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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 31 ·2400911 · IF 27.4

Realization of Fine-Tuning the Lattice Thermal Conductivity and Anharmonicity in Layered Semiconductors via Entropy Engineering

Hongxiang Chen,Jiantao Fu,Shuxian Huang,Yiding Qiu,Enhui Zhao,Shiyu Li,Jianeng Huang,Pinqiang Dai,Hengzhong Fan,Bing Xiao

Entropy engineering is widely proven to be effective in achieving ultra-low thermal conductivity for well-performed thermoelectric and heat management applications. However, no strong correlation between entropy and lattice thermal conductivity is found until now, and the fine-tuning of thermal conductivity continuously via entropy-engineering in a wide entropy range is still lacking. Here, a series of high-entropy layered semiconductors, Ni 1− x (Fe 0.25 Co 0.25 Mn 0.25 Zn 0.25 ) x PS 3 , where 0 ≤ x < 1, with low mass/size disorder is designed. High-purity samples with mixing configuration entropy of metal atomic site in a wide range of 0–1.61 R are achieved. Umklapp phonon-phonon scattering is found to be the dominating phonon scattering mechanism, as revealed by the linear T −1 dependence of thermal conductivity. Meanwhile, fine tuning of the lattice thermal conductivity via continuous entropy engineering at metal atomic sites is achieved, in an almost linear dependence in middle-/high- entropy range. Moreover, the slope of the κ - T −1 curve reduces with the increase in entropy, and a linear response of the reduced Grüneisen parameter is revealed. This work provides an entropy engineering strategy by choosing multiple metal elements with low mass/size disorder to achieve the fine tuning of the lattice thermal conductivity and the anharmonic effect.

研究领域: 材料科学 · 热电学 · 固体物理 · 声子工程
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2023 · IF 10.9

Constructing cell-membrane-mimic grain boundaries for high-performance n-type Ag2Se using high-dielectric-constant TiO2

Yi-Yan Liao,Qiang Sun,Xu-Ping Jiang,Hao Wu,Bang-Zhou Tian,Ze-Gao Wang,Kun Zheng,Lei Yang

The coupling of charge carrier and phonon transport limits the application of Ag 2 Se as a low-toxic near-room-temperature thermoelectric material. Strategies that reduce the thermal conductivity via enhancing the phonon scattering usually lead to reduced carrier mobility due to high grain boundary potential barrier. In this study, we developed a cell-membrane-mimic grain boundary engineering strategy for decoupling the charge carrier and phonon scattering through decorating high-dielectric-constant rutile TiO 2 at Ag 2 Se grain boundaries to enable the charge carrier/phonon selective permeability. The nano-sized TiO 2 with high dielectric permittivity can secure the charge carrier transport by shielding the interfacial Coulomb potential to lower the energy barrier of grain boundaries, rendering an enhanced power factor. Additionally, benefited from the enhanced phonon scattering by TiO 2 nanoparticles, a significantly decreased lattice thermal conductivity of ∼0.20 W m −1 K −1 and a high zT of ∼0.97 at 390 K are obtained in the Ag 2 Se-based nanocomposites. This work demonstrates that such cell-membrane-mimic grain boundary engineering strategy may shed light on developing high-performance thermoelectric materials.

研究领域: 材料科学 · 物理学
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Materials Today Physics · 2023 · IF 11.5

Defect-dominated phonon scattering processes and thermal transports of ferroelastic (Sm1-XYbX)TaO4 solid solutions

Lin Chen,Mingyu Hu,Jing Feng

Thermal transport management is of great significance for materials such as thermal barrier coatings , photovoltaics , and thermoelectrics . In particular, tremendous efforts have been made to tailor phonon thermal transport to improve performance. This work elucidated origins of low thermal conductivity of ferroelastic (Sm 1-X Yb X )TaO 4 solid solutions from defect-dominated phonon scattering processes. We estimated the influences of point defects (misfits in atomic weight and ionic radius , and oxygen vacancies), ferroelastic domains, and the Umklapp process on thermal transports via the corresponding phonon relaxation time ( τ ). The phonon relaxation time caused by point defects ( τ D ), ferroelastic domains ( τ F ), and the Umklapp process ( τ U ) exhibited a trend of τ D − 1 > τ U − 1 > τ F − 1 τD−1>τU−1>τF−1 , indicating that point defects dominated the thermal transports. The effects of ferroelastic domains on thermal conductivity were estimated according to domain widths and space mismatches between neighboring domains. The approximately parallel relationship between the neighboring domains was beneficial for reducing ferroelastic t - m transition energy. Furthermore, a model was developed to derive the high-temperature thermal conductivity, and the contributions of radiative thermal conductivity were separated from the total thermal conductivity. The analysis of thermal transports can be used in other materials to estimate the contributions of different thermal transport mechanisms to the total thermal conductivity at both low and high temperatures, and to effectively tailor thermal transports according to specific applications.

