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INORGANIC CHEMISTRY · 2018 · IF 4.7

Thermoelectric Material SnPb2Bi2S6: The 4,4L Member of Lillianite Homologous Series with Low Lattice Thermal Conductivity

Jingpeng Li,Yiming Zhou,Shiqiang Hao,Tianyan Zhang,Chris Wolverton,Jing Zhao,Li-Dong Zhao

Although the binary sulfides Bi2S3, PbS, and SnS have attracted extensive interest as thermoelectric materials, no quaternary sulfides containing Sn/Pb/Bi/S elements have been reported. Herein, we report the synthesis of a new quaternary sulfide, SnPb2Bi2S6, which crystallizes in the orthorhombic space group Pnma with unit cell parameters of a = 20.5458(12) Å, b = 4.0925(4) Å, c = 13.3219(10) Å. SnPb2Bi2S6 has a lillianite-type crystal structure consisting of two alternately aligned NaCl-type structural motifs separated by a mirror plane of PbS7 monocapped trigonal prisms. In the lillianite homologous series, SnPb2Bi2S6 can be classified as 4,4L, where the superscripted numbers indicate the maximum numbers of edge-sharing octahedra in the two adjacent NaCl-shaped slabs along the diagonal direction. The obtained SnPb2Bi2S6 phase exhibited good thermal stability up to 1000 K and n-type degenerate semiconducting behavior, with a power factor of 3.7 μW cm–1 K–2 at 773 K. Notably, this compound exhibited a very low lattice thermal conductivity of 0.69–0.92 W m–1 K–1 at 300–1000 K. Theoretical calculations revealed that the low thermal conductivity is caused by the complex crystal structure and the related elastic properties of a low Debye temperature, low phonon velocity, and large Grüneisen parameters. A reasonable figure of merit (ZT) of ∼0.3 was obtained at 770 K.

研究领域: 材料科学 · 物理学
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Physica Status Solidi-Rapid Research Letters · 2020 ·Vol. 14 ·期 4 ·1900679 · IF 2.291

Enhanced Thermoelectric Performance of Bi2Te2.7Se0.3/Bi2S3 Synthesized by Anion Exchange Method

Xi Chen,Fanggong Cai,Chuanrong Liu,Rong Dong,Lanxin Qiu,Lili Jiang,Guocai Yuan,Qinyong Zhang

Decoupling the electric conductivity, Seebeck coefficient, and thermal conductivity is a core issue to improve the properties of thermoelectric materials by tuning the electron and phonon transport properties. Herein, Bi 2 Te 2.7 Se 0.3 /Bi 2 S 3 heterostructure is successfully synthesized by a simple anion exchange method with Bi 2 Te 2.7 Se 0.3 as the starting material. The Bi 2 Te 2.7 Se 0.3 /Bi 2 S 3 heterointerfaces can achieve an effective phonon scattering and significant decrease in thermal conductivity, while maintaining a high power factor, resulting in an enhanced figure of merit ( ZT ). By controlling the concentration of Bi 2 Te 2.7 Se 0.3 /Bi 2 S 3 heterointerfaces, the carrier-transporting and phonon-scattering behaviors can be simultaneously optimized. A maximum ZT of 0.7 is obtained at 473 K, which is 23% higher than that of pure Bi 2 Te 2.7 Se 0.3 . In addition, the average ZT at 300–548 K increases from 0.49 to 0.61, which is 25% higher than that of pure Bi 2 Te 2.7 Se 0.3 .

研究领域: 材料科学 · 物理学
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ACS Applied Materials & Interfaces · 2017 · IF 7.504

Enhancing the zT Value of Bi-Doped Mg2Si0.6Sn0.4 Materials through Reduction of Bipolar Thermal Conductivity

Wenhao Fan,Shaoping Chen,Bo Zeng,Qiang Zhang,Qingsen Meng,Wenxian Wang,Zuhair A. Munir

Solid solutions of Mg2Si0.6Sn0.4–xBix with 0 ≤ x ≤ 0.03 were prepared by a one-step synthesis and consolidation method, using MgH2 as a starting material. The thermoelectric properties of these samples were evaluated over the temperature range 300–775 K. Figure of merit, zT, values were determined over this range for all compositions and found to increase with temperature reaching a value of 1.36 at 775 K for samples with x = 0.02. Examination of the components of the total thermal conductivity showed that the bipolar thermal conductivity is suppressed by an increase in the band gap, resulting from solid solution formation, and by low minority carrier mobility. The suppression of the bipolar thermal conductivity is believed to be the consequence of charged grain boundaries.

