Engineering an atomic-level crystal lattice and electronic band structure for an extraordinarily high average thermoelectric figure of merit in n-type PbSe

Ge, Bangzhi; Lee, Hyungseok; Im, Jino; Choi, Y. S.; Kim, Shin‐Yeong; Lee, Jiyeong; Cho, Sung‐Pyo; Sung, Yung‐Eun; Choi, K.-Y.; Zhou, Chenyang; Shi, Zhongqi; Chung, In Jae

doi:10.1039/d3ee01226c

Cited by 39 publications

(16 citation statements)

References 68 publications

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“…Figure d shows the temperature-dependent Hall mobility of pristine and transition-metal-doped AgBiSe 1.995 . After transition-metal doping, the anion vacancy scattering is suppressed, which leads to the change of scattering mechanism and increases the Hall mobility. , The carrier concentration and Hall mobility simultaneously increase, which is beneficial for the power factor of a thermoelectric material. − Electrical resistivity, which is proportional to the reciprocal carrier mobility and concentration, decreases after transition-metal doping (Figure a). The plots still show a trend similar to those of the AgBiSe 2– x samples; however, the electrical resistivity peaks of the transition-metal-doped AgBiSe 1.995 appear at low temperatures, indicating downshifting of the phase transition.…”

Section: Resultsmentioning

confidence: 99%

Thermoelectric Optimization of n-Type AgBiSe₂ via Se Vacancy Control and Transition-Metal Doping

Wang,

Shen,

et al. 2023

ACS Appl. Energy Mater.

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Silver bismuth selenide (AgBiSe2) has garnered attention as a Pb-free material with a high thermoelectric efficiency owing to its intrinsically low thermal conductivity. Although pristine AgBiSe2 is an n-type material, in this study, a weak p-type intrinsic property is achieved in AgBiSe2 owing to the high sensitivity of its carrier type and concentration to Se vacancies. Herein, we report the enhancement of the thermoelectric performance of AgBiSe2 by introducing Se vacancies and aliovalent transition-metal doping at the Ag site. Se vacancies are first introduced to switch the conductivity of AgBiSe2 to the n-type and considerably increase the carrier concentration. Further, aliovalent transition-metal dopants are incorporated to tune the carrier concentration and thus increase the electrical conductivity of AgBiSe2. The electrical mobility and effective mass are also increased, which improves the electrical properties and enhances the power factor. The Ag0.97Cd0.03BiSe1.995 sample exhibited the highest dimensionless figure of merit (zT max) of ∼0.65 at 773 K and an average dimensionless zT avg of ∼0.39 between 323 and 773 K.

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Section: Resultsmentioning

confidence: 99%

Thermoelectric Optimization of n-Type AgBiSe₂ via Se Vacancy Control and Transition-Metal Doping

Wang,

Shen,

et al. 2023

ACS Appl. Energy Mater.

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“…From the electrical performance viewpoint, aliovalent doping and band engineering can enhance the S 2 σ by optimizing the carrier concentration ( n ) and increasing the carrier mobility ( μ ). , From the thermal performance viewpoint, defect engineering can suppress the κ l by enhancing phonon scattering. − Based on these strategies, the ZT of many thermoelectric materials, such as Bi 2 Te 3 , − PbTe, , GeTe, − PbSe, − and Cu 2 Se, , is extensively enhanced. However, the coupled relationship between carrier (contributing to μ ) and phonon scattering (contributing to κ l ) still severely limits the enhancement of ZT .…”

Section: Introductionmentioning

confidence: 99%

Decoupling Carrier-Phonon Scattering Boosts the Thermoelectric Performance of n-Type GeTe-Based Materials

Wang,

Liu,

Mao

et al. 2024

J. Am. Chem. Soc.

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The coupled relationship between carrier and phonon scattering severely limits the thermoelectric performance of n-type GeTe materials. Here, we provide an efficient strategy to enlarge grains and induce vacancy clusters for decoupling carrierphonon scattering through the annealing optimization of n-type GeTe-based materials. Specifically, boundary migration is used to enlarge grains by optimizing the annealing time, while vacancy clusters are induced through the aggregation of Ge vacancies during annealing. Such enlarged grains can weaken carrier scattering, while vacancy clusters can strengthen phonon scattering, leading to decoupled carrier-phonon scattering. As a result, a ratio between carrier mobility and lattice thermal conductivity of ∼492.8 cm 3 V −1 s −1 W −1 K and a peak ZT of ∼0.4 at 473 K are achieved in Ge 0.67 Pb 0.13 Bi 0.2 Te. This work reveals the critical roles of enlarged grains and induced vacancy clusters in decoupling carrier-phonon scattering and demonstrates the viability of fabricating high-performance n-type GeTe materials via annealing optimization.