研究领域: 材料科学 · 物理学
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Nanoscale · 2024 ·Vol. 16 ·期 45 ·21031-21038 · IF 5.8

Decoupled electron–phonon transport in Ag2Se thermoelectric materials through constructing TiO2/MoS2 co-decorated cell-membrane-mimic grain boundaries

Hanwen Hu,Yiyan Liao,Shanshan Tan,Chen Li,Jun Tang,Kun Zheng,Lei Yang

Ag2Se has emerged as a promising n-type thermoelectric material; however, its application is limited mainly due to the strongly coupled charge carrier and phonon transport. Enhancing phonon scattering by constructing interfacial complexes often results in low carrier mobility due to its strong carrier scattering resulting from the high energy barrier at the multiphase interface. Inspired by the cell membrane with selective permeability, we construct bio-mimic grain boundaries with TiO2 and MoS2 co-decoration in Ag2Se to decouple electron scattering from strong phonon scattering. The nanostructured TiO2 with a high dielectric constant screens the interfacial Coulomb potential, ensuring efficient carrier transport and reducing the grain boundary barriers, while the few-layer MoS2 provides significant phonon scattering to further reduce the thermal conductivity. This method effectively enhances the zT value of Ag2Se by as much as 60% and also can significantly enhance the theoretical output performance of the thermoelectric device, which highlights the effectiveness of the bio-mimic grain boundary engineering strategy.

研究领域: 材料科学 · 物理学
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JOURNAL OF ELECTRONIC MATERIALS · 2022 ·Vol. 51 ·期 2 ·486-494 · IF 2.047

Achieving High Thermoelectric Performance of SnTe Composites with 2D WSe2

Wang Xiaochun,Zhou Zhiwei,Lin Xuesong

In this work, we introduced two-dimensional (2D) WSe 2 with the lowest heat conductivity to enhance thermoelectric properties of the non-toxic and cost-effective SnTe. On one hand, the improved power factor can be attributed to the enhancement of Seebeck coefficient due to the decrease of low-energy carriers and minority carriers by the addition of WSe 2 -SnTe p - p -type heterojunction interface barriers. On the other hand, the thermal conductivity also decreased sharply by the heightened phonon scattering from the high-density stacking faults and multiscale hierarchical architectures. Ultimately, benefiting from the dual regulation effect of the introduction of 2D WSe 2 on the electro-acoustic decoupling, an improved figure of merit ( ZT ) of 1.0 is achieved for the composition of SnTe + 6 wt% WSe 2 at 873 K, which is enhanced by 134% in comparison with the pure SnTe sample. Moreover, the meaningful attempt represents an effective and feasible strategy for mixing SnTe with other compounds by the method of ball milling. Graphical Abstract

研究领域: 材料科学 · 热电学
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APPLIED PHYSICS LETTERS · 2024 ·Vol. 124 ·期 24 · IF 3.5

Strain effect on thermal conductivity of 3C-SiC nanowire

Chen Wenkang,Wu Xiangshui,Deng Shichen,Yang Nuo,Xu Xiangfan

Strain provides an additional mechanism in tuning the thermal/electrical properties of nanostructures and therefore has triggered lots of interest in recent years. However, experimental research about the strain effect on the thermal conductivity of nanowires is still limited, especially in the low-temperature range, which is important in understanding the physics of strain-induced regulation in thermal conductivity. Here, we present thermal transport measurements of bent silicon carbide nanowires at temperatures ranging from 20 to 300 K. Reduction in thermal conductivity compared to their straight counterparts is observed. More specifically, the relative change is up to 55% at 20 K and descends with temperature, which is due to the inhomogeneous strain-induced phonon scattering. This study will deepen the understanding of thermal properties in nanostructures with strain.