CAS / MDL: 7440-69-9 7440-21-3
研究领域: 材料科学 · 热电学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2017 · IF 3.133

Enhancing thermoelectric performance of SnTe via nanostructuring particle size

Xiao Zhang,Yiming Zhou,Yanling Pei,Yuexing Chen,Bifei Yuan,Shuangmei Zhang,Yuan Deng,Shengkai Gong,Jiaqing He,Li-Dong Zhao

SnTe, one lead-free analogue of PbTe, has been paid attention in thermoelectric community because it has the similar rock-salt crystal structure and electronic band structure . However, SnTe possesses a very high total thermal conductivity (∼10.0 W m −1  K −1  at room temperature) and a mediocre ZT (∼0.2 at 723 K). In this study, to reduce its thermal conductivity, we prepare SnTe samples by melting reaction followed by mechanical alloying and spark plasma sintering . We demonstrate that both total thermal conductivity and lattice thermal conductivity can be considerably reduced through reducing particle size from micro-scale to nano-scale via facially mechanical alloying method. Experimental results show that the total thermal conductivity at room temperature can be reduced from ∼10 W m −1  K −1 for SnTe ingot to ∼3Wm −1  K −1 for SnTe with mechanical alloying 25 h. Correspondingly, the lattice thermal conductivity at room temperature was reduced from ∼5Wm −1  K −1 to ∼2Wm −1  K −1 . Combination of reduced thermal conductivity and moderate power factor, average ZT ave can be increased by 33.3%, from 0.09 for SnTe ingot to 0.12 for SnTe with nano-grain size.

CAS / MDL: 7440-31-5 13494-80-9
研究领域: 材料科学 · 热电学
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Enhancing power factor and ZT in non-toxic Bi2S3 bulk materials via band engineering and electronic structure modulation

Yu Wang,Jing Feng,Zhen-Hua Ge

Bismuth sulfide-based thermoelectric materials have attracted considerable interest owing to their abundance of raw materials and non-toxicity. However, their poor electrical properties, particularly their conductivity, have limited their practical applications. In this work, a melting method and spark plasma sintering were employed to synthesize bulk Bi 2 S 3 materials. The dopant MoCl 5 was used to regulate the electrical properties of Bi 2 S 3 . The results showed that Mo can significantly enhance the conductivity of Bi 2 S 3 compared to other transition metals. The doped sample exhibited an almost two-orders-of-magnitude rise in conductivity relative to the Bi 2 S 3 sample in its pure form. Due to its superior conductivity, the Bi 2 S 3 +1 wt% MoCl5 sample achieved an excellent power factor of 550 μW m −1 K −1 which is the maximum ever reported in the Bi 2 S 3 system. Simultaneously, the ZT value of this sample approached 0.70 at 773 K, which is a six-fold improvement compared to the pristine sample. Density functional theory was applied to understand the electronic structure changes of the Mo-doped sample, which revealed that trace amounts of MoCl 5 doping could significantly boost the density of states in the vicinity of the conduction band and shift the Fermi level to the valence band, leading to a reduction in the bandgap and an increase in free electrons. This work offers new insights into the role of Mo elements in thermoelectric materials and provides a good strategy for augmenting the thermoelectric figures of merit of other n-type thermoelectric materials with inadequate electrical conductivity in the future.

研究领域: 材料科学 · 热电材料
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Materials · 2024 ·Vol. 17 ·期 7 ·1509 · IF 3.1

Optimizing Thermoelectric Performance of Hybrid Crystals Bi2O2Se1−xTex in the Bi2O2X System

