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Enhanced antimony telluride thermoelectric generators: From material synthesis to device applications
(2025-12-01)
Theekhasuk, Nattharika
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Sakdanuphab, Rachsak
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Voraud, Athorn
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Limsuwan, Pichet
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Sakulkalavek, Aparporn
This study investigates the effect of Bi₄O₄SeCl₂ (BOSC) addition (0–4 wt%) on the thermoelectric performance of p-type Bi₀.₅Sb₁.₅Te₃ synthesized via high-energy ball milling. XRD analysis revealed lattice incorporation at 1 wt% BOSC, while higher concentrations led to phase separation. The 1 wt% BOSC sample exhibited a significantly reduced total thermal conductivity of 0.28 W/m·K, compared to 0.46 W/m·K in the undoped sample, attributed to enhanced phonon scattering. Despite moderate decreases in electrical conductivity and Seebeck coefficient, a peak ZT of 1.02 at 50 °C was achieved—representing a ∼54 % improvement over the undoped material. Furthermore, a prototype thermoelectric module fabricated with BOSC-doped legs produced a power density of 17.6 mW/cm² under a 150 °C temperature gradient. These results demonstrate that BOSC is an effective additive for reducing thermal conductivity and enhancing overall thermoelectric performance, offering potential for energy harvesting applications at moderate temperatures.
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Enhanced thermoelectric properties of bismuth telluride via Ultra-Low thermal conductivity BOSC compound addition
(2024-12-01)
Theekhasuk, Nattharika
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Somdock, Nuttakrit
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Voraud, Athorn
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Limsuwan, Pichet
;
Sakdanuphab, Rachsak
This study aimed to enhance the thermoelectric properties of bismuth telluride by adding Bi<inf>4</inf>O<inf>4</inf>SeCl<inf>2</inf> (BOSC). Commercial N-type bismuth telluride was mixed with BOSC powder in varying concentrations. As the BOSC content increased, the carrier concentration also rose due to chlorine atoms acting as donor impurities. Despite this increase, the power factor values of the samples with BOSC additives did not significantly differ from those of the bare bismuth telluride sample. However, the total thermal conductivity decreased significantly with the addition of BOSC, reaching a minimum value of 0.54 W·m–1·K–1 at 150 °C for the sample with 1 wt% BOSC. Notably, the ZT value for the sample with 1 wt% BOSC was about 0.86, which is four times higher than that of the bare bismuth telluride sample. Our findings demonstrate superior thermoelectric performance, indicating a more efficient modification of thermoelectric properties through the addition of BOSC to the bismuth telluride matrix.
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Enhancing thermoelectric properties of Bi2Te3 film via CuI doping: Sputtering and solid iodination methods verified by ab initio calculation
(2024-04-01)
Khumtong, Tanakorn
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Theekhasuk, Nattharika
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Somdock, Nuttakrit
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Pluengphon, Prayoonsak
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Inceesungvorn, Burapat
We have introduced an innovative method for preparing CuI-doped Bi<inf>2</inf>Te<inf>3</inf> films for the first time, which was also validated through ab initio calculations. The chemical reaction between the Cu-Bi<inf>2</inf>Te<inf>3</inf> film and iodine was conducted using the solid iodination method at room temperature. The results from X-ray diffraction and energy-dispersive spectrometry suggest that the sputtering process, followed by the solid iodination method, holds promise for synthesizing CuI-doped Bi<inf>2</inf>Te<inf>3</inf> films. Additionally, appropriately doping Bi<inf>2</inf>Te<inf>3</inf> with CuI enhances the (00l) crystal orientation, increases carrier concentration and mobility, resulting in improved electrical conductivity. Furthermore, our calculation results align with our experimental findings. An excess of substitutional CuI dopant tends to generate secondary phases, leading to alterations in the intrinsic conductivity and a reduction in the thermoelectric properties of Bi<inf>2</inf>Te<inf>3</inf>. Leveraging the enhanced electrical transport properties achieved through CuI doping, the maximum power factor of the (CuI)<inf>0.2</inf>Bi<inf>2</inf>Te<inf>2.9</inf> film reaches approximately 2.40 × 10−3 W/mK2 at 423 K, representing a 66 % enhancement compared to that of the Bi<inf>2</inf>Te<inf>2.9</inf> film, which has a power factor of 1.44 × 10−3 W/mK2.