CAS / MDL:
研究领域: 材料科学 · 热物理
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CERAMICS INTERNATIONAL · 2025 · IF 5.6

Defect engineering and enhancement of interfacial phonon scattering effects in La-doped SrTiO3 synthesized at high pressure and high temperature

Shan Gao,Haidong Yu,Yuewen Zhang,Hongan Ma,Xiaopeng Jia

Thermoelectrics (TE) have received a lot of attention for their ability to directly convert heat into electricity. This capability provides a promising solution for waste heat recovery and clean energy utilization. Strontium titanate (SrTiO 3 ) is a promising N-type oxide TE material. However, its practical application is limited by low electrical conductivity and high thermal conductivity. Here, we present a high-pressure synthesis technique aimed at simultaneously introducing defects as well as enhancing phonon scattering. Enhancing the thermoelectric properties of strontium titanate thermoelectric materials. SrTiO 3 samples doped with different concentrations of La were synthesized by high-pressure high-temperature (HPHT) synthesis, which effectively promotes the solid-phase reaction and thus allows for a more homogeneous and efficient doping of La atoms into the SrTiO 3 lattice as compared to the conventional synthesis method. The introduction of La 3+ creates a charge imbalance, which is compensated by the formation of oxygen vacancies. These oxygen vacancies act as donor defects, which in turn increase the carrier concentration and significantly improve the electrical conductivity of the samples. At the same time, the HPHT synthesis conditions induced severe lattice distortions, leading to grain refinement and the formation of dislocation networks and nanopores. By modulating the density and distribution of multiscale defects, La doping significantly improves the interfacial phonon scattering efficiency. This condition reduces the thermal conductivity and improves the thermoelectric properties. By combining defect engineering and interfacial phonon scattering, we achieved the decoupling of electrical and thermal transport properties in La-doped SrTiO 3 . Consequently, the thermoelectric figure of merit ( zT ) was significantly enhanced, reaching 0.18 at 973 K. This study introduces a new methodology and theoretical foundation for the development of high-performance oxide TE materials.

CAS / MDL: 1312-81-8 1314-11-0
研究领域: 材料科学 · 热电材料
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MODERN PHYSICS LETTERS B · 2019 · IF 0.929

Influence of multi-sintering on the thermoelectric properties of Bi2Sr2Co2Oy ceramics

Y. Zhang,M. M. Fan,C. C. Ruan,Y. W. Zhang,X.-J. Li,H. Z. Song

Bi 2 Sr 2 Co 2 O y Bi2Sr2Co2Oy ceramic samples have a structure similar to phonon glass electronic crystals, and their thermoelectric properties can be effectively adjusted through repeated grinding and sintering. The results show that multi-sintering can make their grain refined and increase their grain boundary, which will effectively increase density and phonon scattering. Finally, multi-sintering can reduce the resistivity and thermal conductivity, thus obviously improve thermoelectric figure of merit ( Z T ) (ZT) of Bi 2 Sr 2 Co 2 O y Bi2Sr2Co2Oy . The optimum Z T ZT value of 0.26 is achieved at 923 K by the third sintered sample.

研究领域: 材料科学 · 热电材料 · 无机非金属材料 · 凝聚态物理
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2024 · IF 5.8

The ultra-low glasslike thermal conductivities of Y3+- and Ce4+- codoped lanthanum zirconate pyrochlores for potential thermal barrier coating applications

Yanfei Wang,Weiran Zhang,Jinping Du,Duan Li,Rongjun Liu

It is urgent to develop thermal barrier coating (TBC) topcoat materials with ultra-low thermal conductivities for next-generation gas turbine engines. A novel pyrochlore-based single-phased ceramic, tuned by codoping of lanthanum zirconate, (La 1-x Y x ) 2 (Zr 1-y Ce y ) 2 O 7 , has been synthesized from the solid state reaction method. The thermal conductivity of (La 1-x Y x ) 2 (Zr 1-y Ce y ) 2 O 7 not only exhibits a temperature-independent trend but also reaches as low as 0.93 W·m −1 ·K −1 , a value that is lowest of fully dense crystalline solids in open literature, attributing to the following two combined effects. The first is the strong scattering of phonons by small-sized Y 3+ cations occupying the oversized atomic cages formed by the distinctive pyrochlore structure. The second is the lattice softening effects arising from larger-sized Ce 4+ substituting Zr 4+ cations. The above two effects act in concert and thus form a glasslike and ultra-low thermal conductivity of (La 1-x Y x ) 2 (Zr 1-y Ce y ) 2 O 7 solid solutions, which is ideal for next-generation TBC topcoat applications.

