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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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JOURNAL OF ALLOYS AND COMPOUNDS · 2015 · IF 2.999

Microwave synthesis and sintering of TiNiSn thermoelectric bulk

Ying Lei,Yu Li,Lin Xu,Junyou Yang,Rundong Wan,Hongming Long

Nano-structured Half-Heusler TiNiSn thermoelectric bulk was prepared by microwave-assisted rapid solid-state synthesis and sintering. The mixture of powders of Ti, Ni, Sn was cold pressed before being heated by microwave irradiation. A microwave susceptor material rapidly heats the elemental starting materials inside an evacuated quartz tube resulting in near single phase compounds in 4 min 20 s. The synthesized sample was milled for 30 min in an agate mortar and cold pressed for the following sintering. An 86% density of TiNiSn thermoelectric bulk contains ∼100 nm pore and nanocrystal was sintered in 20 min. For TiNiSn bulk, low thermal conductivity of 2–3 W/m·K at temperatures in the range of the room temperature to 773 K. The ZT values of around 0.3 are found, with the microwave-prepared sample displaying noticeable superior properties over conventionally prepared half-Heuslers due to inclusion of nanopore and In-situ nanocrystal.

研究领域: 材料科学 · 无机非金属材料 · 功能材料 · 固态化学 · 纳米材料
✓ 已验证 DOI 高影响因子
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MATERIALS CHEMISTRY AND PHYSICS · 2016 · IF 2.101

Ultrafast one-step combustion synthesis and thermoelectric properties of In-doped Cu2SnSe3

Yuyang Li,Guanghua Liu,Jiangtao Li,Kexin Chen,Gang He,Zengchao Yang,Yemao Han,Min Zhou,Laifeng Li

Bulk In-doped Cu 2 SnSe 3 samples were prepared by a fast and one-step method of high-gravity combustion synthesis . All the synthesized samples were dense with relative densities of >98%. The influence of Indium-doping on the phase composition of the samples was investigated. SEM and EDS measurements confirm the existence of SnSe and Cu 2 Se as secondary phase in the Cu 2 Sn 1−x In x Se 3 samples. In addition, the experimental results show that there is a solubility limit of indium in the Cu 2 SnSe 3 matrix. The thermoelectric properties of the samples were measured in a temperature range from 323 K to 773 K, and the Cu 2 Sn 0.8 In 0.2 Se 3 sample achieved a maximum ZT of 0.65 at 773 K, which was comparable with the best-reported result for Cu 2 SnSe 3 materials prepared by conventional sintering approaches. With much reduced time and energy consumption, high-gravity combustion synthesis may offer a more efficient and economical way for producing thermoelectric materials .

研究领域: 材料科学 · 无机非金属材料 · 热电转换 · 固态化学 · 功能材料
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2023 ·Vol. 11 ·期 43 ·23319-23329 · IF 11.9

Interfacial modulation to achieve low lattice thermal conductivity and enhanced thermoelectric performance in n-type Mg3(Sb, Bi)2-based materials via graphene and MXene

Bang-Zhou Tian,Yi-Yan Liao,Fang Xu,Xiao-Ling Qiu,Fu-Jie Zhang,Ran Ang

Interfacial modulation has been considered an effective strategy to enhance the thermoelectric (TE) performance by decoupling thermal and electrical parameters. However, inappropriate interfacial heterojunctions can significantly deteriorate electrical transport while enhancing phonon scattering, which causes no substantial improvement in TE performance. Herein, we introduce two-dimensional graphene or MXene into the Mg3.2Sb0.5Bi1.49Te0.01 matrix by ball mixing combined with rapid sintering to modify the composition and structure at the interface. The differences in morphology, size and distribution of interfacial graphene and MXene lead to distinct results which show that incorporated graphene flakes with larger size hinder the carrier transport, while the homogeneously dispersed tiny MXene provides improved carrier channels and boosts the mobility. On the other hand, such uniformly diffused heterogeneous MXene structures create stronger scattering on phonons compared to enriched graphene phases, resulting in a low lattice thermal conductivity of ∼0.66 W m−1 K−1 and enhanced zT of ∼1.0 at 513 K in Mg3.2Sb0.5Bi1.49Te0.01-0.6 wt% MXene with good component stability in air. This work highlights the importance of size, concentration, and distribution in the interfacial modulation strategy, demonstrating an effective method for developing high TE performance Mg3(Sb, Bi)2-based near-room-temperature materials.

