Enhanced thermoelectric performance of skutterudite Co1−Ni Sn1.5Te1.5− with switchable conduction behavior

Valiyaveettil, Suneesh Meledath; Qorbani, Mohammad; Hsing, Cheng‐Rong; Chou, Tsung-Lin; Paradis-Fortin, Laura; Sabbah, Amr; Srivastava, Divya; Nguyen, Duc-Long; Ho, Thi-Thong; Billo, Tadesse; Ganesan, Peramaiyan; Wei, C. M.; Chen, Li‐Chyong; Chen, Kuei‐Hsien

doi:10.1016/j.mtphys.2022.100889

Cited by 4 publications

(4 citation statements)

References 63 publications

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“…There was a major reduction in the thermal conductivity of the Gd-filled composition compared to the unfilled composition, as reported previously for other filler elements [20][21][22]. The thermal conductivity was as low as 0.89 W/m.K at 773 K, which was lower than the minimum of ~3 W/m.K reported for other Gd-filled skutterudites synthesized at high pressure [26], and the ~1.5-2 W/m.K reported for other doped skutterudites [51,52]. This decrease in the thermal conductivity was a consequence of the rattling behavior of the Gd atom, which, as we described previously, showed an intrinsic disorder parameter ~5× and ~25× higher than those of the Co and Sb atoms, respectively.…”

Section: Thermoelectric Performancesupporting

confidence: 77%

Thermal Expansion and Rattling Behavior of Gd-Filled Co4Sb12 Skutterudite Determined by High-Resolution Synchrotron X-ray Diffraction

et al. 2022

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In this work, Gd-filled skutterudite GdxCo4Sb12 was prepared using one step method under high pressure in a piston-cylinder-based press at 3.5 GPa and moderate temperature of 800 °C. A detailed structural characterization was performed using synchrotron X-ray diffraction (SXRD), revealing a filling fraction of x = 0.033(2) and an average <Gd–Sb> bond length of 3.3499(3) Å. The lattice thermal expansion accessed via temperature-dependent SXRD led to a precise determination of a Debye temperature of 322(3) K, from the fitting of the unit-cell volume expansion using the second order Grüneisen approximation. This parameter, when evaluated through the mean square displacements of Co and Sb, displayed a value of 265(2) K, meaning that the application of the harmonic Debye theory underestimates the Debye temperature in skutterudites. Regarding the Gd atom, its intrinsic disorder value was ~5× and ~25× higher than those of the Co and Sb, respectively, denoting that Gd has a strong rattling behavior with an Einstein temperature of θE = 67(2) K. As a result, an ultra-low thermal conductivity of 0.89 W/m·K at 773 K was obtained, leading to a thermoelectric efficiency zT of 0.5 at 673 K.

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Section: Thermoelectric Performancesupporting

confidence: 77%

Thermal Expansion and Rattling Behavior of Gd-Filled Co4Sb12 Skutterudite Determined by High-Resolution Synchrotron X-ray Diffraction

et al. 2022

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“…There is a huge reduction in the thermal conductivity of the Gd-filled composition compared to the unfilled one, as reported before for other filler elements [20][21][22]. The thermal conductivity becomes as low as 0.89 W/m.K at 773 K, lower than the minimum of ~3 W/m.K reported for other Gd-filled skutterudites synthesized at high-pressure [26], and the ~1.5-2 W/m.K reported for other doped skutterudites [46,47]. Such a decrease in the thermal conductivity is a consequence of the rattling behavior of the Gd atom which, as we described before, shows an intrinsic disorder parameter ~5× and ~25× higher than those of the Co and Sb atoms, respectively.…”

Section: T [ K ]supporting

confidence: 68%

Thermal Expansion and Rattling Behavior of Gd-filled Co<sub>4</sub>Sb<sub>12</sub> Skutterudite Determined by High-Resolution Synchrotron X-Ray Diffraction

