{"title":"妥协构型熵使锡碲基材料具有非凡的热电特性","authors":"Raza Moshwan, Min Zhang, Meng Li, Siqi Liu, Nanhai Li, Tianyi Cao, Wei-Di Liu, Xiao-Lei Shi, Zhi-Gang Chen","doi":"10.1002/adfm.202418291","DOIUrl":null,"url":null,"abstract":"Incorporating multiple atoms with different masses and radii at distinct atomic sites within a lattice matrix can increase its entropy and, in turn, enable a synergistic approach to both band structure and microstructure engineering. Modifying the band structure enhances electrical transport properties, while changes in the microstructure effectively suppress thermal transport properties, leading to significantly improved thermoelectric performance. Here, entropy engineering is employed to enhance the thermoelectric performance of the SnTe material system. The synergistic alloying of Ge, Mn, and In significantly alters the electronic band structure by merging four valence bands namely L, Σ, Λ, and X, and creating a resonant energy state near the Fermi level, resulting in an outstanding Seebeck coefficient of ≈97 µV K<sup>−1</sup> at room temperature. The high density of point defects, Ge secondary phases, amorphous interfaces, phono–phonon interactions, and grain boundaries significantly disrupts the movement of heat-carrying phonons, leading to an exceptionally low lattice thermal conductivity of 0.32 W m<sup>−1</sup> K<sup>−1</sup>, pushing it below the amorphous limit. Consequently, a peak figure of merit of 1.64 achieves at 873 K in Sn<sub>0.71</sub>Ge<sub>0.2</sub>Mn<sub>0.07</sub>In<sub>0.02</sub>Te. These findings lay the groundwork for developing advanced thermoelectric materials via entropy engineering.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":18.5000,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Compromising Configurational Entropy Leading to Exceptional Thermoelectric Properties in SnTe-Based Materials\",\"authors\":\"Raza Moshwan, Min Zhang, Meng Li, Siqi Liu, Nanhai Li, Tianyi Cao, Wei-Di Liu, Xiao-Lei Shi, Zhi-Gang Chen\",\"doi\":\"10.1002/adfm.202418291\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Incorporating multiple atoms with different masses and radii at distinct atomic sites within a lattice matrix can increase its entropy and, in turn, enable a synergistic approach to both band structure and microstructure engineering. Modifying the band structure enhances electrical transport properties, while changes in the microstructure effectively suppress thermal transport properties, leading to significantly improved thermoelectric performance. Here, entropy engineering is employed to enhance the thermoelectric performance of the SnTe material system. The synergistic alloying of Ge, Mn, and In significantly alters the electronic band structure by merging four valence bands namely L, Σ, Λ, and X, and creating a resonant energy state near the Fermi level, resulting in an outstanding Seebeck coefficient of ≈97 µV K<sup>−1</sup> at room temperature. The high density of point defects, Ge secondary phases, amorphous interfaces, phono–phonon interactions, and grain boundaries significantly disrupts the movement of heat-carrying phonons, leading to an exceptionally low lattice thermal conductivity of 0.32 W m<sup>−1</sup> K<sup>−1</sup>, pushing it below the amorphous limit. Consequently, a peak figure of merit of 1.64 achieves at 873 K in Sn<sub>0.71</sub>Ge<sub>0.2</sub>Mn<sub>0.07</sub>In<sub>0.02</sub>Te. These findings lay the groundwork for developing advanced thermoelectric materials via entropy engineering.\",\"PeriodicalId\":112,\"journal\":{\"name\":\"Advanced Functional Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":18.5000,\"publicationDate\":\"2024-10-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Functional Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/adfm.202418291\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adfm.202418291","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
在晶格矩阵的不同原子位点上加入多个具有不同质量和半径的原子,可以增加其熵,进而实现带状结构和微结构工程的协同方法。改变能带结构可增强电传输特性,而改变微结构则可有效抑制热传输特性,从而显著提高热电性能。在这里,熵工程被用来提高 SnTe 材料体系的热电性能。Ge、Mn 和 In 的协同合金化显著改变了电子能带结构,合并了四个价带(即 L、Σ、Λ 和 X),并在费米级附近形成了一个共振能态,从而使室温下的塞贝克系数达到 ≈97 µV K-1。高密度的点缺陷、Ge 次生相、非晶界面、声子相互作用和晶界极大地扰乱了载热声子的运动,导致 0.32 W m-1 K-1 的超低晶格热导率,使其低于非晶极限。因此,在 873 K 时,Sn0.71Ge0.2Mn0.07In0.02Te 的峰值功勋值达到了 1.64。这些发现为通过熵工程开发先进的热电材料奠定了基础。
Compromising Configurational Entropy Leading to Exceptional Thermoelectric Properties in SnTe-Based Materials
Incorporating multiple atoms with different masses and radii at distinct atomic sites within a lattice matrix can increase its entropy and, in turn, enable a synergistic approach to both band structure and microstructure engineering. Modifying the band structure enhances electrical transport properties, while changes in the microstructure effectively suppress thermal transport properties, leading to significantly improved thermoelectric performance. Here, entropy engineering is employed to enhance the thermoelectric performance of the SnTe material system. The synergistic alloying of Ge, Mn, and In significantly alters the electronic band structure by merging four valence bands namely L, Σ, Λ, and X, and creating a resonant energy state near the Fermi level, resulting in an outstanding Seebeck coefficient of ≈97 µV K−1 at room temperature. The high density of point defects, Ge secondary phases, amorphous interfaces, phono–phonon interactions, and grain boundaries significantly disrupts the movement of heat-carrying phonons, leading to an exceptionally low lattice thermal conductivity of 0.32 W m−1 K−1, pushing it below the amorphous limit. Consequently, a peak figure of merit of 1.64 achieves at 873 K in Sn0.71Ge0.2Mn0.07In0.02Te. These findings lay the groundwork for developing advanced thermoelectric materials via entropy engineering.
期刊介绍:
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