Fan Xie,Zhiyao Ma,Jian Zhou

In addressing the global need for sustainable energy conversion, this study presents a breakthrough in thermoelectric materials research by optimizing the Bi2O2Se1–xTexsystem in the Bi2O2Se/Bi2O2Te pseudobinary series. Leveraging the principles of innovative transport mechanisms and defect engineering, we introduce tellurium (Te) doping into Bi2O2Se to enhance its thermoelectric properties synergistically. With the help of various advanced characterization tools such as XRD, SEM, TEM, XPS, FTIR, TGA, LFA, and DSC, combined with relevant resistance and density measurement techniques, we conducted an in-depth exploration of the complex interactions between various factors within thermoelectric materials. We recognize that the balance and synergy of these factors in the thermoelectric conversion process are crucial to achieving efficient energy conversion. Through systematic research, we are committed to revealing the mechanisms of these interactions and providing a solid scientific foundation for the optimal design and performance enhancement of thermoelectric materials. Finally, the advantage coefficient (ZT) of the thermoelectric material has been significantly improved. The crystallographic analysis confirms the formation of a continuous series of mixed crystals with varying Te concentrations, adhering to Vegard’s law and exhibiting significant improvements in electrical and thermal conductivities. The Bi2O2Se1–xTexcrystals, particularly the Bi2O2Se0.6Te0.4composition, demonstrate a peak ZT of 0.86 at 373 K. This achievement aligns with recent advancements in defect-enabled mechanisms and band convergence and sets a new standard for high-performance thermoelectrics. The study’s findings contribute significantly to the ongoing quest for efficient thermal-to-electrical energy conversion, offering a promising avenue for future sustainable energy technologies.

CAS / MDL: 7440-69-9 7782-49-2
研究领域: 材料科学 · 能源转换技术
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Nanomaterials · 2022 ·Vol. 12 ·期 9 ·1575 · IF 5.719

Enhanced Thermoelectric Properties of Te Doped Polycrystalline Sn0.94Pb0.01Se

Fujin Li,Lin Bo,Ruipeng Zhang,Sida Liu,Junliang Zhu,Min Zuo,Degang Zhao

Thermoelectric materials can directly convert heat and electricity, which is a kind of promising energy material. In view of cost and mechanical properties, polycrystalline SnSe material with highzTvalue is greatly desired. In this study, polycrystalline Sn0.94Pb0.01Se1-xTexsamples were prepared by the vacuum melting–hot pressing sintering method. Sn vacancies, Pb and Te atoms were simultaneously introduced into the polycrystalline SnSe. The power factor of Sn0.94Pb0.01Se1-xTexsamples was decreased, which could be attributed to the generation ofn-type semiconductor SnSe2. In addition, the phonons were strongly scattered by point defects and dislocations, which led to the decrease of thermal conductivity—from 0.43 Wm−1K−1to 0.29 Wm−1K−1at 750 K. Finally, the polycrystalline Sn0.94Pb0.01Se0.96Te0.04sample achieved the maximumzTvalue of 0.60 at 750 K.Keywords:SnSe;nanoparticles;zT;thermoelectric;TEM

研究领域: 材料科学 · 能源工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Simultaneous realization of high power factor and low thermal conductivity in medium-entropy La-doped (Sr1/3Ba1/3Ca1/3)1-xLaxTiO3 oxides with porous structure

Juan Bi,Yuxin Liang,Yang Bai,Baoning Cui,Zhaopeng Lu,Bangsheng Li

Some studies have proven the effectiveness of high-entropy alloying in reducing lattice thermal conductivity; however, the synchronous degradation in carrier mobility limits the thermoelectric properties of high-entropy materials. Herein, we present a series of medium-entropy oxides (Sr 1/3 Ba 1/3 Ca 1/3 ) 1-x La x TiO 3 (x = 0.05, 0.1, 0.15) with different levels of La doping, breaking the trade-off between carrier and phonon transport. The medium-entropy design helps keep the carrier mobility at a moderate level while modulating the carrier concentration through La 3+ doping, thereby yielding a peak power factor value of 1842 μW/(m⋅K 2 ) at 773 K. Meanwhile, the incorporation of nano-micro-porous structure and medium entropy effect leads to a significant reduction in lattice thermal conductivity, reaching 2.3 W/(m⋅K) at 1073 K. Consequently, a ZT max value of 0.67 is obtained for the MEP-10La sample at 1073 K, which is one of the state-of-the-art ZT values reported for the SrTiO 3 -based materials. The present work provides a viable approach for the development of thermoelectric materials with enhanced performance.

研究领域: 材料科学 · 热电学
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CERAMICS INTERNATIONAL · 2025 · IF 5.6

High thermoelectric performance of polycrystalline SnSe prepared by cold sintering

Lijie Shi,Jun Ding,Xiangbin Chen,Xiang Qu,Zhiquan Chen,Man Jiang

Low-cost preparation of thermoelectric materials is crucial for reducing energy consumption. In this study, we prepared the nanopolycrystalline SnSe ceramic by combining the hydrothermal and cold sintering process (CSP) at a relatively low temperature of 170 °C from 300 MPa to 510 MPa. XRD analyses indicated that a pronounced preferential orientation of the cold sintered SnSe along the (h00) directions. SEM observations showed that a well-crystallized layered structure was formed. All SnSe samples exhibit remarkably low thermal conductivity of 0.3 Wm −1 K −1  at 773 K. This low thermal conductivity can be attributed to the use of ethanol as a transient liquid phase and the application of high pressure, which promotes the rearrangement of nanopolycrystals and introduces high densities of dislocations and stacking faults in SnSe. A maximum ZT value of 1.35 at 773 K was achieved for the 405 MPa sintered sample. This study provides a cost-effective and efficient strategy for the preparation of polycrystalline SnSe thermoelectric material.