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Enhancement of thermoelectric properties in rapidly synthesised β-Cu2Se using optimized Cu content and microwave hybrid heating
(2024-01-15)
Sakulkalavek, Aparporn
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Rudradawong, Chalermpol
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Gobpant, Jakrit
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Harnwunggmoung, Adul
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Limsuwan, Pichet
To our knowledge, this is the first study to successfully synthesise high-temperature-phase copper selenide (β-Cu<inf>2</inf>Se) at room temperature using rapid microwave hybrid heating (MHH). Controlling the starting Cu/Se ratio is the critical parameter for adjusting the content of α- and β-phases in the as-synthesised sample. The relatively low Cu composition causes impurities to form in the Cu<inf>3</inf>Se<inf>2</inf> phase, deteriorating the thermoelectric (TE) properties of the Cu<inf>2</inf>Se material. The β phase formation at room temperature promotes electrical conductivity. The thermal conductivities of the Cu<inf>2.0</inf>Se samples were 0.5–0.8 Wm−1K−1 at 303–673 K. A strong electronic-phonon interaction may potentially couple electronic thermal conductivity (κ<inf>e</inf>) and lattice thermal conductivity (κ<inf>L</inf>), resulting in incomplete separability of κ<inf>L</inf> and κ<inf>e</inf> in the β-Cu<inf>2.0</inf>Se sample. The Cu<inf>2.0</inf>Se exhibited a ZT value of 0.65 at 523 K because of its considerably lowered thermal conductivity.
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Understanding the effect of sputtering pressures on the thermoelectric properties of GeTe films
(2022-02-10)
Daichakomphu, Noppanut
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Abbas, Suman
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Chou, Ta Lei
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Chen, Li Chyong
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Chen, Kuei Hsien
In this work, we study the effect of sputtering pressures on the thermoelectric properties of GeTe films. The working pressures were differentiated from 3 to 30 mTorr, and the as-deposited films were annealed at 623 K for 10 min in Ar atmosphere. The results show that the working pressure has a significant effect on the Ge content and crystalline size. The turning trend of the Seebeck coefficient with different sputtering pressures corresponds to the Ge content. The surface morphology of annealed film will change from cracks to voids with increasing sputtering pressure. This behavior can be explained by the growth mechanisms model. The voids and relatively low crystalline size of GeTe films affect to the reduction of the electrical conductivity. In addition, the void content decreased as film thickness was increased. Therefore, controlling the working pressures in the sputtering process and film thickness is important for the thermoelectric performance of GeTe thin film. In our work, we prove that the thermoelectric properties of GeTe films could be optimized effectively by simply tuning different sputtering conditions.
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Graphene addition improved figure of merit in SnTe prepared by the rapid hybrid microwave solid-state method
(2022-02-01)
Gobpant, Jakrit
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Somdock, Nuttakrit
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Limsuwan, Pichet
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Sakulkalavek, Aparporn
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Sakdanuphab, Rachsak
We successfully synthesised SnTe-based powders (SnTe, Sn<inf>0.95</inf>Bi<inf>0.05</inf>Te, and SnTe with graphene addition) by a hybrid microwave solid-state method. This demonstrated comparable thermoelectric performance to the conventional heating method but had low energy consumption and rapid synthesis. Graphene addition to SnTe materials resulted in significant reduction of thermal conductivity. The SnTe with 5 wt% graphene exhibited a reduction in overall thermal conductivity from ∼10 W m−1 K−1 for SnTe to ∼2 W m−1 K−1 at 325 K and showed a moderate power factor. The Debye model was used to explain the origin of the effects of graphene on lattice thermal conductivity. The dimensionless figure of merit was increased by five times, from 0.07 for SnTe to 0.35 for SnTe with 5 wt% graphene. Our results demonstrated an effective method and additive material to synthesise and enhance the thermoelectric properties of SnTe materials.
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Improving the thermoelectric properties of thick Sb2Te3 film via Cu doping and annealing deposited by DC magnetron sputtering using a mosaic target
(2021-11-01)
Theekhasuk, Nattharika
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Sakdanuphab, Rachsak
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Nuthongkum, Pilaipon
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Pluengphon, Prayoonsak
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Harnwunggmoung, Adul
Thick Cu-doped Sb<inf>2</inf>Te<inf>3</inf> films were deposited on flexible substrate by DC magnetron sputtering from a mosaic Cu–Sb<inf>2</inf>Te<inf>3</inf> target. The Cu-doped Sb<inf>2</inf>Te<inf>3</inf> films were vacuum annealed to improve their thermoelectric properties. Density functional theory was used to clarify the internal mechanism of the Cu doped into the Sb<inf>2</inf>Te<inf>3</inf> system. The results showed that Cu substitution on a Sb site induced electronic states or impurity peaks of Sb<inf>2</inf>Te<inf>3</inf> at a valence band maximum. The carrier concentration of the Cu-doped Sb<inf>2</inf>Te<inf>3</inf> films increased as the Cu-doped concentration increased. However, the crystallite size and Seebeck coefficient of the Cu-doped Sb<inf>2</inf>Te<inf>3</inf> films decreased as the Cu-doped concentration increased. Post-annealing treatment improved the microstructure and thermoelectric properties of the Cu-doped Sb<inf>2</inf>Te<inf>3</inf> films. The maximum electrical conductivity and power factor values of 754.20 S/cm at 50 °C and 1.56 10−3 W/mK2 at 100 °C were obtained in the annealed film with a Cu-doped concentration of 3 at%.
