 8 We utilize the constant electronic relaxation time approximation, 8 presuming that the electronic relaxation time is isotropic and band-independent, which has proven to be a good approximation, 51,52 and is commonly used in transport coefficients calculations. 42,45,53 For temperatures above 300 K, which are more relevant in practice, the main contribution for the total electronic relaxation time is associated with scattering by acoustic and optical phonons.…”

Section: B Calculation Of Electronic Propertiesmentioning

confidence: 99%

“…4,5 Another important effect that is often overlooked is formation of point defects in the form of substitutional elements; the latter reduces the lattice thermal conductivity by affecting the elastic behavior of the material (as reported by us formerly for La-doped AgSbTe 2 6,7 and La-doped PbTe). 8 First-principles methods allow us to calculate most of the TE properties, including the Seebeck coefficient and the electrical and thermal conductivities.…”

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confidence: 99%

“…This approach is based on a comprehensive method reported by us formerly 8 this study, we rely on several experimental studies, reporting the effects of the introduction of different doping elements to the PbTe compound; for example, Na and K, 22 La, Pr, and Gd, 23 Ce, 24 Sm, 25 Eu, 26 Yb, 27 Tl, 28 Sn, 29 Pd, 30 V, 31 S, 32 Cl, 33 and Fe. 34 We note that several of the dopants examined in our study have not been tested experimentally so far, and we consider the current predictive approach to be valuable on both scientific and technological aspects.…”

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Towards a predictive route for selection of doping elements for the thermoelectric compound PbTe from first-principles

Joseph

Amouyal

2015

Journal of Applied Physics

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Striving for improvements of the thermoelectric (TE) properties of the technologically important lead telluride (PbTe) compound, we investigate the influence of different doping elements on the thermal conductivity, Seebeck coefficient, and electrical conductivity applying density functional theory calculations. Our approach combines total-energy calculations yielding lattice vibrational properties with the Boltzmann transport theory to obtain electronic transport properties. We find that doping with elements from the 1st and 3rd columns of the periodic table reduces the sound velocity and, consequently, the lattice thermal conductivity, while 2nd column dopants have no such influence. Furthermore, 1.6 at. % doping with 4th and 5th column elements provides the highest reduction of lattice thermal conductivity. Out of this group, Hf doping results in maximum reduction of the sound velocity from 2030 m s−1 for pure PbTe to 1370 m s−1, which is equivalent to ca. 32% reduction of lattice thermal conductivity. The highest power factor values calculated for 1.6 at. % doping range between 40 and 56 μW cm−1 K−2, and are obtained for substitution with dopants having the same valence as Pb or Te, such as those located at the 2nd, 14th, and 16th columns of the periodic table. We demonstrate how this method may be generalized for dopant-selection-oriented materials design aimed at improving TE performance of other compounds.

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IV‐VI/I‐V‐VI₂ Thermoelectrics: Recent Progress and Perspectives

Li,

Wang,

Zhou

et al. 2024

Adv Funct Materials

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Thermoelectric energy conversion technology is considered as one of the most promising solutions for recovering waste heat generated by fossil fuel combustion. As typical types of thermoelectric materials in the middle and high‐temperature range (500–900 K), binary IV‐VI (IV = Ge, Sn, Pb; VI = Se, Te) compounds are extensively studied. Lately, the obtained high‐performance thermoelectric solid solutions between IV‐VI and I‐V‐VI2 (I = Li, Na, K, Ag, Cu; V = Sb, Bi; VI = S, Se, Te) compounds have brought those complex chalcogenides back to the central point of thermoelectric community due to the emerging rich physical phenomena. Profiting from this effective approach, unveiling the underlying mechanism and understanding of alloying effect on the transport properties of these solid solutions becomes particularly significant. This review presents the latest progress in designing high‐performance IV‐VI/I‐V‐VI2 solid solutions and the underlining physical mechanisms, in which detailed discussion about the role of I‐V‐VI2 compounds play in optimizing individual properties of IV‐VI materials is made. This comprehensive review highlights the multiple effects of I‐V‐VI2 alloying on thermoelectric properties of IV‐VI compounds and will drive the related research interests aiming at developing new‐generation thermoelectric compounds in this family.

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Enhancing Thermoelectric Performance of PbTe-Based Compounds by Substituting Elements: A First Principles Study

Cited by 22 publications

References 43 publications

Silver-Antimony-Telluride: From First-Principles Calculations to Thermoelectric Applications

Silver-Antimony-Telluride: From First-Principles Calculations to Thermoelectric Applications

Towards a predictive route for selection of doping elements for the thermoelectric compound PbTe from first-principles

IV‐VI/I‐V‐VI₂ Thermoelectrics: Recent Progress and Perspectives

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Enhancing Thermoelectric Performance of PbTe-Based Compounds by Substituting Elements: A First Principles Study

Cited by 22 publications

References 43 publications

Silver-Antimony-Telluride: From First-Principles Calculations to Thermoelectric Applications

Silver-Antimony-Telluride: From First-Principles Calculations to Thermoelectric Applications

Towards a predictive route for selection of doping elements for the thermoelectric compound PbTe from first-principles

IV‐VI/I‐V‐VI2 Thermoelectrics: Recent Progress and Perspectives

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IV‐VI/I‐V‐VI₂ Thermoelectrics: Recent Progress and Perspectives