研究领域: 材料科学 · 能源材料
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JOURNAL OF NANOPARTICLE RESEARCH · 2015 ·Vol. 17 ·期 7 ·1-7 · IF 2.184

Facile synthesis of monodisperse Cu3SbSe4 nanoparticles and thermoelectric performance of Cu3SbSe4 nanoparticle-based materials

Wu Yimin,Qiao Xvsheng,Fan Xianping,Zhang Xianghua,Cui Shuo,Wan Jun

In this study, large-scale synthesis of Cu 3 SbSe 4 and Cu 3 Sb 0.98 Sn 0.02 Se 4 nanoparticles with a narrow size distribution was achieved through a rapid-injection route. These nanoparticles showed a monodisperse and quasi-spherical morphology. The Cu 3 SbSe 4 and Cu 3 Sb 0.98 Sn 0.02 Se 4 nanoparticle-based bulk materials were then prepared by hot-pressed sinter of the nanoparticles, and their thermoelectric performances were systematically studied. Due to the reduced lattice thermal conductivity from enhanced phonon scattering at the grain interfaces of the bulk materials, the maximum ZT value of the Cu 3 Sb 0.98 Sn 0.02 Se 4 bulk materials reached 0.50 at 575 K.

研究领域: 材料科学 · 纳米技术 · 热电材料
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2023 ·Vol. 34 ·期 6 ·1-8 · IF 2.8

Fast synthesis and thermoelectric properties of BixCu2−3xSe0.95Te0.05 (x = 0, 0.001, 0.002, 0.003, 0.004)

Xue Lisha,Wang Yuan,Zhu Shuangmei,Mao Qianhui,Jia Xiaopeng,Zhang Yuewen

We have synthesized the quaternary copper selenide Bi x Cu 2−3 x Se 0.95 Te 0.05 compounds by high-pressure followed with ball milling method and investigated their thermoelectric properties. The crystal structure and element doping are characterized and verified by the X-ray diffraction, high-resolution transmission electron microscope and X-ray photoelectron spectroscopy. Compared with other samples, the samples with x  = 0.001 and 0.002 have larger layered grain size and smaller grain boundary. This may lead to the reduction of resistivity in a wide temperature range, thus realizing the optimization of electronic characteristics. The dislocation-induced lattice strain fluctuations may cause the abrupt thermal conductivity, which is contrary to the previous results. Eventually, a peak value of zT  = 1.03 at 873 K is obtained for Bi 0.001 Cu 1.997 Se 0.95 Te 0.05 and Bi 0.002 Cu 1.994 Se 0.95 Te 0.05 .

研究领域: 材料科学 · 物理学
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Advanced Electronic Materials · 2024 ·Vol. 10 ·期 6 ·2300809 · IF 5.3

Enhanced Thermoelectric Performance of MnTe by Decoupling of Electrical and Thermal Transports

Abdul Basit,Jiwu Xin,Yubo Luo,Ji-Yan Y. Dai,Junyou Yang

Lead-free polycrystalline manganese telluride holds great potential in the development of waste heat recovery due to its fascinating physical properties. However, the poor thermoelectric (TE) performance in the p-type MnTe alloys always results from their inferior carrier concentration, leading to low power factor and high thermal conductivity which restrict the overall thermoelectric performance. In this work, the problem is solved by decoupling its electrical and thermal transports through the hole donor Ge-deficiency in MnTe + x mol.% GeTe (0 ≤ x ≤ 4) compounds. Intrinsically, extra GeTe in MnTe + x mol.% GeTe compound offers free charge carriers due to a narrow bandgap comparatively, realizing not only a full assessment of stimulated electrical performance but also an enhanced power factor. Moreover, benefiting from the nano-precipitates and tweed microstructures, the lattice thermal conductivity effectively reduces due to the intensive phonon scattering accordingly. Ultimately, a maximum ZT of ≈1.2 at 873 K in the 3 mol.% GeTe doped MnTe sample is realized.

研究领域: 材料科学 · 能源工程
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