研究领域: 材料科学 · 凝聚态物理 · 纳米材料 · 能源材料 · 固体化学
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CERAMICS INTERNATIONAL · 2022 ·Vol. 48 ·期 22 ·33967-33975 · IF 5.532

Enhanced thermoelectric properties of Ca3Co4O9 by adding nano MoSi2

Ya-nan Li,Ping Wu,Shiping Zhang,Yili Pei,Jinguang Yang,Sen Chen,Li Wang

Adding nanoparticles is a method to regulate the performance of thermoelectric materials. Ca 3 Co 4 O 9 /x MoSi 2 (x = 0, 0.05, 0.10, 0.13, and 0.16) was synthesized by a wet chemical method combined with atmospheric pressure sintering. The XRD and SEM results reveal that there are no other reaction in the samples. The grain size of all samples decrease with increasing MoSi 2 content, and all presented a similar flake morphology. The influence of MoSi 2 on the thermoelectric performance of Ca 3 Co 4 O 9 is systematically analysed. The appropriate addition of nano-MoSi 2 particles can increase the carrier concentration and enhance conductivity of Ca 3 Co 4 O 9 . The electrical conductivity of Ca 3 Co 4 O 9 /0.05 MoSi 2 is 83.16 Scm −1 , which is 49.2% higher than that of Ca 3 Co 4 O 9 at 1080 K. The Seebeck coefficient of the Ca 3 Co 4 O 9 /0.16 MoSi 2 sample reaches 197.56 μVK −1 at 980 K, which is significantly better than that of previously reported samples prepared by the same method. Moreover, combined with the experimental results and the analysis of the effective medium theory model, the addition of MoSi 2 can effectively debase the thermal conductivity of Ca 3 Co 4 O 9 . The thermal conductivity of Ca 3 Co 4 O 9 /0.16 MoSi 2 (∼1.26 Wm −1 K −1 , 1080 K) samples decrease greatly, which is attributed to the influence of interfacial thermal resistance and pores in the Ca 3 Co 4 O 9 /MoSi 2 . The ZT value of the Ca 3 Co 4 O 9 /0.05 MoSi 2 sample increases by 44.4% compare with that of Ca 3 Co 4 O 9 and reaches 0.26 at 1080 K. These results demonstrate that adding an appropriate amount of MoSi 2 particles is one of the methods to enhance the thermoelectric performance of Ca 3 Co 4 O 9 ceramic samples.

研究领域: 材料科学 · 凝聚态物理 · 无机非金属材料 · 能源材料 · 热电转换
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2019 · IF 4.175

Synergistically optimizing charge and phonon transport properties in n-type PbTe via introducing ternary compound AgSb(Se, Te)2

Siqi Wang,Zhi Yang,Yuejun Sun,Yu Xiao,Li-Dong Zhao

PbTe-based thermoelectric materials are considered to be a medium-temperature thermoelectric candidates and the high-performance n -type PbTe is urgently to be developed to match its p -type counterpart on account of practical application. Herein, we firstly optimized the carrier density of n -type PbTe through Sb doping, and obtained a maximum ZT value of ∼1.0. Then, based on the optimized carrier density, we introduced ternary compounds AgSb(Se, Te) 2 to suppress the lattice thermal conductivity . Minimum lattice thermal conductivity of n -type PbTe was reduced as low as ∼0.53 W m −1 K −1 and ∼0.62 Wm −1 K −1 through introducing AgSbSe 2 and AgSbTe 2 , respectively. Combining the maintained electrical properties with suppressed thermal conductivity , maximum ZT values ∼1.2 and ∼1.3 were obtained in PbTe+2%AgSbSe 2 and PbTe+2%AgSbTe 2 , respectively. This work provides an effective strategy of synergistically balancing charge and phonon transports in n -type PbTe with ternary AgSb(Se, Te) 2 compounds.

