High-Performance Thermoelectrics from Cellular Nanostructured Sb2Si2Te6

Luo, Yubo; Cai, Songting; Hao, Shiqiang; Pielnhofer, Florian; Hadar, Ido; Luo, Zhong‐Zhen; Xu, Jianwei; Wolverton, Chris; Dravid, Vinayak P.; Pfitzner, Arno; Yan, Qingyu; Kanatzidis, Mercouri G.

doi:10.1016/j.joule.2019.10.010

Cited by 114 publications

(167 citation statements)

References 65 publications

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“…Established routes to achieve low κlat include: (1) enhancing phonon scattering through the introduction of point defects, 2 nanostructures 3 and all-scale hierarchical architec-tures; [4][5] and (2) exploring new materials with inherently low lattice thermal conductivity, typically originating from complex crystal structures and strong lattice anharmonicity. 6 Examples of the second approach include In4Se3, 7 Ag9GaSe6 8 , Sb2Si2Te6 3 , AgCuTe 9 , Ba5Cu8In2S12 10 and SnSe. [11][12][13][14] SnSe is a rapidly emerging thermoelectric compound.…”

Section: ■ Introductionmentioning

confidence: 99%

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe₃ by High-Entropy Engineering

Luo

Hao²,

Cai³

et al. 2020

J. Am. Chem. Soc.

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139

136

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We investigate the structural and physical properties of the AgSnmSbSem+2 system with m=1-20 (i.e. SnSe matrix and ~5-50 % AgSbSe2) from length scales ranging from atomic, nano and macro. We find the 50:50 composition, with m=1 (i.e. AgSnSbSe3), forms a stable cation disordered cubic rock-salt p-type semiconductor with a special multipeak electronic valence band structure. AgSnSbSe3 has an intrinsically low lattice thermal conductivity of ~0.47 Wm -1 K -1 at 673 K owing to the synergy of cation disorder, phonon anharmonicity, low phonon velocity, and low-frequency optical modes. Furthermore, Te alloying on the Se sites creates a quinary high entropy NaCl-type solid solution AgSnSbSe3-xTex with randomly disordered cations and anions. The extra point defects and lattice dislocations lead to glass-like lattice thermal conductivities of ~0.32 Wm -1 K -1 at 723 K and higher hole carrier concentration than AgSnSbSe3. Concurrently, the Te alloying promotes greater convergence of the multiple valence band maxima in AgSnSbSe1.5Te1.5, the composition with the highest configurational entropy. Facilitated by these favorable modifications, we achieve a high average power factor of ~9.54 μWcm -1 K -2 (400-773 K), a peak thermoelectric figure of merit ZT of 1.14 at 723 K and a high average ZT of ~1.0 over a wide temperature range of 400-773 K in AgSnSbSe1.5Te1.5.

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Section: ■ Introductionmentioning

confidence: 99%

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe₃ by High-Entropy Engineering

Luo

Hao²,

Cai³

et al. 2020

J. Am. Chem. Soc.

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139

136

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“…[7][8][9][10][11][12][13][14][15] Moreover, to induce phonon scattering, complex crystal structure, large lattice anharmonicity and defect engineering such as nanocomposites, dislocation and strain have also been extensively leveraged to reduce lattice thermal conductivity. [16][17][18][19][20] Among the prominent thermoelectric compounds, GeTe has been overlooked for decades, and was mainly used as an alloy in TAGS compounds despite the fact that GeTe has a similar or even superior electronic band structure to PbTe. 21 A pervasive problem hindering widespread attention to this compound is its high concentration of holes in pristine GeTe (p-type) as well as the difficulty in achieving n-type GeTe via doping.…”

Section: Introductionmentioning

confidence: 99%

Tailoring the phase transition temperature to achieve high-performance cubic GeTe-based thermoelectrics

Suwardi

Cao

et al. 2020

J. Mater. Chem. A

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“…In addition, another significant theme is to search for intrinsically low thermal conductivity, like SnSe 19 , 20 , 21 as well as superionic semiconductors Cu 2 Se 22 and Ag 9 GaSe 6 23 , and to build up diverse phonon scattering centers extrinsically, such as introducing rattling phonon modes in open frameworks in Ba 8 Ga 16 Ge 30 24 and AgBi 3 S 5 , 25 and engineering hierarchical defect structures (atomic alloying, nanostructured inclusions and grain-boundary interfaces) to scatter phonons with full length scales. 26,27,28 To promote energy conversion efficiency, a large temperature gradient is beneficial. 29 Hence, thermoelectric materials with higher operating temperatures are attractive, especially for radioisotope thermoelectric generators (RTGs) used in deep space missions.…”

Section: Introductionmentioning

confidence: 99%

Crystal Structure and Atomic Vacancy Optimized Thermoelectric Properties in Gadolinium Selenides

et al. 2020

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Thermoelectric materials enable the mutual energy conversion of waste heat and electricity, critical to relieve global energy crisis. Hightemperature thermoelectric materials are special species due to their high-temperature stability and noticeable energy conversion efficiency.Here, we report a systematic investigation on high-temperature thermoelectric gadolinium selenides, cubic Gd 3-x Se 4 (x = 0.16, 0.21 and 0.25) and orthorhombic Gd 2 Se 3-y (y = 0.02, 0.06 and 0.08). High energy synchrotron x-ray diffraction and total scattering are used to investigate the crystallographic and local structures. The atomic-scale cluster of Gd vacancy in cubic Gd 2.84 Se 4 is observed by employing the reverse Monte Carlo simulation. For cubic Gd 3-x Se 4 , its carrier concentration is tuned and multiple conduction bands are incorporated by adjusting Gd vacancy. Experimentally, the gradual increase in effective masses is evidently observed in cubic Gd 3-x Se 4 , which is consistent with the density functional theory (DFT) calculation. A reasonable peak zT value of 0.27 is achieved at 850 K for Gd 2.84 Se 4 . On the other hand, adjusting Se vacancy enables the optimization of electron concentration for orthorhombic Gd 2 Se 3-y phase. Its low deformation potential (Ξ = 12eV) with single conduction band gives rise to enhanced electron mobility and higher peak zT value of 0.54 at 850 K for Gd 2 Se 2.98 . In addition, a higher zT of 1.2 at1200 K is reasonably predicted for Gd 2 Se 2.98 by using quality factor analysis. This work not just presents a systematic crystallographic investigation of gadolinium selenides, but also provides a deep insight into the charge transport and phonon scattering mechanisms. This study facilitates the exploration of more hightemperature thermoelectric materials.

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High-Performance Thermoelectrics from Cellular Nanostructured Sb2Si2Te6

Cited by 114 publications

References 65 publications

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe₃ by High-Entropy Engineering

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe₃ by High-Entropy Engineering

Tailoring the phase transition temperature to achieve high-performance cubic GeTe-based thermoelectrics

Crystal Structure and Atomic Vacancy Optimized Thermoelectric Properties in Gadolinium Selenides

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High-Performance Thermoelectrics from Cellular Nanostructured Sb2Si2Te6

Cited by 114 publications

References 65 publications

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe3 by High-Entropy Engineering

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe3 by High-Entropy Engineering

Tailoring the phase transition temperature to achieve high-performance cubic GeTe-based thermoelectrics

Crystal Structure and Atomic Vacancy Optimized Thermoelectric Properties in Gadolinium Selenides

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High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe₃ by High-Entropy Engineering

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe₃ by High-Entropy Engineering