研究领域: 材料科学 · 工程热物理
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JOURNAL OF ELECTRONIC MATERIALS · 2016 ·Vol. 46 ·期 5 ·2697-2704 · IF 1.491

Fabrication of Cu-Doped Bi2Te3 Nanoplates and Their Thermoelectric Properties

Liu Shuai,Peng Nan,Bai Yu,Ma Dayan,Ma Fei,Xu Kewei

Cu-doped Bi 2 Te 3 hexagonal nanoplates were fabricated by a simple solvothermal method. Scanning electron microscopy and transmission electron microscopy characterization illustrated that the nanoplates are single-crystal ones with an average width of 300 nm and thickness in the range of 20–30 nm. It was demonstrated that Cu x Bi 2 Te 3 nanoplates possess the lowest thermal conductivity (0.8–1.2 W/m K) at 300 K, which is mainly due to the enhanced phonon scattering by grain boundaries. Furthermore, the doped Cu could evidently enhance the power factor of Bi 2 Te 3 through optimizing the carrier transport properties. As a result, Cu 0.02 Bi 2 Te 3 nanoplates exhibit the best thermoelectric performance with a figure of merit of 0.33, which is more than two times higher than that of Bi 2 Te 3 nanoplates.

研究领域: 材料科学 · 热电材料研究
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY · 2017 ·Vol. 100 ·期 12 ·5723-5730 · IF 2.841

Thermoelectric performance of SnTe with ZnO carrier compensation, energy filtering, and multiscale phonon scattering

Zhiwei Zhou,Junyou Yang,Qinghui Jiang,Dan Zhang,Jiwu Xin,Xin Li,Yangyang Ren,Xu He

In this work, the thermoelectric properties of SnTe have been regulated synergistically by introduction of n -type ZnO nanoinclusions. On one hand, the excessive holes in SnTe matrix were compensated properly by n -type ZnO, and the Seebeck coefficient has been improved greatly due to the carrier energy filtering effect by a large quantity of ZnO-SnTe hetero-junction interface barriers; On the other hand, the thermal conductivity gets reduced by the enhanced phonon scattering from multiscale hierarchical architectures. Consequently, a maximum ZT of ~0.9 at 873K has been obtained in the 0.8 wt% sample, which enhances by 112% in comparison with the nanoinclusion-free sample.

研究领域: 材料科学 · 热电学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2017 · IF 3.133

Enhanced thermoelectric performance of heavy-fermion YbAl3 via multi-scale microstructures

Danqi He,Wenyu Zhao,Xin Mu,Hongyu Zhou,Ping Wei,Wanting Zhu,Xiaolei Nie,Xianli Su,Huijun Liu,Jiaqing He,Qingjie Zhang

How to optimize the thermoelectric performance of heavy-fermion systems remains a key challenge due to the extremely high thermal conductivity rooted in the extraordinarily high electrical conductivity . Here we report a new approach to simultaneously optimize the electron and phonon transport properties of heavy-fermion YbAl 3 by fabricating the multi-scale microstructures spanning from the atomic to nanometer to mesoscopic scales. We discover theoretically and experimentally that in YbAl 3 the nanostructures with less than 30 nm in size and atomic-scale dislocations and Yb vacancies can simultaneously scatter electron and phonon and thus significantly decrease the electrical conductivity and electronic thermal conductivity, while other hierarchical microstructures from the nanometer to mesoscopic scales can effectively scatter phonons and remarkably decrease the lattice thermal conductivity. The highest thermoelectric figure of merit ZT reaches 0.4 at 300 K and increased by 74%, which is a new record for un-doped YbAl 3 . Our work demonstrates that the electron and phonon transport properties of heavy-fermion system can be simultaneously enhanced by the multi-scale microstructures.

CAS / MDL: 7429-90-5 7440-64-4
研究领域: 材料科学 · 凝聚态物理
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