Rodrigues¹,

Gainza²,

Serrano‐Sánchez³

et al. 2022

Preprint

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In this work, Gd-filled skutterudite GdxCo4Sb12 has been prepared in one-step method under high-pressure conditions in a piston-cylinder press at 3.5 GPa and moderate temperature of 800 °C. A detailed structural characterization was performed using synchrotron X-ray diffraction (SXRD), revealing a filling fraction of x = 0.066(4) and an average &lt;Gd–Sb&gt; bond length of 3.3499(3) Å. The lattice thermal expansion accessed via temperature-dependent SXRD led to a precise determination of a Debye temperature of 322(3) K, from the fitting of the unit-cell volume expansion using the second order Grüneisen approximation. Such parameter, when evaluated from the mean square displacements of Co and Sb, displayed a value of 265(2) K, meaning that the application of the harmonic Debye theory underestimates the Debye temperature in skutterudites. Regarding the Gd atom, its intrinsic disorder value is ~5× and ~25× higher than those of Co and Sb, respectively, denoting that Gd has a strong rattling behavior with an Einstein temperature of θE = 67(2) K. As a result, an ultra-low thermal conductivity of ~0.89 W/m·K at 773 K was obtained, leading to a thermoelectric efficiency zT of ~0.5 at 673 K.

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“…This distortion causes significant reduction in lattice thermal conductivity, also harms electronic conduction. In the pursuit of improved electronic properties, researchers have investigated ternary skutterudite with extrinsic doping. − While substantial progress has been achieved in improving the thermoelectric (TE) properties of ternary skutterudite-based materials in their bulk form, a lack of reports on the ternary skutterudite-based thin films underscores a promising research avenue.…”

Section: Introductionmentioning

confidence: 99%

Boosting Thermoelectric Performance in Nanocrystalline Ternary Skutterudite Thin Films through Metallic CoTe₂ Integration

Jarwal,

Abbas,

Chou

et al. 2024

ACS Appl. Mater. Interfaces

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Metal−semiconductor nanocomposites have emerged as a viable strategy for concurrently tailoring both thermal and electronic transport properties of established thermoelectric materials, ultimately achieving synergistic performance. In this investigation, a series of nanocomposite thin films were synthesized, embedding metallic cobalt telluride (CoTe 2 ) nanophase within the nanocrystalline ternary skutterudite (Co-(Ge 1.22 Sb 0.22 )Te 1.58 or CGST) matrix. Our approach harnessed composition fluctuation-induced phase separation and in situ growth during thermal annealing to seamlessly integrate the metallic phase. The distinctive band structures of both materials have developed an ohmic-type contact characteristic at the interface, which raised carrier density considerably yet negligibly affected the mobility counterpart, leading to a substantial improvement in electrical conductivity. The intricate balance in transport properties is further influenced by the metallic CoTe 2 phase's role in diminishing lattice thermal conductivity. The presence of the metallic phase instigates enhanced phonon scattering at the interface boundaries. Consequently, a 2-fold enhancement in the thermoelectric figure of merit (zT ∼ 1.30) is attained with CGST-7 wt. % CoTe 2 nanocomposite film at 655 K compared to that of pristine CGST.

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Enhanced thermoelectric performance of skutterudite Co1−Ni Sn1.5Te1.5− with switchable conduction behavior

Cited by 4 publications

References 63 publications

Thermal Expansion and Rattling Behavior of Gd-Filled Co4Sb12 Skutterudite Determined by High-Resolution Synchrotron X-ray Diffraction

Thermal Expansion and Rattling Behavior of Gd-Filled Co4Sb12 Skutterudite Determined by High-Resolution Synchrotron X-ray Diffraction

Thermal Expansion and Rattling Behavior of Gd-filled Co<sub>4</sub>Sb<sub>12</sub> Skutterudite Determined by High-Resolution Synchrotron X-Ray Diffraction

Boosting Thermoelectric Performance in Nanocrystalline Ternary Skutterudite Thin Films through Metallic CoTe₂ Integration

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Enhanced thermoelectric performance of skutterudite Co1−Ni Sn1.5Te1.5− with switchable conduction behavior

Cited by 4 publications

References 63 publications

Thermal Expansion and Rattling Behavior of Gd-Filled Co4Sb12 Skutterudite Determined by High-Resolution Synchrotron X-ray Diffraction

Thermal Expansion and Rattling Behavior of Gd-Filled Co4Sb12 Skutterudite Determined by High-Resolution Synchrotron X-ray Diffraction

Thermal Expansion and Rattling Behavior of Gd-filled Co<sub>4</sub>Sb<sub>12</sub> Skutterudite Determined by High-Resolution Synchrotron X-Ray Diffraction

Boosting Thermoelectric Performance in Nanocrystalline Ternary Skutterudite Thin Films through Metallic CoTe2 Integration

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Boosting Thermoelectric Performance in Nanocrystalline Ternary Skutterudite Thin Films through Metallic CoTe₂ Integration