研究领域: 材料科学 · 热电转换 · 凝聚态物理 · 半导体物理 · 功能材料 · 能量转换材料
✓ 已验证 DOI 高影响因子
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SOLID STATE SCIENCES · 2024 · IF 3.4

Enhancement of thermoelectric properties in Sr0.6La0.4Nb2O6-δ-based ceramics by addition of graphite

Kaiwu Fu,Dandan Ma,Nan Zhang,Jiacheng Cao,Xiaonan Chen,Min Zhu,Peiqing La

Oxide thermoelectric materials have a wide range of applications due to their excellent stability, low cost, and non-toxic properties. However, their low thermoelectric conversion efficiency limits their practical use. Therefore, improving the performance of oxide thermoelectric materials has become the focus of current research. Interface engineering is an important approach to enhance thermoelectric properties by optimizing electrical transport properties through multiphase composite regulation of phase interface structure. A series of Sr 0.6 La 0.4 Nb 2 O 6-δ /x wt% graphite (x = 0, 0.6, 1.0, 1.5, 2.0) composite ceramics thermoelectric materials were prepared, and the mechanism for improving their thermoelectric properties was explored. Graphite serves as an electron momentum amplifier within the Sr 0.6 Ba 0.4 Nb 2 O 6-δ matrix, thereby augmenting both conductivity and power factor values significantly. Notably, the incorporation of 1.5 wt% graphite led to a remarkable enhancement in the thermoelectric power factor at 1073 K, reaching an impressive value of 254.84 μW/K 2 m - representing a notable increase of approximately 51 % compared to the unmodified sample - primarily attributed to the elevated electrical conductivity .

研究领域: 材料科学 · 无机非金属材料 · 热电转换 · 固态物理 · 功能陶瓷
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CERAMICS INTERNATIONAL · 2024 ·Vol. 51 ·期 8 ·10774-10782 · IF 5.1

Optimization of interface properties in BiCuSeO-based thermoelectric devices via hot pressing process

Jitao Yi,Xinyue Zhang,Shanliang Chen,Ting Sun,Qinghui Jiang,Yong Liu

BiCuSeO-based materials show great promise for thermoelectric generators in waste heat recovery due to their excellent thermoelectric properties. However, the limited focus on device development has hindered their industrial-scale implementation. Here, high-performance BiCuSeO-based compounds with exceptional thermal stability were synthesized and remained stable aging for 400 h, making them suitable for investigation in the device bonding process. The BiCu80AgP is identified as the optimal solder from eight candidates, effectively connecting the copper (Cu) electrode with BiCuSeO-based compounds. The optimized bonding process substantially resulted in an impressive interfacial shear strength of about 15 MPa and reduced interfacial resistance to 2.2 mΩ cm 2 . Interface analysis revealed the formation of diverse, complex compounds, with variations in their concentrations greatly affecting joint performance. Achieving a uniform distribution of these compounds effectively mitigated thermal expansion mismatches and extended joint longevity by a factor of 6.6. This research proposes a novel fabrication method for BiCuSeO-based thermoelectric devices utilizing BCu80AgP solder, providing a foundation for future advancements in this field.

研究领域: 材料科学 · 热电转换 · 固态物理 · 能源材料 · 界面工程
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 15 ·8893-8899 · IF 10.7

Plastic Mg3(Sb,Bi)2-based thermoelectric compounds with enhanced texture via cold-deformation

Ziming Zhang,Zhiqiang Gao,Tingting Deng,Qingfeng Song,Lidong Chen,Shengqiang Bai

Mg3(Sb,Bi)2-based Zintl compounds have attracted lots of attention due to their high thermoelectric performance and good mechanical properties. However, thermally activated mobility, which is ascribed to the grain boundary scattering, greatly limits their practical use. In this work, we reveal the plasticity of Mg3(Sb,Bi)2-based compounds in the compressive strength test. The ab initio analysis indicates that this plasticity should be ascribed to the low slip barrier energy (∼580 mJ m−2), which is only one third of the cleavage energy (∼1600 mJ m−2). Based on this finding, we propose a cold-deformation procedure to elongate particles and to enhance texture, which successfully suppresses the grain boundary scattering. As a result, a high carrier mobility of 86.6 cm2 V−1 s−1 and a high power factor of 16.2 μW cm−1 K−2 in Mg3.1Bi1.5Sb0.49Te0.01 are obtained at room temperature. The plastic deformation capacity of Mg3(Sb,Bi)2 compounds provides a near-net-forming method to fabricate special-shaped devices at room-temperature, which will extend the application fields of thermoelectric techniques.