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“…The efforts to reduce κ L are generally sorted into two aspects. One is constructing hierarchical architectures or nanostructures, including defects, − nanoprecipitation, − and grain boundaries . It should be noted that the possible increase of κ e needs to be carefully dealt with to prevent its harmful effect on ZT .…”

Section: Introductionmentioning

confidence: 99%

Ultralow Thermal Conductivity of a Chalcogenide System Pt₃Bi₄Q₉ (Q = S, Se) Driven by the Hierarchy of Rigid [Pt₆Q₁₂]^12– Clusters Embedded in Soft Bi-Q Sublattice

Wang,

Liang,

Zhang

et al. 2024

J. Am. Chem. Soc.

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Knowledge of structure–property relationships in solids with intrinsic low thermal conductivity is crucial for fields such as thermoelectrics, thermal barrier coatings, and refractories. Herein, we propose a new “rigidness in softness” structural scheme for intrinsic low lattice thermal conductivity (κL), which embeds rigid clusters into the soft matrix to induce large lattice anharmonicity, and accordingly discover a new series of chalcogenides Pt3Bi4Q9 (Q = S, Se). Pt3Bi4S9–x Se x (x = 3, 6) achieved an intrinsic ultralow κL down to 0.39 W/(m K) at 773 K, which is considerably low among the Bi chalcogenide thermoelectric materials. Pt3Bi4Q9 contains the rigid cubic [Pt6Q12]12– clusters embedded in the soft Bi-Q sublattice, involving multiple bonding interactions and vibration hierarchy. The hierarchical structure yields a large lattice anharmonicity with high Grüneisen parameters (γ) 1.97 of Pt3Bi4Q9, as verified by the effective scatter of low-lying optical phonons toward heat-carrying acoustic phonons. Consequently, the rigid-soft coupling significantly inhibits heat propagation, exhibiting low acoustic phonon frequencies (∼25 cm–1) and Debye temperatures (ΘD = 170.4 K) in Pt3Bi4Se9. Owing to the suppressed κL and considerable power factor (PF), the ZT value of Pt3Bi4S6Se3 can reach 0.56 at 773 K without heavy carrier doping, which is competitive among the pristine Bi chalcogenides. Theoretical calculations predicted a large potential for performance improvement via proper doping, indicating the great potential of this structure type for promising thermoelectric materials.

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Engineering an atomic-level crystal lattice and electronic band structure for an extraordinarily high average thermoelectric figure of merit in n-type PbSe

Abstract: We stabilize multiscale defect structures involving interstitial Cu, displaced Pb and Se atoms from the regular lattice points, dislocations driven by scarce anion vacancies, and nanoscale mosaics driven thermodynamically by...

Cited by 39 publications

References 68 publications

Thermoelectric Optimization of n-Type AgBiSe₂ via Se Vacancy Control and Transition-Metal Doping

Thermoelectric Optimization of n-Type AgBiSe₂ via Se Vacancy Control and Transition-Metal Doping

Decoupling Carrier-Phonon Scattering Boosts the Thermoelectric Performance of n-Type GeTe-Based Materials

Ultralow Thermal Conductivity of a Chalcogenide System Pt₃Bi₄Q₉ (Q = S, Se) Driven by the Hierarchy of Rigid [Pt₆Q₁₂]^12– Clusters Embedded in Soft Bi-Q Sublattice

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Engineering an atomic-level crystal lattice and electronic band structure for an extraordinarily high average thermoelectric figure of merit in n-type PbSe

Abstract: We stabilize multiscale defect structures involving interstitial Cu, displaced Pb and Se atoms from the regular lattice points, dislocations driven by scarce anion vacancies, and nanoscale mosaics driven thermodynamically by...

Cited by 39 publications

References 68 publications

Thermoelectric Optimization of n-Type AgBiSe2 via Se Vacancy Control and Transition-Metal Doping

Thermoelectric Optimization of n-Type AgBiSe2 via Se Vacancy Control and Transition-Metal Doping

Decoupling Carrier-Phonon Scattering Boosts the Thermoelectric Performance of n-Type GeTe-Based Materials

Ultralow Thermal Conductivity of a Chalcogenide System Pt3Bi4Q9 (Q = S, Se) Driven by the Hierarchy of Rigid [Pt6Q12]12– Clusters Embedded in Soft Bi-Q Sublattice

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Thermoelectric Optimization of n-Type AgBiSe₂ via Se Vacancy Control and Transition-Metal Doping

Thermoelectric Optimization of n-Type AgBiSe₂ via Se Vacancy Control and Transition-Metal Doping

Ultralow Thermal Conductivity of a Chalcogenide System Pt₃Bi₄Q₉ (Q = S, Se) Driven by the Hierarchy of Rigid [Pt₆Q₁₂]^12– Clusters Embedded in Soft Bi-Q Sublattice