<strong>p</strong>型方钴矿热电材料纳米<strong>-</strong>介观尺度微结构调控

doi:10.11900/0412.1961.2021.00515

金属学报

2022, Vol. 58

Issue (8): 979-991 DOI: 10.11900/0412.1961.2021.00515

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p型方钴矿热电材料纳米-介观尺度微结构调控

刘志愿¹^,²(

), 王永贵², 赵成玉², 杨婷², 夏爱林¹^,²

^1.安徽工业大学先进金属材料绿色制备与表面技术教育部重点实验室马鞍山 243002
^2.安徽工业大学材料科学与工程学院马鞍山 243002

Nano-Mesoscopic Scale Microstructure Regulation for p-Type Skutterudite Thermoelectric Materials

LIU Zhiyuan¹^,²(

), WANG Yonggui², ZHAO Chengyu², YANG Ting², XIA Ailin¹^,²

^1.Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials, Ministry of Education, Anhui University of Technology, Ma'anshan 243002, China
^2.School of Materials Science and Engineering, Anhui University of Technology, Ma'anshan 243002, China

引用本文:

刘志愿, 王永贵, 赵成玉, 杨婷, 夏爱林. p型方钴矿热电材料纳米-介观尺度微结构调控[J]. 金属学报, 2022, 58(8): 979-991.
Zhiyuan LIU, Yonggui WANG, Chengyu ZHAO, Ting YANG, Ailin XIA. Nano-Mesoscopic Scale Microstructure Regulation for p-Type Skutterudite Thermoelectric Materials[J]. Acta Metall Sin, 2022, 58(8): 979-991.

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摘要:

方钴矿热电材料具有优异的电输运性能,是热电器件核心部件最有前途的候选材料之一。热电器件需要性能相匹配的p型和n型方钴矿热电材料,然而p型方钴矿材料的热电性能和力学性能远低于n型方钴矿材料,因此提升p型方钴矿材料的热电性能和力学性能对于开发高效热电器件具有重要意义。本文总结了近年来在纳米-介观尺度调控p型方钴矿热电材料微结构的主要研究进展。通过微结构的调控可显著提升p型方钴矿材料的热电性能和力学性能,为热电器件的应用提供科学和技术支撑。

关键词 ： p型方钴矿热电材料, 纳米-介观调控, 微结构, 热电性能

Abstract：

Skutterudite thermoelectric materials are one of the most promising candidates for critical components in thermoelectric devices because of their excellent electrical transport properties. Thermoelectric devices require p- and n-type skutterudite materials with matching properties. However, the p-type skutterudite materials have considerably worse thermoelectric and mechanical properties than those of n-type. Thus, it is important to enhance the thermoelectric and mechanical properties of p-type skutterudite materials for the development of high-efficiency thermoelectric devices. This study summarizes the recent research progress on the nano-mesoscopic scale regulation of the microstructure for p-type skutterudite thermoelectric materials. The thermoelectric and mechanical properties of p-type skutterudite materials can be notably enhanced by adjusting the microstructure at the nano-mesoscopic scale; thus, providing scientific and technical supports for the thermoelectric device's application.

Key words： p-type skutterudite thermoelectric material nano-mesoscopic regulation microstructure thermoelectric property

收稿日期: 2021-11-29

ZTFLH:

TG132.24

基金资助:国家自然科学基金项目(51872006);国家创新创业本科培养计划项目(S202110360181)

作者简介: 刘志愿,男,1982年生,副教授,博士

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图1 纳米-介观尺度p型方钴矿热电材料的微结构调控方法[34,40~46]

图2 具有低维纳米结构的p型方钴矿材料La0.5Ce0.5Fe3CoSb12样品的SEM像[40],p型填充方钴矿Ce0.45Nd0.45Fe3.5Co0.5Sb12粉体经球磨5 h后的SEM像[25],通过传统固相反应和熔融旋甩法制备的Nd0.9Fe3CoSb12样品的SEM像[41],La x Ti0.1Ga0.1Fe3CoSb12样品甩带自由面的SEM像及La x Ti0.1Ga0.1Fe3CoSb12熔融旋甩样品和退火样品的热电优值(ZT值)[60]

图3 Co0.95Fe0.05Sb3薄膜的SEM像[49],Co1 - x Fe x Sb3 (0 ≤ x ≤ 0.1)样品的功率因子(S2σ)[49],CoSb3 + 0.72%Ti薄膜的SEM像[42],Ti掺杂的CoSb3薄膜的生长过程示意图[42],纳米结构和Ti基点缺陷的各种声子散射机制[42],不同Ti含量CoSb3薄膜的Seebeck系数和ZT值与温度(T)的依赖关系曲线图[42]

图4 含纳米孔结构的CeFe4Sb11.9Te0.1样品的FESEM像和CeFe4Sb12 - x Te x 方钴矿材料的ZT值[34],具有纳米膜结构的CeFe3.8Zn0.2Sb12样品的FESEM像和CeFe4 - x Zn x Sb12样品的ZT值[43]

图5 CeFe3CoSb12 + 5%MoO2 (摩尔分数)纳米复合样品的SEM像[44],CeFe3CoSb12和(CeFe3CoSb12)1 - x (MoO2) x 复合样品的ZT值[44],MmFe4Sb12 + 16%Mm2O3 (质量分数)纳米复合材料(Nano-composite 2)断口的SEM像[74],MmFe4Sb12 + 16%Mm2O3纳米复合热电材料及参考样品的ZT值[74]

图6 CoSb3/0.2%G FeCl3 (质量分数)样品横截面SEM像[77],CoSb3/x%G FeCl3 (质量分数)样品的功率因子[77],CoSb3/3%MoS2 (质量分数)纳米复合材料断裂面SEM像[45],CoSb3/xMoS2纳米复合材料的ZT值[45]

图7 La0.8Ti0.1Ga0.1Fe3CoSb12/0.1Fe3Si样品SEM像[33],La0.8Ti0.1Ga0.1Fe3CoSb12/xFe3Si纳米复合材料的ZT值[33],Nd0.6Fe2Co2-Sb11.6Sn0.4样品的SEM像[46],Nd0.6Fe2Co2Sb12 - x Sn x 纳米复合材料的ZT值[46],CeFe4Sb12 + 0.2Ce样品的FESEM像[82],CeFe4Sb12 + 0.1Ce样品的TEM像[82],CeFe4Sb12 + yCe纳米复合材料的ZT值[82]

图8 CeFe4Sb12/3%Cf (体积分数)样品断裂面的SEM像和抛光面的SEM像[84],Ce0.85Fe3CoSb12/1.4%rGO (还原氧化石墨烯,体积分数)样品的断面SEM像[85],石墨烯增韧机理示意图和Ce0.85Fe3CoSb12/y%rGO (体积分数)复合材料的弯曲强度(σ)和断裂韧性(KIC)[85]

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