研究领域: 材料科学 · 凝聚态物理 · 无机非金属材料 · 热电转换 · 固态物理化学
✓ 已验证 DOI 高影响因子
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Materials Today Physics · 2023 · IF 11.5

Decoupled electron and phonon transport in thermoelectric GeTe compounded with multi-walled carbon nanotubes

Ruifan Si,Zhongwei Zhang,Chengyan Liu,Ying Peng,Xiaobo Bai,Baoquan Feng,Junliang Chen,Jie Gao,Lei Miao

With developing of thermoelectric (TE) performance, GeTe-based TE materials present great promising application at medium temperatures as a replacement for toxic PbTe. However, the further improvement of TE properties is severely constrained by the coupling of electron and phonon transport. In this study, we achieve decoupled electron and phonon transport by effectively creating a special phase boundary to scatter phonon but transmit electron by implanting multi-walled carbon nanotubes (MWCNTs) into Bi-doped GeTe. With the help of this decoupling mechanism, the power factor is effectively improved and reaches up to ∼4482 μW −1  m −1  K −2 at 673 K while the thermal conductivity shows an obvious drop to ∼1.27 W m −1  K −1 at 723 K, leading to an impressive increase in zT to a maximum value of ∼2.3 at 723 K. In particular, a competitive average zT value of ∼1.43 in the temperature range of 323–773 K is obtained, which is at a high level in lead-free GeTe-based materials. Our method could be used as a guidance for the decoupling of electron and phonon transport in other TE materials .

研究领域: 材料科学 · 凝聚态物理 · 能源材料 · 热电转换 · 纳米复合材料
✓ 已验证 DOI 高影响因子
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Advanced Electronic Materials · 2021 ·Vol. 8 ·期 4 ·2101125 · IF 7.295

In-Situ Loading Bridgman Growth of Mg3Bi1.49Sb0.5Te0.01 Bulk Crystals for Thermoelectric Applications

Qi-Qi Wang,Fan Li,Sheng-Qing Xia,Jian Liu,Xiao-Cun Liu,Ling Chen,Cheng-Qian Zhang

The single crystal growth of Mg 3 Bi 2 -based thermoelectric materials is of great significance for their applications near room temperature. So far, it is still a big challenge to grow such bulk single crystals and attempts are primarily focused on the metal flux methods. For the first time, bulk single crystals of n-type Mg 3 Bi 1.49 Sb 0.5 Te 0.01 are directly grown by applying an In-situ Loading Bridgman method. The as-grown single crystal features an excellent carrier mobility of 220 cm 2 V −1 s −1 , which is among the best compared to other Mg 3 Bi 2 -based bulk materials. Besides, this method is successfully developed to fast grow uniform polycrystalline materials with high thermoelectric and mechanic performance. As demonstrated by the single-leg device, a large temperature difference of 10.5 K is achieved at the supplied electric current of 0.6 A, much superior to other room temperature state-of-the-art thermoelectric materials. With the single crystalline and polycrystalline materials prepared reliably and conveniently, in-depth investigations on the Mg 3 Bi 2 thermoelectric system can be greatly benefited, which should as well significantly facilitate their practical applications at room temperature.

研究领域: 材料科学 · 热电学 · 凝聚态物理 · 晶体生长 · 功能材料 · 能源材料
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SCRIPTA MATERIALIA · 2019 · IF 4.539

Ni metal coating boosting the thermoelectric performance of In2O3(ZnO)5 ceramics

Jun Guo,Peng Qin,Zheng Ma,Qiong-Lian Yang,Jing Feng,Zhen-Hua Ge

A new approach was developed for enhancing the thermoelectric performance of In 2 O 3 (ZnO) 5 ceramics. Ni coating layer on the surface of In 2 O 3 (ZnO) 5 powders was prepared by chemical plating. The Ni-Coated In 2 O 3 (ZnO) 5 powders was densified to composite bulk with Ni enrichment in the grain boundaries. The composite sample obtained a remarkably enhanced dimensionless thermoelectric figure of merit (ZT) of 0.39 at 973   K, which is 3.6 times higher than that of a pristine In 2 O 3 (ZnO) 5 sample.

研究领域: 材料科学 · 凝聚态物理 · 功能陶瓷 · 热电材料 · 纳米复合材料
✓ 已验证 DOI 高影响因子
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