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Energy-saving synthesis and β-phase enhancement of Cu2Se thermoelectric materials via the microwave hybrid heating technique
(2021-10-25)
Rudradawong, Chalermpol
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Sukwisute, Pisan
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Limsuwan, Pichet
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Harnwunggmoung, Adul
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Horprathum, Mati
Thermoelectric generators harvest energy from waste heat and convert it to electricity. β-Cu<inf>2</inf>Se is a candidate for them due to its outstanding thermoelectric properties and its environmentally friendly component elements. A microwave hybrid heating (MHH) method was used for the fast synthesis and enhancement of β-Cu<inf>2</inf>Se materials. The effects of the MHH reaction time on the phase microstructure and thermoelectric properties of the Cu<inf>2</inf>Se material were investigated, and the MHH method was compared with the conventional heating method. The X-ray diffraction patterns of samples, synthesized via the MHH method, showed monoclinic- (α) and cubic- (β) Cu<inf>2</inf>Se crystalline structures, whereas a single monoclinic-(α) structure was identified in a sample, synthesized via a conventional heating method. In addition, the β-Cu<inf>2</inf>Se phase was enhanced with increased MHH reaction time. The carrier concentration increased with β-Cu<inf>2</inf>Se content, which increased electrical conductivity and decreased the Seebeck coefficient. The Cu+ ions in the β-Cu<inf>2</inf>Se phase led to the reduced thermal conductivity. A low thermal conductivity of 0.86 W m−1 K−1 and a maximum dimensionless figure of merit of 0.32 at 523 K were realized for 10 min MHH sample. Finally, MHH showed very low energy consumption and saved time, which are essential for industrialization.
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Effect of real working environment/formation of oxide phase on thermoelectric properties of flexible Sb2Te3 films
(2019-09-01)
Somdock, Nuttakrit
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Harnwunggmoung, Adul
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Sakulkalavek, Aparporn
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Sakdanuphab, Rachsak
Flexible Sb<inf>2</inf>Te<inf>3</inf> thin films, for thermoelectric generator applications, were deposited by DC magnetron sputtering. As-deposited films were annealed in air to simulated a realistic operating environment. The oxidation behavior of the films was studied by monitoring their phase change on exposure to air at different temperatures between 50 and 300 °C for annealing times from 1 to 15 h. Oxidation of Sb and Te formed Sb<inf>2</inf>Te<inf>4</inf> and TeO<inf>2</inf> phases when annealing above 100 °C and Sb<inf>2</inf>Te<inf>3</inf> decomposed into oxide phases at an annealing temperature of 250 °C for 15 h. The thermoelectric performance decreased as the content of Sb<inf>2</inf>O<inf>4</inf> and TeO<inf>2</inf> phases increased. These findings show the limitations of Sb<inf>2</inf>Te<inf>3</inf> films operating in air without vacuum or a protective environment. We propose that the kinetic growth of oxide formation on the Sb<inf>2</inf>Te<inf>3</inf> thin films depend on chemical activation energy and oxygen diffusion through the oxide barrier by the variation of annealing temperature and annealing time, respectively.
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Effects of annealing temperature on the structural, mechanical and electrical properties of flexible bismuth telluride thin films prepared by high-pressure RF magnetron sputtering
(2017-09-01)
Singkaselit, Kamolmad
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Sakulkalavek, Aparporn
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Sakdanuphab, Rachsak
In this work BixTey thin films were deposited on polyimide substrate by a high-pressure RF magnetron sputtering technique. The deposited condition was maintained using a high pressure of 1.3 × 10-2 mbar. The as-deposited films show Bi<inf>2</inf>Te<inf>3</inf> structure with Te excess phase (Te-rich Bi<inf>2</inf>Te<inf>3</inf>). After that, as-deposited films were annealed in the vacuum chamber under the N<inf>2</inf> flow at temperatures from 250 to 400 °C for one hour. The microstructure, cross-section, [Bi]:[Te] content, and the mechanical, electrical and thermoelectric properties of as-deposited and different annealed films were investigated. It was found that the annealing temperature enhanced the crystallinity and film density for the temperature range 250-300 °C. However, the crystal structure of Bi<inf>2</inf>Te<inf>3</inf> almost changed to the BiTe structure after annealing the films above 350 °C, due to the re-evaporation of Te. Nano-indentation results and cross-section images indicated that the hardness of the films related to the film density. The maximum hardness of 2.30 GPa was observed by annealing the films at 300 °C. As a result of an improvement in crystallinity and phase changes, the highest power factor of 11.45 × 10-4 W m-1K-2 at 300 °C with the carrier concentration and mobility of 6.15 × 1020 cm-3 and 34.03cm2 V-1 s-1, respectively, was achieved for the films annealed at 400 °C.

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